WO2012094743A1 - Plasma reactor and method of operation thereof - Google Patents

Plasma reactor and method of operation thereof Download PDF

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Publication number
WO2012094743A1
WO2012094743A1 PCT/CA2012/000029 CA2012000029W WO2012094743A1 WO 2012094743 A1 WO2012094743 A1 WO 2012094743A1 CA 2012000029 W CA2012000029 W CA 2012000029W WO 2012094743 A1 WO2012094743 A1 WO 2012094743A1
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WO
WIPO (PCT)
Prior art keywords
electrode
reaction zone
plasma
surface portion
fluid
Prior art date
Application number
PCT/CA2012/000029
Other languages
French (fr)
Inventor
Tobie Boutot
Thomas Whidden
Yun Yang
Zhoumin Liu
Original Assignee
Atlantic Hydrogen Inc.
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by Atlantic Hydrogen Inc. filed Critical Atlantic Hydrogen Inc.
Publication of WO2012094743A1 publication Critical patent/WO2012094743A1/en

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Classifications

    • HELECTRICITY
    • H05ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
    • H05HPLASMA TECHNIQUE; PRODUCTION OF ACCELERATED ELECTRICALLY-CHARGED PARTICLES OR OF NEUTRONS; PRODUCTION OR ACCELERATION OF NEUTRAL MOLECULAR OR ATOMIC BEAMS
    • H05H1/00Generating plasma; Handling plasma
    • H05H1/24Generating plasma
    • H05H1/48Generating plasma using an arc
    • BPERFORMING OPERATIONS; TRANSPORTING
    • B01PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01JCHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J19/00Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J19/08Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor
    • B01J19/087Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor employing electric or magnetic energy
    • B01J19/088Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor employing electric or magnetic energy giving rise to electric discharges
    • CCHEMISTRY; METALLURGY
    • C01INORGANIC CHEMISTRY
    • C01BNON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B3/00Hydrogen; Gaseous mixtures containing hydrogen; Separation of hydrogen from mixtures containing it; Purification of hydrogen
    • C01B3/02Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen
    • C01B3/32Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air
    • C01B3/34Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air by reaction of hydrocarbons with gasifying agents
    • C01B3/342Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air by reaction of hydrocarbons with gasifying agents with the aid of electrical means, electromagnetic or mechanical vibrations, or particle radiations
    • BPERFORMING OPERATIONS; TRANSPORTING
    • B01PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01JCHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J2219/00Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J2219/08Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor
    • B01J2219/0803Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor employing electric or magnetic energy
    • B01J2219/0805Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor employing electric or magnetic energy giving rise to electric discharges
    • B01J2219/0807Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor employing electric or magnetic energy giving rise to electric discharges involving electrodes
    • B01J2219/0824Details relating to the shape of the electrodes
    • B01J2219/0826Details relating to the shape of the electrodes essentially linear
    • B01J2219/0828Wires
    • BPERFORMING OPERATIONS; TRANSPORTING
    • B01PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01JCHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J2219/00Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J2219/08Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor
    • B01J2219/0803Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor employing electric or magnetic energy
    • B01J2219/0805Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor employing electric or magnetic energy giving rise to electric discharges
    • B01J2219/0807Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor employing electric or magnetic energy giving rise to electric discharges involving electrodes
    • B01J2219/0824Details relating to the shape of the electrodes
    • B01J2219/0826Details relating to the shape of the electrodes essentially linear
    • B01J2219/083Details relating to the shape of the electrodes essentially linear cylindrical
    • BPERFORMING OPERATIONS; TRANSPORTING
    • B01PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01JCHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J2219/00Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J2219/08Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor
    • B01J2219/0803Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor employing electric or magnetic energy
    • B01J2219/0805Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor employing electric or magnetic energy giving rise to electric discharges
    • B01J2219/0807Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor employing electric or magnetic energy giving rise to electric discharges involving electrodes
    • B01J2219/0837Details relating to the material of the electrodes
    • B01J2219/0841Metal
    • BPERFORMING OPERATIONS; TRANSPORTING
    • B01PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01JCHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J2219/00Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J2219/08Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor
    • B01J2219/0873Materials to be treated
    • B01J2219/0875Gas
    • BPERFORMING OPERATIONS; TRANSPORTING
    • B01PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01JCHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J2219/00Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J2219/08Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor
    • B01J2219/0894Processes carried out in the presence of a plasma
    • HELECTRICITY
    • H05ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
    • H05HPLASMA TECHNIQUE; PRODUCTION OF ACCELERATED ELECTRICALLY-CHARGED PARTICLES OR OF NEUTRONS; PRODUCTION OR ACCELERATION OF NEUTRAL MOLECULAR OR ATOMIC BEAMS
    • H05H2245/00Applications of plasma devices
    • H05H2245/10Treatment of gases
    • H05H2245/15Ambient air; Ozonisers

Definitions

  • the present disclosure relates to effecting reactions in a plasma.
  • a method of operating a plasma reactor including a reaction zone.
  • the method includes generating a plasma in the reaction zone, and contacting reactant matter with the plasma in the reaction zone, wherein the pressure in the reaction zone is at least 75 psig.
  • a reactor defining an internal space including a reaction zone, and includes a plasma generator.
  • the plasma generator includes first and second electrodes.
  • the first electrode is configured for electrical coupling to a current and voltage source.
  • the second electrode is spaced apart from and disposed in electrical discharge communication with the first electrode through the internal space, and includes an operative second electrode surface portion.
  • the reaction zone is disposed between the first and second electrodes.
  • the operative second electrode surface portion is defined by a radius of curvature of less than 0.002 inches.
  • a reactor including an internal surface defining an internal space including a reaction zone.
  • the reactor includes a plasma generator.
  • the plasma generator includes first and second electrodes.
  • the first electrode is configured for electrical coupling to a current and voltage source.
  • the second electrode is spaced apart from and disposed in electrical discharge communication with the first electrode through the internal space, and includes an operative second electrode surface portion.
  • the reaction zone is disposed between the first electrode and the operative second electrode surface portion.
  • the first electrode is mounted within a reaction vessel with a mounting structure including an internal mounting structure surface defining a portion of the internal surface, wherein the mounting surface is disposed in fluid communication with the reaction zone.
  • the minimum distance between the operative second electrode surface and the mounting structure is at least two (2) inches.
  • a reactor defining a fluid passage portion for flowing a plasma forming gaseous fluid, wherein the fluid passage portion includes an upstream fluid passage portion and a downstream fluid passage portion.
  • the reactor includes a plasma generator.
  • the plasma generator includes first and second electrodes.
  • the first electrode is configured for electrical coupling to a current and voltage source.
  • the second electrode is spaced apart from and disposed in electrical discharge communication with the first electrode through the internal space, and includes an operative second electrode surface portion.
  • the reaction zone is defined between the first electrode and the operative second electrode portion, and the downstream fluid portion extends downstream from within the reaction zone.
  • the operative second electrode surface portion is spaced apart from the first electrode by a minimum distance of less than 0.15 inches.
  • the upstream fluid passage portion is defined by an upstream conduit wall disposed upstream of the reaction zone, wherein the upstream conduit wall includes at least one electrically conductive upstream conduit wall portion.
  • Any electrically conductive upstream conduit wall portion which is disposed in electrical discharge communication with the first electrode, is disposed further from the first electrode than the operative second electrode surface portion.
  • the operative second electrode surface portion is disposed in thermal communication with at least one electrically conductive upstream conduit wall portion.
  • a reactor defining a fluid passage portion for flowing a plasma forming gaseous fluid, wherein the fluid passage portion includes an upstream fluid passage portion and a downstream fluid passage portion.
  • the reactor includes a plasma generator.
  • the plasma generator includes first and second electrodes.
  • the first electrode is configured for electrical coupling to a current and voltage source.
  • the second electrode is spaced apart from and disposed in electrical discharge communication with the first electrode through the internal space.
  • the reaction zone is defined between the first electrode and the second electrode, and the downstream fluid passage portion extends downstream from within the reaction zone, and the upstream fluid passage portion is disposed upstream of the reaction zone.
  • the plasma forming gaseous fluid When the plasma forming gaseous fluid is disposed within the reaction zone and a sufficient electrical potential difference is applied between the first electrode and the second electrode, an electrical discharge is effected between the first electrode and the second electrode and through the reaction zone, and at least a fraction of the plasma forming gaseous fluid is converted into a plasma.
  • the first electrode is at least partially disposed in the downstream fluid passage portion and is spaced apart from an internal conduit wall of the downstream fluid passage portion to define a fluid flow space in the downstream fluid passage portion, wherein, in any plane which intersects that portion of the first electrode disposed in the downstream fluid passage portion, and which is disposed in a normal orientation relative to an axis of the downstream fluid passage portion being intersected, the ratio of the diameter of the first electrode to the diameter of the downstream fluid passage portion is between two (2) and five (5).
  • a reactor including an internal space defining a fluid passage portion for flowing a plasma forming gaseous fluid, wherein the fluid passage portion includes a reaction zone.
  • the reactor includes a plasma generator.
  • the plasma generator includes first and second electrodes.
  • the first electrode is configured for electrical coupling to a current and voltage source, and including an operative first electrode surface portion.
  • the second electrode is spaced apart from and disposed in electrical discharge communication with the first electrode through the internal space, and including an operative second electrode surface portion.
  • the reaction zone is disposed between the first and second electrodes.
  • An operative distance is defined along the longitudinal axis of the first electrode between: (i) a plane in which is disposed an axis normal to the operative first electrode surface portion and (ii) a tip of the first electrode downstream of the operative first electrode surface portion, wherein the operative distance is at least 0.25 inches.
  • a reactor defining an internal space including a reaction zone, and including an inlet fluidly coupled to the reaction zone with a fluid introduction passage for introducing a plasma forming gaseous fluid into the reaction zone.
  • the reactor includes a plasma generator.
  • the plasma generator includes first and second electrodes.
  • the first electrode is configured for electrical coupling to a current and voltage source.
  • the second electrode is spaced apart from and disposed in electrical discharge communication with the first electrode through the internal space.
  • the reaction zone is disposed between the first and second electrodes.
  • the reaction vessel includes a heat exchanger disposed in heat transfer communication with the fluid introduction passage for effecting heat transfer to plasma forming gaseous fluid being introduced to the reaction zone.
  • Figure 1 is a schematic illustration of an embodiment of an electric circuit for effecting a high voltage power supply to a reactor
  • Figure 2 is a schematic illustration of a sectional, front elevation view of an embodiment of the reactor
  • Figure 3A is an exploded sectional view of the high voltage feedthrough assembly of the reactor in Figure 1 ;
  • Figure 3B is an exploded sectional view of a lower portion of the reactor in Figure 2;
  • Figure 4 is a sectional detailed front elevation fragmentary view of an upper portion of the reactor in Figure 2;
  • Figure 5 is a sectional detailed front elevation fragmentary view of a lower portion of the reactor in Figure 2;
  • Figure 6 is a sectional detailed front elevation exploded view of the lower portion of the reactor in Figure 2;
  • Figure 7 is a schematic illustration of a sectional, front elevation view of another embodiment of the reactor.
  • Figure 8 is the same view as in Figure 2, and illustrates the dimension Dl , which is the minimum distance between the operative second electrode surface portion and the mounting surface within the reactor.
  • Figure 9 is a sectional detailed front elevation fragmentary view of a lower portion of the reactor in Figure 2, and illustrates the dimension D2, which is the minimum distance by which the operative second electrode surface portion is spaced apart from the first electrode within the reactor.
  • Figures 10 and 11 illustrate the relationship between dimensions D3, which is the diameter of the first electrode, and D4, which is the diameter of the downstream fluid passage portion, wherein Figure 10 is the same view as in Figure 5 and also illustrates generated plasma, and Figure 11 is a cross-sectional view of the downstream fluid passage portion taken along plane 200; and
  • Figure 12 is the same view as in Figure 5 and also illustrates generated plasma, and also illustrates the dimension D5, which is an operative distance defined along the longitudinal axis of the first electrode between: (i) a plane in which is disposed an axis normal to the operative first electrode surface portion, and (ii) the tip of the first electrode.
  • a reactor 10 configured for generating a plasma.
  • the reactor 10 includes an internal space 26 including a reaction zone 32.
  • the reactor 10 also includes a plasma generator 34.
  • the plasma generator 34 includes a first electrode 36 and a second electrode 52.
  • the first electrode 36 is configured for electrical coupling to a current and voltage source 44.
  • the second electrode 52 is spaced apart from and disposed in electrical discharge communication with the first electrode 36 through the internal space 26.
  • the second electrode 52 is a ground electrode.
  • the reaction zone 32 is disposed between the first electrode 36 and the second electrode 52.
  • the plasma forming gaseous fluid When the plasma forming gaseous fluid is disposed within the reaction zone 32 and a sufficient electrical potential difference is applied between the first electrode 36 and the second electrode 52, an electrical discharge is effected between the first electrode 36 and the second electrode 52 and through the reaction zone 32, and at least a fraction of the plasma forming gaseous fluid is converted into a plasma.
  • the internal space 26 includes a fluid passage portion 64 for flowing a plasma forming gaseous fluid through the reaction zone 32.
  • the fluid passage portion 64 includes an upstream fluid passage portion 66 disposed upstream of the reaction zone 32, and also includes a downstream fluid passage portion 74 extending downstream from within the reaction zone 32.
  • the second electrode 52 includes an operative second electrode surface portion 54.
  • the effected electrical discharge is between the first electrode 36 surface and the operative second electrode surface portion 54 and at least a fraction of the plasma forming gaseous fluid is converted into a plasma.
  • the reaction zone 32 is provided in an internal space 26 defined by an internal surface 28 of the reactor 10, and the operative second electrode surface portion 54 is an electrically conductive surface portion of the internal surface 28 that is closest to the first electrode 36.
  • the reactor 10 includes a reaction vessel 12, and the first electrode 36 is mounted within the reaction vessel 12 with a mounting structure 46.
  • the reaction vessel is constructed of stainless (such as 304 stainless steel, or 316 stainless steel).
  • standard pipe flange connections are provided to effect coupling to feed and exhaust systems.
  • the first electrode 36 is electrically coupled to the current and voltage source 44.
  • the frequency of the current and voltage source 44 is from lOKHz to 20KHz
  • the pulse width of the current and voltage source 44 is from 10 to 20 micro-seconds.
  • An exemplary electrical circuit for effecting a high voltage power supply to the first and second electrodes 36, 52 is illustrated in Figure 1.
  • the first electrode 36 is electrically connected to a power supply.
  • the power supply 2011 includes a rectifier 2013, a pulser 2015 (or inverter), a high voltage pulse transformer 2017, and, optionally, high voltage capacitors 2019 connected in series with the secondary winding of the pulse transformer 2017.
  • the high voltage capacitors 2019 function in multi-discharge generation and for impedance matching, and, in this respect, allow simultaneous powering of multiple electrodes by a single power source, such as various embodiments of the reactor 10 which are described and illustrated in Canadian Patent Application No. 2,516,499 which is herein incorporated by reference in its entirety.
  • the high voltage capacitors 2019 can be omitted under single discharge conditions.
  • the power supply provides controlled bipolar high voltage pulses to a high voltage transformer which acts as a filter to make the current almost sinusoidal. For example, switching frequencies are between 10 kHz to 20 kHz, such as between 15 kHz to 17 kHz. For example, the pulse widths are between 10 to 20 microseconds, such as between 15 to 17 microseconds.
  • a stable flow of plasma forming gaseous fluid is established through the reactor vessel, and once substantially all of the ambient air has been purged from the reaction vessel 12, a high voltage pulse is supplied to the first electrode 36, and plasma is created in the reaction zone 32 between the first electrode 36 and the second electrode 52.
  • each one of these electrodes is electrically conductive and is configured to operate robustly in high temperature conditions.
  • the first electrode 36 includes a lanthanated tungsten rod.
  • suitable materials for the first electrode 36 structure include substantially pure tungsten, 2% thoriated tungsten, tungsten carbide, and other tungsten alloys.
  • the first electrode 36 is electrically coupled to the voltage and power source through a high voltage feedthrough assembly 300.
  • the high voltage feedthrough assembly (HVFA) 300 is configured to provide high voltage (HV) power to the first electrode 36 and to contain any pressurized gas within the reaction vessel 12.
  • the HVFA 300 is configured to operate continuously at 20 kV and 20 kHz and at a working pressure of 300psig.
  • a set of releasably coupled flanges 302, 121 provide for access to the HVFA.
  • the HVFA 300 is composed of a top flange 302, an insulator 304, a high voltage input conductor 306, a threaded insert 308, a high voltage conductor holder 310, and an alignment ring 312.
  • the HVFA defines an upper reaction vessel portion 1202 of the reaction vessel 12.
  • the top flange 302 is provided for holding the HVFA 300 while simultaneously ensuring a hermetic seal for the reaction vessel 12.
  • the top flange 302 maintains the integrity of coupling between the HVFA 300 and the remaining portion of the reaction vessel 12 when pressurized gas is provided within the reaction vessel 12.
  • the insulator 304 provides electrical insulation between the metallic high voltage and grounding components of the reactor 10 and contains the pressure inside the reaction vessel 12.
  • the material of the insulator 304 is MACORTM made by Corning Incorporated.
  • the insulator carries two (2) o-ring seals 314, 316 that provide a positive seal with the top flange 302.
  • the high voltage feed conductor 306 extends through a passage provided through the center of the insulator 304.
  • the high voltage input conductor 306 is electrically coupled to the first electrode 36 and is provided for conducting high voltage power to the first electrode 36.
  • the high voltage input conductor 306 also provides a pressure barrier to gas pressure within the reaction vessel 12.
  • the high voltage input conductor 306 is made from stainless steel but can be made from any conductive metal that is compatible with the fluid used and that is rated for the operating pressure.
  • the first electrode 36 is attached to the high input conductor 306 by friction fit within a hole 322 provided in the high voltage input conductor 306.
  • the hole 322 is sized slightly smaller than the first electrode 36 and is drilled inside the high voltage input conductor 306. Slits are formed on the side to allow the wall to expand slightly, when the first electrode 36 is inserted.
  • the high voltage input conductor 306 is coupled to the insulator 304 by the threaded insert 308.
  • the threaded insert 308 is manufactured from TeflonTM made by E. I. du Pont de Nemours and Company.
  • the high voltage conductor holder 310 maintains positioning of the high voltage input conductor 306 at the center of the assembly 300 and includes a passage through which the high voltage input conductor 306 extends.
  • the holder 310 also provides electrical insulation between the high voltage input conductor 306 and the internal surface 28 of reaction vessel 12.
  • the high voltage conductor holder 310 is made from TeflonTM.
  • the high voltage conductor holder 310 is supported by the alignment ring 312.
  • the alignment ring 312 supports the high voltage conductor holder 310 and provides a seal between the flanges 302, 121 .
  • the alignment ring 312 is made from stainless steel.
  • the reactor includes the upper reaction vessel portion 122, an intermediate reaction vessel portion 124, and a lower reaction vessel portion 126.
  • the intermediate reaction vessel portion 124 includes a second electrode assembly 1244 coupled to and disposed internally within an intermediate containment component 1242.
  • the second electrode assembly 1244 includes a second electrode- comprising structure 1246 (for example, made from tungsten), a containment structure
  • the second electrode— comprising structure includes the second electrode 52.
  • the combination of the upper and lower sleeves 1250, 1252 define at least a portion of the downstream fluid passage portion extending from the within the reaction zone 32.
  • the heat transfer medium 94 is provided to effect dissipation of heat from an internal surface portion 96, of a downstream internal conduit surface 76, adjacent to the reaction zone 32.
  • the insulator 1254 is disposed downstream of the heat transfer medium 94, and is provided for mitigating heat transfer from a downstream fluid passage portion 74 so as to assist in sustaining reactive processes within the plasma, as described below.
  • the assembly of the second electrode assembly 1244 is now described.
  • the upper sleeve 1250 is seated on a seating surface provided on the lower sleeve (see Detail "A" in Figure 6).
  • the second electrode-comprising structure 1246 is then seated on the upper sleeve 1250, and this intermediate assembly is then inserted into a receiving space
  • the second electrode-comprising structure 1246 is then returned, and positioned such that the second electrode-comprising structure 1246 is seated on the upper sleeve 1250, the heat transfer medium 94, and the containment structure 1248.
  • a set screw is inserted through passage 1264 and then tightened against the second electrode-comprising structure to effect its desired positioning relative to the containment structure 1248.
  • the second electrode assembly 1244 is then inserted into a receiving space 1257 defined within the intermediate containment component 1242, and threadably coupled to the intermediate containment component 1242 by co-operative threads 1260, 1262 (see Figure 3B) provided on the second electrode assembly 1244 and the intermediate containment component 1242, respectively.
  • Positioning of the second electrode assembly 1244, and, therefore, the second electrode 52 and the operative second electrode portion 54, is adjusted by rotating the second electrode assembly 1244 relative to the intermediate containment component 1242 while the second electrode assembly 1244 is threadably engaged to the intermediate containment component 1242.
  • the upper reaction vessel portion 122 defined by the HVFA 300, is integrated into the reactor 10 by coupling to the assembled intermediate reaction vessel portion 124.
  • the insulator/pressure barrier 304 with its two (2) o-rings 314, 316 in place is inserted from below into the upper reaction vessel portion flange 302, making sure it is firmly in contact with the flange 302.
  • the high voltage input conductor 306, with its two (2) o-rings installed 318, 320, is inserted through the passage provided in the insulator/pressure barrier 304.
  • the larger diameter section of the high voltage input conductor 306 is firmly seated against the insulator/pressure barrier 304.
  • the threaded insert 308 is screwed into the insulator/pressure barrier 304 to hold the high voltage input conductor 306 in place.
  • the high voltage conductor holder 310 is then inserted into the alignment ring and this assembly is inserted through the top of and into the flanged lower reaction vessel portion 13.
  • the flange 302 is coupled to a intermediate reaction vessel portion upper flange 121 of the intermediate containment component 1242, with the alignment ring 312 disposed in-between the two flanges 302, 121.
  • Bolts and nuts are inserted in each flange hole and tightened appropriately to effect coupling of the HVFA 300 to the intermediate containment component 1242.
  • the lower reaction vessel portion 126 is then coupled to the intermediate reaction vessel portion 124.
  • the lower reaction vessel portion 126 includes the outlet 22.
  • a lower reaction vessel portion flange 1261 of the lower reaction vessel portion 126 is connected to an intermediate reaction vessel portion lower flange 1256 using bolts and nuts.
  • the second electrode 52 is made from stainless steel.
  • suitable materials include lanthanated tungsten, substantially pure tungsten, 2% thoriated tungsten, tungsten carbide, other tungsten alloys, graphite, or silicon carbide.
  • the plasma forming gaseous fluid is any one of those fluids that can be ionized through electron impact events within a voltage potential gradient, and thereby create a reduced impedance pathway that provides a current path.
  • Any ionisable fluid can form a plasma provided that a sufficient electric potential gradient exists.
  • Such ionisable fluids include, but are not limited to, elemental species such as the noble gases (He, Ne, Ar, etc.), molecular gases (i.e. H 2 , 0 2 , 0 3 , CH 4 , CF 4 , SF 6 , H 2 S, etc.) and vaporizable organic liquids (i.e.
  • the plasma forming gaseous fluid includes no gaseous oxygen or substantially no gaseous oxygen.
  • the reactor 10 includes an inlet 20 configured for introducing the plasma forming gaseous fluid flow to the plasma generator 34 so as to effect the plasma discharge into the reaction zone 32 by the plasma generator 34 such that the plasma discharge facilitates conversion of reactant matter in the reaction zone 32 into product matter.
  • the reactor 10 is configured for receiving reactant matter within the reaction zone 32.
  • the reactant matter is in the form of a fluid, such as a gaseous fluid
  • the reactor includes the inlet 20 for introducing reactant matter fluid as reactant matter fluid flow into the reaction zone 32.
  • the inlet 20 for the plasma forming gaseous fluid flow is the same as the inlet 20 for the reactant matter fluid flow as the plasma forming gaseous fluid is the same as the reactant matter fluid.
  • the plasma forming gaseous fluid flow when it is the same as the reactant matter fluid flow, is introduced through the inlet 20 at a flow rate of 3.5 cubic metres per hour.
  • the reactant matter consists of any one of: (i) an element, (ii) a compound, (iii) a homogeneous or inhomogeneous mixture of any one of: (a) at least two elements, or (b) at least two compounds, or (iv) a homogeneous or inhomogeneous mixture of any combination of: (a) at least one element, and (b) at least one compound.
  • the reactant matter which is suitable for conversion within the plasma generated by the plasma generator 34 includes gaseous and liquid hydrocarbons such as natural gas, volatile petroleum fractions, landfill and other bio-generated fuel gases, methane, ethane, propane, propene, butane, pentane, and hexane, and volatile oxygenated organic compounds such as methanol, and ethanol, and reactive molecular element species such as, but not limited to, hydrogen, oxygen and ozone, and volatile inorganic hydrides such as, but not limited to, H 2 S, SiH 4 , PH 3 , and As3 ⁇ 4.
  • the reactant matter includes syngas (carbon dioxide and methane). At least a fraction of the reactant matter is subjected to a reactive process in the plasma generated by the plasma generator 34, such that the reactive process effects creation of product matter.
  • the product matter includes solid particulate matter.
  • the solid particulate matter includes carbon- comprising matter, such as carbon.
  • at least a fraction of the solid particulate matter of the product matter becomes coupled to an internal surface 28 of the reaction vessel 12.
  • the solid particulate matter is said to be coupled to the internal surface 28 when the solid particulate matter adheres to the internal surface 28 or becomes associated with solid matter which is already adhered to the internal surface 28.
  • Mechanisms for association of the solid particulate matter with the solid matter adhered to the internal surface 28 include absorption, dissolution, covalent bonding, or ionic bonding.
  • the operative forces, whose action effects the adhesion or the association, include any one of, or any combination of, Van der Waals adhesive forces, electrostatic forces, and gravity.
  • the plasma forming gaseous fluid includes the reactant matter.
  • the plasma forming gaseous fluid includes any of the suitable reactant matter described above.
  • a suitable plasma forming gaseous fluid is natural gas, typically including 70 mole % to 95 mole % methane, based on the total number of moles of plasma forming gaseous fluid, with small amounts of other hydrocarbons such as ethane and propane and varying levels of inert gases such as nitrogen and contaminant gases such as hydrogen sulphide.
  • these fluids are introduced into the plasma reactor 10 at flows that can vary between very low (lO's of cc/min) to very high (lO's of Nm /hour).
  • the plasma forming gaseous fluid is provided within the reaction zone 32.
  • natural gas feed flow to the reactor 10 ranges between 0.1 Nm /hour and 10 Nm 3 /hour.
  • the reaction is carried out at pressures that may range from medium vacuum (100's of Torr) to atmospheric and relatively high pressures (i.e. up to at least 300 psig). In this respect, for example, the reaction is carried out at a pressure of 150 psig.
  • the system temperature is allowed to equilibrate to accommodate the small zone of very high (1000-1500°C) temperature in the plasma plume.
  • internal wall temperatures of the reactor 10 may be as high as 500°C.
  • the reactant matter of the plasma forming gaseous fluid is converted in the reaction zone 32 in accordance with any one of or any combination of the reaction steps described in Appendix "A".
  • the conversion of the reactant matter of the plasma forming gaseous fluid results in product matter including solid particulate matter, wherein the solid particulate matter includes carbon.
  • the reactor 10 includes an outlet 22 configured for discharging the product matter.
  • the reaction vessel 12 also includes a heat exchanger disposed in thermal communication with the outlet 22 and configured for effecting heat transfer from the product matter discharging through the outlet 22.
  • heat transfer effects cooling of the discharging product matter.
  • heat transfer could effect heating of the plasma forming gaseous fluid before the plasma- forming gaseous fluid is introduced into the reaction vessel 12.
  • the heat exchanger is configured to receive the plasma-forming gaseous fluid and effect heat transfer from the discharging product matter and to the plasma-forming gaseous fluid.
  • an internal surface portion 96, of a downstream internal conduit surface 76, adjacent to the reaction zone 32 is disposed in thermal communication with a heat transfer medium 94 extending between the reaction zone adjacent internal surface portion 96 and an external surface 98 of the reactor for effecting dissipation of heat from the internal surface portion 96.
  • the heat transfer medium 94 is steel wool.
  • the plasma reactor 10 includes a reaction zone 32.
  • the method includes contacting reactant matter with a plasma 102 in a reaction zone 32.
  • the plasma 102 is generated in the reaction zone 32.
  • the pressure in the reaction zone 32 is at least 75 psig. In some embodiments, for example, the pressure in the reaction zone 32 is greater than 300 psig. In other embodiments, for example, the pressure in the reaction zone 32 is 150 psig.
  • the plasma 102 (see Figures 10 or 12) is generated by flowing a plasma forming fluid flow through a reaction zone 32 through which an electrical discharge is being effected.
  • the plasma forming fluid includes reactant matter.
  • the reactant matter includes natural gas.
  • the reactant matter includes methane.
  • the reactor 10 includes an electrode surface portion with a relatively low radius of curvature for, amongst other things, facilitating an electrical discharges at a relatively lower applied electrical potential difference.
  • the reactor 10 includes an internal space 26 including a reaction zone 32.
  • the reactor 10 also includes a plasma generator 34.
  • the plasma generator 34 includes a first electrode 36 and a second electrode.
  • the first electrode 36 is configured for electrical coupling to a current and voltage source 44.
  • the second electrode 52 is spaced apart from and disposed in electrical discharge communication with the first electrode 36 through the internal space 26, and includes an operative second electrode surface portion 54.
  • the second electrode 52 is a ground electrode.
  • the operative second electrode surface portion 54 is defined by a radius of curvature of less than 0.002 inches.
  • the radius of curative is between 0.002 inches and 0.0055 inches.
  • the radius of curvature is as small as permitted by existing manufacturing techniques so as to facilitate generation of a larger electric field, which eases the ignition process of the plasma.
  • the reaction zone 32 is disposed between the first and second electrodes 36, 52.
  • the operative second electrode surface portion 54 is defined by an edge 58.
  • the reactor 10 includes an internal surface 28 defining the internal space 26, and the operative second electrode surface portion 54 is the conductive surface portion of the internal surface 28 which is closest to the first electrode 36.
  • the reactor 10 includes a fluid passage which includes the reaction zone 32.
  • the fluid passage includes upstream and downstream fluid passage portions 66, 74, and the operative second electrode surface portion 54 defines an orifice 92 which effects fluid communication between the upstream fluid passage portion 66 and the downstream fluid passage portion 74.
  • a method of operating any of the above-described embodiments of the reactor 10 in (B) includes contacting reactant matter with a plasma in a reaction zone 32, wherein the pressure in the reaction zone 32 is at least 75 psig.
  • the plasma is plasma generated by providing a plasma forming fluid in the reaction zone 32, and applying a sufficient electrical potential difference between the first electrode 36 and the operative second electrode surface portion 54, so as to effect an electrical discharge between the first electrode 36 and the operative second electrode surface portion 54 and through the reaction zone 32.
  • a sufficient electrical potential difference between the first electrode 36 and the operative second electrode surface portion 54, so as to effect an electrical discharge between the first electrode 36 and the operative second electrode surface portion 54 and through the reaction zone 32.
  • the plasma forming fluid includes reactant matter.
  • the reactant matter includes natural gas.
  • the reactant matter includes methane.
  • a further aspect includes providing a reactor 10 configured for generating a plasma by virtue of an electrical discharge between first and second electrodes 36, 52, and providing a minimum distance between an operative second electrode surface portion 54 of the second electrode 52 and a mounting structure 46 for mounting the first electrode 36.
  • a reactor 10 configured for generating a plasma by virtue of an electrical discharge between first and second electrodes 36, 52, and providing a minimum distance between an operative second electrode surface portion 54 of the second electrode 52 and a mounting structure 46 for mounting the first electrode 36.
  • the mounting structure 46 includes an internal mounting structure surface 48 defining a portion of the internal surface 28.
  • the internal mounting structure surface 48 is defined by an electrically non-conductive material 49 of the mounting structure 46.
  • the electrically non-conductive material 49 in some embodiments, for example, the electrically non-conductive material 49 defining the internal mounting structure surface 48 is disposed between the first electrode 36 and electrically conductive material, wherein such electrically conductive material is disposed within the reaction vessel 12 and in closer proximity to the first electrode 36 relative to the second electrode 52.
  • the electrically non-conductive material 49 includes a polymeric material, such as TEFLONTM.
  • the reaction vessel 12 includes an internal reaction vessel wall 14, and the electrically non-conductive material 49 extends to the internal reaction vessel wall 14 such that a reaction zone remote electrically non- conductive material surface 481 is provided in abutting relationship with the internal reaction vessel wall 14.
  • the internal reaction vessel wall 14 includes an electrically conductive internal reaction vessel wall portion 16 and, in some embodiments, the electrically conductive internal reaction vessel wall portion 16 is disposed in closer proximity to the first electrode 36 relative to the second electrode 52.
  • the electrically non-conductive material 49 in such cases, insulates the electrically conductive internal reaction vessel wall portion 16 from the first electrode 36.
  • the mounting structure 46 is the high voltage feedthrough assembly 300.
  • the reactor 10 includes an internal surface 28 defining an internal space 26 including a reaction zone 32.
  • the reactor 10 also includes a plasma generator 34.
  • the plasma generator 34 includes a first electrode 36 and a second electrode 52.
  • the first electrode 36 is configured for electrical coupling to a current and voltage source 44.
  • the second electrode 52 is spaced apart from and disposed in electrical discharge communication with the first electrode 36 through the internal space 26.
  • the second electrode 52 further includes an operative second electrode surface portion 54.
  • the second electrode 52 is a ground electrode.
  • the reaction zone 32 is disposed between the first electrode 36 and the operative second electrode surface portion 54.
  • the first electrode 36 is mounted within a reaction vessel 12 with a mounting structure 46.
  • the internal mounting structure surface 48 includes an internal mounting structure surface portion 482 defining a portion of the internal surface 28.
  • the internal mounting structure surface portion 482 is disposed in fluid communication with the reaction zone 32.
  • the minimum distance Dl between the operative second electrode surface portion 54 and the internal mounting structure surface portion 48 is at least two (2) inches. The minimum distance Dl varies depending on the fluid flow characteristics in the reaction zone 32.
  • the operative second electrode surface portion 54 is the electrically conductive surface portion of the internal surface 28 which is closest to the first electrode 36.
  • the internal mounting structure surface portion 48 is electrically non-conductive.
  • the mounting structure surface portion 48 includes a solid particulate deposition susceptible mounting surface portion 50 configured for becoming coupled to a solid particulate upon approach of the solid particulate to the solid particulate deposition susceptible mounting surface portion 50.
  • the solid particulate includes carbon-comprising particulate, such as particulate carbon.
  • the upstream fluid passage portion 66 is defined by an upstream conduit wall 68 disposed upstream of the reaction zone 32, wherein the upstream conduit wall 68 includes at least one electrically conductive upstream conduit wall surface portion 70. Further, any electrically conductive upstream conduit wall surface portion 70, which is disposed in electrical discharge communication with the first electrode 36, is disposed further from the first electrode 36 than the operative second electrode surface portion 54.
  • any electrically conductive upstream conduit wall surface portion 70 of the upstream conduit wall 68 that is spaced apart from the mounting structure by a minimum distance of D6 of at least 1.118 inches is also spaced apart from the first electrode 36 by a minimum distance D7 that is greater than 0.5 inches .
  • any electrically conductive upstream conduit wall surface portion 70 of the upstream conduit wall 68 that is spaced apart from the mounting structure by a minimum distance of D6 of 1.39 inches is also spaced apart from the first electrode 36 by a minimum distance D7 of 0.845 inches.
  • the upstream conduit wall 68 includes an upstream solid particulate deposition susceptible conduit wall surface portion 72 configured for becoming coupled to a solid particulate upon approach of the solid particulate to the upstream solid particulate deposition susceptible conduit wall surface portion 72.
  • the solid particulate includes carbon-comprising particulate, such as particulate carbon.
  • the upstream fluid passage portion 66 extends between the reaction zone 32 and the mounting structure 46.
  • the internal space 26 includes a fluid passage portion 64 for flowing a plasma forming gaseous fluid through the reaction zone 32.
  • the fluid passage portion 64 includes an upstream fluid passage portion 66 disposed upstream of the reaction zone 32 and between the mounting structure 46 and the reaction zone 32.
  • the fluid passage portion 64 also includes a downstream fluid passage portion 74 extending downstream from within the reaction zone 32.
  • the downstream fluid passage portion 74 is defined by a downstream internal conduit surface 76 including a downstream solid particulate deposition susceptible conduit surface portion 78.
  • the downstream solid particulate deposition susceptible conduit surface portion 78 is configured for becoming coupled to a solid particulate upon approach of the solid particulate to the downstream solid particulate deposition susceptible conduit surface portion 78.
  • the method includes contacting reactant matter with a plasma in a reaction zone 32 to effect production of product matter including solid particulate, such as carbon-comprising particulate.
  • solid particulate such as carbon-comprising particulate.
  • the solid particulate is carbon particulate.
  • the plasma is plasma generated by providing a plasma forming fluid in the reaction zone 32, and applying a sufficient electrical potential difference between the first electrode 36 and the operative second electrode surface portion 54, so as to effect an electrical discharge between the first electrode 36 and the operative second electrode surface portion 54 and through the reaction zone 32.
  • a sufficient electrical potential difference between the first electrode 36 and the operative second electrode surface portion 54, so as to effect an electrical discharge between the first electrode 36 and the operative second electrode surface portion 54 and through the reaction zone 32.
  • the plasma forming fluid includes a plasma forming fluid flow.
  • the plasma forming fluid includes reactant matter.
  • the reactant matter includes natural gas.
  • the reactant matter includes methane.
  • a carrier fluid flow for sweeping produced solid particulate from the reaction zone 32.
  • the downstream fluid passage portion 74 is defined by a downstream internal conduit surface 76 including a downstream solid particulate deposition susceptible conduit surface portion 78, wherein the downstream solid particulate deposition susceptible conduit surface portion 78 is configured for becoming coupled to the produced solid particulate upon approach of the produced solid particulate to the downstream solid particulate deposition susceptible conduit surface portion 78.
  • the minimum velocity of carrier fluid flow is 0.4 metres per second to 0.5 metres per second for flow through a circular fluid passage of a diameter of 0.4 inches. Further, in some embodiments, for example, the minimum velocity of carrier fluid flow is 0.5 metres per second to 0.6 metres per second for flow through a circular fluid passage of a diameter of 0.3 inches.
  • the carrier fluid flow in some embodiments, for example, at least a fraction of the carrier fluid flow is derived from the plasma forming fluid flow. In some embodiments, for example, the carrier fluid flow is entirely derived from the plasma forming fluid flow.
  • a maximum distance between electrodes is provided for, amongst other things, mitigating against the formation of a higher temperature environment at the electrodes during electrical discharge between the electrodes. Such higher temperatures would then effect formation of higher temperatures at non-preferred surfaces through heat transfer, and increase the likelihood of electrical discharge at these non-preferred surfaces.
  • the reactor 10 includes a fluid passage portion 64 for flowing a plasma forming gaseous fluid.
  • the fluid passage portion 64 includes a reaction zone 32.
  • the fluid passage portion 64 includes an upstream fluid passage portion 66 and a downstream fluid passage portion 74.
  • the upstream fluid passage portion 66 is defined by an upstream conduit wall 68 disposed upstream of the reaction zone 32, wherein the upstream conduit wall 68 includes at least one electrically conductive upstream conduit wall 68 portion.
  • the downstream fluid passage portion 74 extends downstream from within the reaction vessel 32.
  • the reactor 10 also includes a plasma generator 34.
  • the plasma generator 34 includes a first electrode 36 and a second electrode 52.
  • the first electrode 36 is configured for electrical coupling to a current and voltage source 44.
  • the second electrode 52 is spaced apart from and disposed in electrical discharge communication with the first electrode 36 through the internal space 26.
  • the second electrode 52 is a ground electrode.
  • the second electrode 52 includes an operative second electrode surface portion 54.
  • the reaction zone 32 is defined between the first electrode 36 and the operative second electrode surface portion 54.
  • the operative second electrode surface portion 54 is spaced apart from the first electrode 36 by a minimum distance D2 of less than 0.15 inches.
  • the minimum distance D2 is greater than 0.075 inches.
  • the minimum distance D2 is between 0.075 inches and 0.15 inches.
  • the operative second electrode surface portion 54 is disposed in thermal communication with at least one electrically conductive upstream conduit wall portion 70. Any of the at least one electrically conductive upstream conduit wall portion 70, that is disposed in electrical discharge communication with the first electrode 36, is disposed further from the first electrode 36 than the operative second electrode surface portion 54. Amongst other things, disposition of the operative second electrode surface portion 54 from the first electrode 36 beyond the above-described maximum distance increases the likelihood that heat is generated during the electrical discharge at the operative second electrode surface portion 54 and effects heating of an electrically conductive upstream conduit wall portion 70 to a temperature which is effective to facilitate an electrical discharge between the first electrode 36 and the electrically conductive upstream conduit wall portion 70. It is preferred to effect electrical discharge further downstream, rather than upstream, so as to effect reduced residence time of any produced solid particulate in the reactor 10 and thereby mitigate against deposition, within the reactor 10, of the produced solid particulate.
  • the upstream conduit wall 68 includes an upstream solid particulate deposition susceptible conduit wall portion 72 configured for becoming coupled to the solid particulate upon approach of solid particulate to the upstream solid particulate deposition susceptible conduit wall portion 72.
  • the downstream fluid passage portion 74 is defined by a downstream internal conduit surface 76 including a downstream solid particulate deposition susceptible conduit surface portion 78.
  • the downstream solid particulate deposition susceptible conduit surface portion 78 is configured for becoming coupled to solid particulate upon approach of the solid particulate to the downstream solid particulate deposition susceptible conduit surface portion 78.
  • the reaction zone 32 is provided in an internal space 26 defined by an internal surface 28 of the reactor 10, and the operative second electrode surface portion 54 is the electrically conductive surface portion of the internal surface 28 which is closest to the first electrode 36.
  • the upstream conduit wall 68 merges with the operative second electrode surface portion 54.
  • the solid particulate is carbon particulate.
  • the plasma is plasma generated by providing a plasma forming fluid in the reaction zone 32, and applying a sufficient electrical potential difference between the first electrode 36 and the operative second electrode surface portion 54, so as to effect an electrical discharge between the first electrode 36 and the operative second electrode surface portion 54 and through the reaction zone 32.
  • a sufficient electrical potential difference between the first electrode 36 and the operative second electrode surface portion 54, so as to effect an electrical discharge between the first electrode 36 and the operative second electrode surface portion 54 and through the reaction zone 32.
  • the plasma forming fluid includes a plasma forming fluid flow.
  • the plasma forming fluid includes reactant matter.
  • the reactant matter includes natural gas.
  • the reactant matter includes methane.
  • the downstream fluid passage portion 74 is defined by a downstream internal conduit surface 76 including a downstream solid particulate deposition susceptible conduit surface portion 78.
  • the downstream solid particulate deposition susceptible conduit surface portion 78 is configured for becoming coupled to the produced solid particulate upon approach of the produced solid particulate to the downstream solid particulate deposition susceptible conduit surface portion 78 Amongst other things, the carrier fluid flow mitigates against such deposition.
  • the minimum velocity of carrier fluid flow is 0.5 metres per second to 0.6 metres per second for flow through the downstream fluid passage portion 74 having an internal diameter of 0.3 inches.
  • at least a fraction of the carrier fluid flow is derived from the plasma forming fluid flow.
  • Another aspect is associated with a reactor 10 configured for generating a plasma.
  • This aspect provides, within a fluid passage within the reactor 10, an electrode with a defined electrode surface area which, amongst other things, effects cooling of the electrode while allowing sufficient space to effect desired conversion of reactants while mitigating against solid particulate deposition.
  • the reactor 10 includes a fluid passage portion 64 for flowing a plasma forming gaseous fluid.
  • the fluid passage portion 64 includes an upstream fluid passage portion 66 and a downstream fluid passage portion 74.
  • the reactor 10 also includes a plasma generator 34.
  • the plasma generator 34 includes a first electrode 36 and a second electrode 52.
  • the first electrode 36 is configured for electrical coupling to a current and voltage source 44.
  • the second electrode 52 is spaced apart from and disposed in electrical discharge communication with the first electrode 36 through the internal space 26.
  • the second electrode 52 is a ground electrode.
  • a reaction zone 32 is defined within the fluid passage portion 64 between the first electrode 36 and the second electrode 52.
  • the downstream fluid passage portion 74 extends downstream from within the reaction zone 32.
  • the upstream fluid passage portion 66 is disposed upstream of the reaction zone 32.
  • the first electrode 36 is at least partially disposed in the downstream fluid passage portion 74 and is spaced apart from an internal conduit wall 76, which defines the downstream fluid passage portion 74 to define a fluid flow space 741 in the downstream fluid passage portion 74 between the first electrode 36 and the internal conduit wall 76.
  • the ratio of the diameter D3 of the first electrode 36 to the diameter D4 of the downstream fluid passage portion 74 is between two (2) and five (5). For example, in some embodiments, this ratio is three (3).
  • the second electrode 52 includes an operative second electrode surface portion 54.
  • the effected electrical discharge is between the first electrode 36 and the operative second electrode surface portion 54 and at least a fraction of the plasma forming gaseous fluid is converted into a plasma 102.
  • the reaction zone 32 is provided in an internal space 26 defined by an internal surface 28 of the reactor 10, and the operative second electrode surface portion 54 is the electrically conductive surface portion of the internal surface 28 which is closest to the first electrode 36.
  • the upstream fluid passage portion 66 is defined by an upstream conduit wall 68 disposed upstream of the reaction zone 32.
  • the upstream conduit wall 68 includes at least one electrically conductive upstream conduit wall portion 70. Any electrically conductive upstream conduit wall portion 70, which is disposed in electrical discharge communication with the first electrode 36, is disposed further from the first electrode 36 than the operative second electrode surface portion 54.
  • the upstream conduit wall 68 includes an upstream solid particulate deposition susceptible conduit wall portion 72 configured for becoming coupled to solid particulate upon approach of the solid particulate to the upstream solid particulate deposition susceptible conduit wall portion 72.
  • the downstream fluid passage portion 74 is defined by a downstream internal conduit surface 76 including a downstream solid particulate deposition susceptible conduit surface portion 78.
  • the downstream solid particulate deposition susceptible conduit surface portion 78 is configured for becoming coupled to solid particulate upon approach of the solid particulate to the downstream solid particulate deposition susceptible conduit surface portion 78.
  • the method includes contacting reactant matter with a plasma in a reaction zone 32 to effect production of product matter including solid particulate such as carbon-comprising particulate.
  • the solid particulate is carbon particulate.
  • the plasma is plasma generated by providing a plasma forming fluid in the reaction zone 32, and applying a sufficient electrical potential difference between the first electrode 36 and the operative second electrode surface portion 54, so as to effect an electrical discharge between the first electrode 36 and the second electrode 52 (and, in some embodiments, the operative second electrode surface portion 54) and through the reaction zone 32.
  • a sufficient electrical potential difference between the first electrode 36 and the operative second electrode surface portion 54 so as to effect an electrical discharge between the first electrode 36 and the second electrode 52 (and, in some embodiments, the operative second electrode surface portion 54) and through the reaction zone 32.
  • the plasma forming fluid includes a plasma forming fluid flow.
  • the plasma forming fluid includes reactant matter.
  • the reactant matter includes natural gas.
  • the reactant matter includes methane.
  • the downstream fluid passage portion 74 is defined by a downstream internal conduit surface 76 including a downstream solid particulate deposition susceptible conduit surface portion 78.
  • the downstream solid particulate deposition susceptible conduit surface portion 78 is configured for becoming coupled to the produced solid particulate upon approach of the produced solid particulate to the downstream solid particulate deposition susceptible conduit surface portion 78 Amongst other things, the carrier fluid flow mitigates against such deposition.
  • the minimum velocity of carrier fluid flow is 0.5 metres per second to 0.6 metres per second for flow through the downstream fluid passage portion 74 having an internal diameter of 0.3 inches.
  • at least a fraction of the carrier fluid flow is derived from the plasma forming fluid flow.
  • a reactor 10 configured for generating a plasma, which, amongst other things, effects increased service life of the electrode.
  • the reactor 10 includes an internal space 26 defining a fluid passage portion 64 for flowing a plasma forming gaseous fluid.
  • the fluid passage portion 64 includes a reaction zone 32.
  • the reactor 10 also includes a plasma generator 34.
  • the plasma generator 34 includes a first electrode 36 and a second electrode 52.
  • the first electrode 36 is configured for electrical coupling to a current and voltage source 44, and includes an operative first electrode surface portion 38.
  • the second electrode 52 is spaced apart from and disposed in electrical discharge communication with the first electrode 36 through the internal space 26, and includes an operative second electrode surface portion 54.
  • the second electrode 52 is a ground electrode.
  • the reaction zone 32 is disposed between the first and second electrodes 36, 52.
  • an operative distance D5 is defined along the longitudinal axis 36 of the first electrode 36 between: (i) a plane in which is disposed an axis normal to the operative first electrode surface portion 38, and (ii) a tip 100 of the first electrode 36, disposed downstream of the operative first electrode surface portion 38, wherein the operative distance D5 is at least 0.25 inches.
  • the operative distance D5 is less than 1.25 inches.
  • the operative distance D5 is one inch.
  • the reaction zone 32 is provided in an internal space 26 defined by an internal surface 28 of the reactor 10, and the operative second electrode surface portion 54 is the electrically conductive surface portion of the internal surface 28 which is closest to the first electrode 36.
  • the method includes contacting reactant matter with a plasma in a reaction zone 32 to effect production of product matter including solid particulate.
  • the plasma is plasma generated by providing a plasma forming fluid in the reaction zone 32, and applying a sufficient electrical potential difference between the first electrode 36 and the operative second electrode surface portion 54, so as to effect an electrical discharge between the first electrode 36 and the operative second electrode surface portion 54 and through the reaction zone 32.
  • a sufficient electrical potential difference between the first electrode 36 and the operative second electrode surface portion 54, so as to effect an electrical discharge between the first electrode 36 and the operative second electrode surface portion 54 and through the reaction zone 32.
  • the plasma forming fluid includes a plasma forming fluid flow.
  • the plasma forming fluid includes reactant matter.
  • the reactant matter includes natural gas.
  • the reactant matter includes methane.
  • the plasma 102 is generated in the reaction zone 32, and the pressure in the reaction zone 32 is at least 75 psig.
  • the pressure in the reaction zone 32 is at least 75 psig.
  • a reactor 10 configured for generating a plasma, which, amongst other things, includes a heat exchanger 18 for effecting heating of plasma forming fluid being introduced into the reactor 10.
  • a reactor 10 including an internal space 26 including a reaction zone 32.
  • the reactor includes an inlet 20 fluidly coupled to the reaction zone 32 with a fluid introduction passage 24 for introducing a plasma forming gaseous fluid into the reaction zone 32.
  • the reactor 10 also includes a plasma generator 34.
  • the plasma generator 34 includes a first electrode 36 and a second electrode 52.
  • the first electrode 36 is configured for electrical coupling to a current and voltage source 44.
  • the second electrode 52 is spaced apart from and disposed in electrical discharge communication with the first electrode 36 through the internal space 26.
  • the reaction zone 32 is disposed between the first and second electrodes 36, 52.
  • the reaction vessel 12 includes a heat exchanger 18 disposed in heat transfer communication with the fluid introduction passage 24 for effecting heat transfer to plasma forming gaseous fluid being introduced to the reaction zone 32.
  • the heat exchanger 18 includes an induction heater.
  • the method includes contacting reactant matter with a plasma in a reaction zone 32 to effect production of product matter.
  • the plasma is plasma generated by providing a plasma forming fluid in the reaction zone 32, and applying a sufficient electrical potential difference between the first electrode 36 and the second electrode 52, so as to effect an electrical discharge between the first electrode 36 and the second electrode 52 and through the reaction zone 32.
  • a sufficient electrical potential difference between the first electrode 36 and the second electrode 52 so as to effect an electrical discharge between the first electrode 36 and the second electrode 52 and through the reaction zone 32.
  • the plasma forming fluid is heated by the heat exchanger 18.
  • the plasma forming fluid is heated by the heat exchanger 18 to a temperature of between 400°C and 700°C from any defined temperature.
  • the plasma forming fluid includes a plasma forming fluid flow.
  • the plasma forming fluid includes reactant matter.
  • the reactant matter includes natural gas.
  • the reactant matter includes methane.
  • Another aspect is provided relating to the method of operating a plasma reactor 10. Amongst other things, this aspect effects heat transfer from an electrode at a sufficiently desirable rate so as to mitigate against providing high temperatures at the electrode which would facilitate deposition of solid particulate at the electrode.
  • a plasma reactor 10 including an internal surface 28 defining an internal space 26 including a reaction zone 32.
  • the plasma reactor also includes a plasma generator 34.
  • the plasma generator 34 includes a first electrode 36 and a second electrode 52.
  • the first electrode 36 is configured for electrical coupling to a current and voltage source 44.
  • the second electrode 52 is spaced apart from and disposed in electrical discharge communication with the first electrode 36 through the internal space 26.
  • the second electrode 52 is a ground electrode.
  • the reaction zone 32 is disposed between the first and second electrode 36, 52.
  • a plasma forming gaseous fluid is provided within the reaction zone 32.
  • the plasma reactor 10 includes a pressure boundary 960, which includes an internal surface portion 96 adjacent to and in thermal communication with the reaction zone 32, and which also defines an extemalmost surface 962 which is disposed in heat transfer relationship with the outside environment 1000 (ie. the atmosphere).
  • the internal surface portion 96 is defined by the second electrode 52.
  • the material of the pressure boundary 960 is characterized by an average heat transfer coefficient of at least 100 W / (meter-Kelvin). In some embodiments, for example, this average heat transfer coefficient is between 100 W / (meter-Kelvin) and 200 W / (meter-Kelvin). In some embodiments, for example, this average heat transfer coefficient is 173 W / (meter-Kelvin).
  • the pressure boundary 960 includes a heat transfer medium 94.
  • the heat transfer medium 94 includes steel wool. In other embodiments, for example, the heat transfer medium includes copper.
  • the plasma forming fluid includes a plasma forming fluid flow.
  • the plasma forming fluid includes reactant matter.
  • the reactant matter includes natural gas.
  • the reactant matter includes methane.

Abstract

There is provided a reactor, defining a fluid passage portion for flowing a plasma forming gaseous fluid, wherein the fluid passage portion includes an upstream fluid passage portion and a downstream fluid passage portion, comprising a plasma generator. The plasma generator includes a first electrode configured for electrical coupling to a current and voltage source, and a second electrode spaced apart from and disposed in electrical discharge communication with the first electrode through the internal space. The reaction zone is defined between the first electrode and the second electrode, and the downstream fluid passage portion extends downstream from within the reaction zone, and the upstream fluid passage portion is disposed upstream of the reaction zone. When the plasma forming gaseous fluid is disposed within the reaction zone and a sufficient electrical potential difference is applied between the first electrode and the second electrode, an electrical discharge is effected between the first electrode and the second electrode and through the reaction zone, and at least a fraction of the plasma forming gaseous fluid is converted into a plasma.

Description

PLASMA REACTOR AND METHOD OF OPERATION THEREOF
RELATED APPLICATIONS
[0001] This application claims the benefits of priority under 35 U.S.C. 119 (e) to U.S. Provisional Patent Application Serial No. 61/432,794, filed on January 14, 2011.
FIELD
[0002] The present disclosure relates to effecting reactions in a plasma. BACKGROUND
[0003] Plasma based reactions for effecting reformation of natural gas are known. However, existing methods operate with less than desirable conversion efficiencies and are plagued with issues of carbon deposition.
SUMMARY
[0004] In one aspect, there is provided method of operating a plasma reactor including a reaction zone. The method includes generating a plasma in the reaction zone, and contacting reactant matter with the plasma in the reaction zone, wherein the pressure in the reaction zone is at least 75 psig.
[0005] In another aspect, there is provided a reactor, defining an internal space including a reaction zone, and includes a plasma generator. The plasma generator includes first and second electrodes. The first electrode is configured for electrical coupling to a current and voltage source. The second electrode is spaced apart from and disposed in electrical discharge communication with the first electrode through the internal space, and includes an operative second electrode surface portion. The reaction zone is disposed between the first and second electrodes. When a plasma forming gaseous fluid is disposed within the reaction zone and a sufficient electrical potential difference is applied between the first electrode and the operative second electrode surface portion, an electrical discharge is effected between the first electrode and the operative second electrode surface portion and through the reaction zone, and at least a fraction of the plasma forming gaseous fluid is converted into a plasma. The operative second electrode surface portion is defined by a radius of curvature of less than 0.002 inches.
[0006] In another aspect, there is provided a reactor including an internal surface defining an internal space including a reaction zone. The reactor includes a plasma generator. The plasma generator includes first and second electrodes. The first electrode is configured for electrical coupling to a current and voltage source. The second electrode is spaced apart from and disposed in electrical discharge communication with the first electrode through the internal space, and includes an operative second electrode surface portion. The reaction zone is disposed between the first electrode and the operative second electrode surface portion. When a plasma forming gaseous fluid is disposed within the reaction zone and a sufficient electrical potential difference is applied between the first electrode and the operative second electrode surface portion, an electrical discharge is effected between the first electrode and the operative second electrode surface portion and through the reaction zone, and at least a fraction of the plasma forming gaseous fluid is converted into a plasma. The first electrode is mounted within a reaction vessel with a mounting structure including an internal mounting structure surface defining a portion of the internal surface, wherein the mounting surface is disposed in fluid communication with the reaction zone. The minimum distance between the operative second electrode surface and the mounting structure is at least two (2) inches.
[0007] In another aspect, there is provided a reactor, defining a fluid passage portion for flowing a plasma forming gaseous fluid, wherein the fluid passage portion includes an upstream fluid passage portion and a downstream fluid passage portion. The reactor includes a plasma generator. The plasma generator includes first and second electrodes. The first electrode is configured for electrical coupling to a current and voltage source. The second electrode is spaced apart from and disposed in electrical discharge communication with the first electrode through the internal space, and includes an operative second electrode surface portion. The reaction zone is defined between the first electrode and the operative second electrode portion, and the downstream fluid portion extends downstream from within the reaction zone. When the plasma forming gaseous fluid is disposed in the reaction zone and a sufficient electrical potential difference is applied between the first electrode and the operative second electrode surface portion, an electrical discharge is effected between the first electrode and the operative second electrode surface portion and through the reaction zone, and at least a fraction of the plasma forming gaseous fluid is converted into a plasma. The operative second electrode surface portion is spaced apart from the first electrode by a minimum distance of less than 0.15 inches. The upstream fluid passage portion is defined by an upstream conduit wall disposed upstream of the reaction zone, wherein the upstream conduit wall includes at least one electrically conductive upstream conduit wall portion. Any electrically conductive upstream conduit wall portion, which is disposed in electrical discharge communication with the first electrode, is disposed further from the first electrode than the operative second electrode surface portion. The operative second electrode surface portion is disposed in thermal communication with at least one electrically conductive upstream conduit wall portion.
[0008] In another aspect, there is provided, a reactor, defining a fluid passage portion for flowing a plasma forming gaseous fluid, wherein the fluid passage portion includes an upstream fluid passage portion and a downstream fluid passage portion. The reactor includes a plasma generator. The plasma generator includes first and second electrodes. The first electrode is configured for electrical coupling to a current and voltage source. The second electrode is spaced apart from and disposed in electrical discharge communication with the first electrode through the internal space. The reaction zone is defined between the first electrode and the second electrode, and the downstream fluid passage portion extends downstream from within the reaction zone, and the upstream fluid passage portion is disposed upstream of the reaction zone. When the plasma forming gaseous fluid is disposed within the reaction zone and a sufficient electrical potential difference is applied between the first electrode and the second electrode, an electrical discharge is effected between the first electrode and the second electrode and through the reaction zone, and at least a fraction of the plasma forming gaseous fluid is converted into a plasma. The first electrode is at least partially disposed in the downstream fluid passage portion and is spaced apart from an internal conduit wall of the downstream fluid passage portion to define a fluid flow space in the downstream fluid passage portion, wherein, in any plane which intersects that portion of the first electrode disposed in the downstream fluid passage portion, and which is disposed in a normal orientation relative to an axis of the downstream fluid passage portion being intersected, the ratio of the diameter of the first electrode to the diameter of the downstream fluid passage portion is between two (2) and five (5).
[0009] In another aspect, there is provided a reactor, including an internal space defining a fluid passage portion for flowing a plasma forming gaseous fluid, wherein the fluid passage portion includes a reaction zone. The reactor includes a plasma generator. The plasma generator includes first and second electrodes. The first electrode is configured for electrical coupling to a current and voltage source, and including an operative first electrode surface portion. The second electrode is spaced apart from and disposed in electrical discharge communication with the first electrode through the internal space, and including an operative second electrode surface portion. The reaction zone is disposed between the first and second electrodes. When a plasma forming gaseous fluid is disposed within the reaction zone and a sufficient electrical potential difference is applied between the operative first electrode surface portion and the operative second electrode surface portion, an electrical discharge is effected between the operative first electrode surface portion and the operative second electrode surface portion and through the reaction zone, and at least a fraction of the plasma forming gaseous fluid is converted into a plasma. An operative distance is defined along the longitudinal axis of the first electrode between: (i) a plane in which is disposed an axis normal to the operative first electrode surface portion and (ii) a tip of the first electrode downstream of the operative first electrode surface portion, wherein the operative distance is at least 0.25 inches.
[0010] In another aspect, there is provided a reactor, defining an internal space including a reaction zone, and including an inlet fluidly coupled to the reaction zone with a fluid introduction passage for introducing a plasma forming gaseous fluid into the reaction zone. The reactor includes a plasma generator. The plasma generator includes first and second electrodes. The first electrode is configured for electrical coupling to a current and voltage source. The second electrode is spaced apart from and disposed in electrical discharge communication with the first electrode through the internal space. The reaction zone is disposed between the first and second electrodes. When a plasma forming gaseous fluid is disposed within the reaction zone and a sufficient electrical potential difference is applied between the first electrode and the second electrode, an electrical discharge is effected between the first electrode and the second electrode and through the reaction zone, and at least a fraction of the plasma forming gaseous fluid is converted into a plasma. The reaction vessel includes a heat exchanger disposed in heat transfer communication with the fluid introduction passage for effecting heat transfer to plasma forming gaseous fluid being introduced to the reaction zone.
BRIEF DESCRIPTION OF THE DRAWINGS
[0011] The apparatus and method of the preferred embodiments of the invention will now be described with the following accompanying drawings:
[0012] Figure 1 is a schematic illustration of an embodiment of an electric circuit for effecting a high voltage power supply to a reactor;
[0013] Figure 2 is a schematic illustration of a sectional, front elevation view of an embodiment of the reactor;
[0014] Figure 3A is an exploded sectional view of the high voltage feedthrough assembly of the reactor in Figure 1 ;
[0015] Figure 3B is an exploded sectional view of a lower portion of the reactor in Figure 2;
[0016] Figure 4 is a sectional detailed front elevation fragmentary view of an upper portion of the reactor in Figure 2;
[0017] Figure 5 is a sectional detailed front elevation fragmentary view of a lower portion of the reactor in Figure 2; [0018] Figure 6 is a sectional detailed front elevation exploded view of the lower portion of the reactor in Figure 2;
[0019] Figure 7 is a schematic illustration of a sectional, front elevation view of another embodiment of the reactor;
[0020] Figure 8 is the same view as in Figure 2, and illustrates the dimension Dl , which is the minimum distance between the operative second electrode surface portion and the mounting surface within the reactor.
[0021] Figure 9 is a sectional detailed front elevation fragmentary view of a lower portion of the reactor in Figure 2, and illustrates the dimension D2, which is the minimum distance by which the operative second electrode surface portion is spaced apart from the first electrode within the reactor.
[0022] Figures 10 and 11 illustrate the relationship between dimensions D3, which is the diameter of the first electrode, and D4, which is the diameter of the downstream fluid passage portion, wherein Figure 10 is the same view as in Figure 5 and also illustrates generated plasma, and Figure 11 is a cross-sectional view of the downstream fluid passage portion taken along plane 200; and
[0023] Figure 12 is the same view as in Figure 5 and also illustrates generated plasma, and also illustrates the dimension D5, which is an operative distance defined along the longitudinal axis of the first electrode between: (i) a plane in which is disposed an axis normal to the operative first electrode surface portion, and (ii) the tip of the first electrode.
DETAILED DESCRIPTION
[0024] Referring to Figures 1 to 12, there is provided a reactor 10 configured for generating a plasma.
[0025] Referring to Figure 2, the reactor 10 includes an internal space 26 including a reaction zone 32. The reactor 10 also includes a plasma generator 34. The plasma generator 34 includes a first electrode 36 and a second electrode 52. The first electrode 36 is configured for electrical coupling to a current and voltage source 44. The second electrode 52 is spaced apart from and disposed in electrical discharge communication with the first electrode 36 through the internal space 26. In some embodiments, for example, the second electrode 52 is a ground electrode. The reaction zone 32 is disposed between the first electrode 36 and the second electrode 52. When the plasma forming gaseous fluid is disposed within the reaction zone 32 and a sufficient electrical potential difference is applied between the first electrode 36 and the second electrode 52, an electrical discharge is effected between the first electrode 36 and the second electrode 52 and through the reaction zone 32, and at least a fraction of the plasma forming gaseous fluid is converted into a plasma.
[0026] In some embodiments, the internal space 26 includes a fluid passage portion 64 for flowing a plasma forming gaseous fluid through the reaction zone 32. For example, in some embodiments, the fluid passage portion 64 includes an upstream fluid passage portion 66 disposed upstream of the reaction zone 32, and also includes a downstream fluid passage portion 74 extending downstream from within the reaction zone 32.
[0027] With respect to the second electrode 52, in some embodiments, for example, the second electrode 52 includes an operative second electrode surface portion 54. When the plasma forming gaseous fluid is disposed within the reaction zone 32 and a sufficient electrical potential difference is applied between the first electrode 36 and the operative second electrode surface portion 54, the effected electrical discharge is between the first electrode 36 surface and the operative second electrode surface portion 54 and at least a fraction of the plasma forming gaseous fluid is converted into a plasma. In this respect, in some embodiments, for example, the reaction zone 32 is provided in an internal space 26 defined by an internal surface 28 of the reactor 10, and the operative second electrode surface portion 54 is an electrically conductive surface portion of the internal surface 28 that is closest to the first electrode 36.
[0028] In some embodiments, the reactor 10 includes a reaction vessel 12, and the first electrode 36 is mounted within the reaction vessel 12 with a mounting structure 46. In some embodiments, for example, the reaction vessel is constructed of stainless (such as 304 stainless steel, or 316 stainless steel). In some embodiments, for example, standard pipe flange connections are provided to effect coupling to feed and exhaust systems.
[0029] In some embodiments, the first electrode 36 is electrically coupled to the current and voltage source 44. For example, with respect to the current and voltage source 44, the frequency of the current and voltage source 44 is from lOKHz to 20KHz, and the pulse width of the current and voltage source 44 is from 10 to 20 micro-seconds. An exemplary electrical circuit for effecting a high voltage power supply to the first and second electrodes 36, 52 is illustrated in Figure 1. The first electrode 36 is electrically connected to a power supply. The power supply 2011 includes a rectifier 2013, a pulser 2015 (or inverter), a high voltage pulse transformer 2017, and, optionally, high voltage capacitors 2019 connected in series with the secondary winding of the pulse transformer 2017. The high voltage capacitors 2019 function in multi-discharge generation and for impedance matching, and, in this respect, allow simultaneous powering of multiple electrodes by a single power source, such as various embodiments of the reactor 10 which are described and illustrated in Canadian Patent Application No. 2,516,499 which is herein incorporated by reference in its entirety. The high voltage capacitors 2019 can be omitted under single discharge conditions. The power supply provides controlled bipolar high voltage pulses to a high voltage transformer which acts as a filter to make the current almost sinusoidal. For example, switching frequencies are between 10 kHz to 20 kHz, such as between 15 kHz to 17 kHz. For example, the pulse widths are between 10 to 20 microseconds, such as between 15 to 17 microseconds. For example, in operation, a stable flow of plasma forming gaseous fluid is established through the reactor vessel, and once substantially all of the ambient air has been purged from the reaction vessel 12, a high voltage pulse is supplied to the first electrode 36, and plasma is created in the reaction zone 32 between the first electrode 36 and the second electrode 52.
[0030] For example, with respect to the first electrode 36 and the second electrode 52, each one of these electrodes is electrically conductive and is configured to operate robustly in high temperature conditions. [0031] For example, with respect to the first electrode 36, the first electrode 36 includes a lanthanated tungsten rod. Other examples of suitable materials for the first electrode 36 structure include substantially pure tungsten, 2% thoriated tungsten, tungsten carbide, and other tungsten alloys.
[0032] Referring to Figures 2, 3A, and 4, in some embodiments, for example, the first electrode 36 is electrically coupled to the voltage and power source through a high voltage feedthrough assembly 300. The high voltage feedthrough assembly (HVFA) 300 is configured to provide high voltage (HV) power to the first electrode 36 and to contain any pressurized gas within the reaction vessel 12. The HVFA 300 is configured to operate continuously at 20 kV and 20 kHz and at a working pressure of 300psig. A set of releasably coupled flanges 302, 121 provide for access to the HVFA.
[0033] In some embodiments, the HVFA 300 is composed of a top flange 302, an insulator 304, a high voltage input conductor 306, a threaded insert 308, a high voltage conductor holder 310, and an alignment ring 312. The HVFA defines an upper reaction vessel portion 1202 of the reaction vessel 12.
[0034] The top flange 302 is provided for holding the HVFA 300 while simultaneously ensuring a hermetic seal for the reaction vessel 12. The top flange 302 maintains the integrity of coupling between the HVFA 300 and the remaining portion of the reaction vessel 12 when pressurized gas is provided within the reaction vessel 12.
[0035] The insulator 304 provides electrical insulation between the metallic high voltage and grounding components of the reactor 10 and contains the pressure inside the reaction vessel 12. For example, the material of the insulator 304 is MACOR™ made by Corning Incorporated. The insulator carries two (2) o-ring seals 314, 316 that provide a positive seal with the top flange 302. The high voltage feed conductor 306 extends through a passage provided through the center of the insulator 304.
[0036] The high voltage input conductor 306 is electrically coupled to the first electrode 36 and is provided for conducting high voltage power to the first electrode 36. The high voltage input conductor 306 also provides a pressure barrier to gas pressure within the reaction vessel 12. There are two (2) o-rings 318, 320 carried by the larger, middle section of the high voltage input conductor 306. The high voltage input conductor 306 is made from stainless steel but can be made from any conductive metal that is compatible with the fluid used and that is rated for the operating pressure. The first electrode 36 is attached to the high input conductor 306 by friction fit within a hole 322 provided in the high voltage input conductor 306. The hole 322 is sized slightly smaller than the first electrode 36 and is drilled inside the high voltage input conductor 306. Slits are formed on the side to allow the wall to expand slightly, when the first electrode 36 is inserted.
[0037] The high voltage input conductor 306 is coupled to the insulator 304 by the threaded insert 308. In some embodiments, for example, the threaded insert 308 is manufactured from Teflon™ made by E. I. du Pont de Nemours and Company.
[0038] The high voltage conductor holder 310 maintains positioning of the high voltage input conductor 306 at the center of the assembly 300 and includes a passage through which the high voltage input conductor 306 extends. The holder 310 also provides electrical insulation between the high voltage input conductor 306 and the internal surface 28 of reaction vessel 12. In some embodiments, for example, the high voltage conductor holder 310 is made from Teflon™. The high voltage conductor holder 310 is supported by the alignment ring 312.
[0039] The alignment ring 312 supports the high voltage conductor holder 310 and provides a seal between the flanges 302, 121 . In some embodiments, for example, the alignment ring 312 is made from stainless steel.
[0040] Assembly of an embodiment of the reactor 10 will now be described. The reactor includes the upper reaction vessel portion 122, an intermediate reaction vessel portion 124, and a lower reaction vessel portion 126.
[0041] The intermediate reaction vessel portion 124 includes a second electrode assembly 1244 coupled to and disposed internally within an intermediate containment component 1242. The second electrode assembly 1244 includes a second electrode- comprising structure 1246 (for example, made from tungsten), a containment structure
1248 (for example, made from stainless steel), an upper sleeve 1250 (for example, made from tungsten), a lower sleeve 1252 (for example, made from tungsten), a heat transfer medium 94 (for example, steel wool), and an insulator 1254 (for example, made from MACOR™. The second electrode— comprising structure includes the second electrode 52. The combination of the upper and lower sleeves 1250, 1252 define at least a portion of the downstream fluid passage portion extending from the within the reaction zone 32. The heat transfer medium 94 is provided to effect dissipation of heat from an internal surface portion 96, of a downstream internal conduit surface 76, adjacent to the reaction zone 32. The insulator 1254 is disposed downstream of the heat transfer medium 94, and is provided for mitigating heat transfer from a downstream fluid passage portion 74 so as to assist in sustaining reactive processes within the plasma, as described below.
[0042] The assembly of the second electrode assembly 1244 is now described. The upper sleeve 1250 is seated on a seating surface provided on the lower sleeve (see Detail "A" in Figure 6). The second electrode-comprising structure 1246 is then seated on the upper sleeve 1250, and this intermediate assembly is then inserted into a receiving space
1249 defined within the containment structure 1248 to provide a second intermediate assembly, such that the second-electrode comprising structure 1246 is seated on the containment structure 1248. A set screw is inserted through passage 1266 and tightened against the lower sleeve 1252 to effect desired positioning of the lower sleeve 1252 relative to the containment structure 1248. The second electrode-comprising structure 1246 is then removed from the second intermediate assembly, and the insulator 1254 is inserted into space provided between the containment structure 1248 and the lower sleeve 1252, such that sufficient space remains for receiving the heat transfer medium 94 between the sleeves 1250, 1252 and the containment structure 1248. The heat transfer medium 94 is then inserted into this remaining space in a well-packed condition. The second electrode-comprising structure 1246 is then returned, and positioned such that the second electrode-comprising structure 1246 is seated on the upper sleeve 1250, the heat transfer medium 94, and the containment structure 1248. A set screw is inserted through passage 1264 and then tightened against the second electrode-comprising structure to effect its desired positioning relative to the containment structure 1248. [0043] The second electrode assembly 1244 is then inserted into a receiving space 1257 defined within the intermediate containment component 1242, and threadably coupled to the intermediate containment component 1242 by co-operative threads 1260, 1262 (see Figure 3B) provided on the second electrode assembly 1244 and the intermediate containment component 1242, respectively. Positioning of the second electrode assembly 1244, and, therefore, the second electrode 52 and the operative second electrode portion 54, is adjusted by rotating the second electrode assembly 1244 relative to the intermediate containment component 1242 while the second electrode assembly 1244 is threadably engaged to the intermediate containment component 1242.
[0044] The upper reaction vessel portion 122, defined by the HVFA 300, is integrated into the reactor 10 by coupling to the assembled intermediate reaction vessel portion 124. The insulator/pressure barrier 304 with its two (2) o-rings 314, 316 in place is inserted from below into the upper reaction vessel portion flange 302, making sure it is firmly in contact with the flange 302. The high voltage input conductor 306, with its two (2) o-rings installed 318, 320, is inserted through the passage provided in the insulator/pressure barrier 304. The larger diameter section of the high voltage input conductor 306 is firmly seated against the insulator/pressure barrier 304. The threaded insert 308 is screwed into the insulator/pressure barrier 304 to hold the high voltage input conductor 306 in place. The high voltage conductor holder 310 is then inserted into the alignment ring and this assembly is inserted through the top of and into the flanged lower reaction vessel portion 13. The flange 302 is coupled to a intermediate reaction vessel portion upper flange 121 of the intermediate containment component 1242, with the alignment ring 312 disposed in-between the two flanges 302, 121. Bolts and nuts are inserted in each flange hole and tightened appropriately to effect coupling of the HVFA 300 to the intermediate containment component 1242.
[0045] The lower reaction vessel portion 126 is then coupled to the intermediate reaction vessel portion 124. The lower reaction vessel portion 126 includes the outlet 22. A lower reaction vessel portion flange 1261 of the lower reaction vessel portion 126 is connected to an intermediate reaction vessel portion lower flange 1256 using bolts and nuts. [0046] For example, with respect to the second electrode 52, the second electrode 52 is made from stainless steel. Other examples of suitable materials include lanthanated tungsten, substantially pure tungsten, 2% thoriated tungsten, tungsten carbide, other tungsten alloys, graphite, or silicon carbide.
[0047] For example, with respect to the plasma forming gaseous fluid, the plasma forming gaseous fluid is any one of those fluids that can be ionized through electron impact events within a voltage potential gradient, and thereby create a reduced impedance pathway that provides a current path. Any ionisable fluid can form a plasma provided that a sufficient electric potential gradient exists. Such ionisable fluids include, but are not limited to, elemental species such as the noble gases (He, Ne, Ar, etc.), molecular gases (i.e. H2, 02, 03, CH4, CF4, SF6, H2S, etc.) and vaporizable organic liquids (i.e. butane, hexane), organometallic liquids (i.e. tetaethoxysilane, trimethylphosphine, etc) and inorganic liquids (water, TiCl4). For example, the plasma forming gaseous fluid includes no gaseous oxygen or substantially no gaseous oxygen.
[0048] For example, with respect to the reactor 10, the reactor 10 includes an inlet 20 configured for introducing the plasma forming gaseous fluid flow to the plasma generator 34 so as to effect the plasma discharge into the reaction zone 32 by the plasma generator 34 such that the plasma discharge facilitates conversion of reactant matter in the reaction zone 32 into product matter.
[0049] As a further example with respect to the reactor 10, the reactor 10 is configured for receiving reactant matter within the reaction zone 32. For example, the reactant matter is in the form of a fluid, such as a gaseous fluid, and the reactor includes the inlet 20 for introducing reactant matter fluid as reactant matter fluid flow into the reaction zone 32. In the illustrated embodiment, the inlet 20 for the plasma forming gaseous fluid flow is the same as the inlet 20 for the reactant matter fluid flow as the plasma forming gaseous fluid is the same as the reactant matter fluid. For example, the plasma forming gaseous fluid flow, when it is the same as the reactant matter fluid flow, is introduced through the inlet 20 at a flow rate of 3.5 cubic metres per hour. [0050] For example, with respect to the reactant matter, the reactant matter consists of any one of: (i) an element, (ii) a compound, (iii) a homogeneous or inhomogeneous mixture of any one of: (a) at least two elements, or (b) at least two compounds, or (iv) a homogeneous or inhomogeneous mixture of any combination of: (a) at least one element, and (b) at least one compound.
[0051] As a further example, with respect to the reactant matter, the reactant matter, which is suitable for conversion within the plasma generated by the plasma generator 34 includes gaseous and liquid hydrocarbons such as natural gas, volatile petroleum fractions, landfill and other bio-generated fuel gases, methane, ethane, propane, propene, butane, pentane, and hexane, and volatile oxygenated organic compounds such as methanol, and ethanol, and reactive molecular element species such as, but not limited to, hydrogen, oxygen and ozone, and volatile inorganic hydrides such as, but not limited to, H2S, SiH4, PH3 , and As¾. In some embodiments, for example, the reactant matter includes syngas (carbon dioxide and methane). At least a fraction of the reactant matter is subjected to a reactive process in the plasma generated by the plasma generator 34, such that the reactive process effects creation of product matter.
[0052] For example, with respect to the product matter, the product matter includes solid particulate matter. For example, the solid particulate matter includes carbon- comprising matter, such as carbon. For example, with respect to the solid particulate matter of the product matter, at least a fraction of the solid particulate matter of the product matter becomes coupled to an internal surface 28 of the reaction vessel 12. The solid particulate matter is said to be coupled to the internal surface 28 when the solid particulate matter adheres to the internal surface 28 or becomes associated with solid matter which is already adhered to the internal surface 28. Mechanisms for association of the solid particulate matter with the solid matter adhered to the internal surface 28 include absorption, dissolution, covalent bonding, or ionic bonding. The operative forces, whose action effects the adhesion or the association, include any one of, or any combination of, Van der Waals adhesive forces, electrostatic forces, and gravity. [0053] For example, with respect to the plasma forming gaseous fluid, the plasma forming gaseous fluid includes the reactant matter. In this respect, for example, the plasma forming gaseous fluid includes any of the suitable reactant matter described above.
[0054] As a further example, with respect to the plasma forming gaseous fluid including the reactant matter, a suitable plasma forming gaseous fluid is natural gas, typically including 70 mole % to 95 mole % methane, based on the total number of moles of plasma forming gaseous fluid, with small amounts of other hydrocarbons such as ethane and propane and varying levels of inert gases such as nitrogen and contaminant gases such as hydrogen sulphide. For example, these fluids are introduced into the plasma reactor 10 at flows that can vary between very low (lO's of cc/min) to very high (lO's of Nm /hour). The plasma forming gaseous fluid is provided within the reaction zone 32. For example, natural gas feed flow to the reactor 10 ranges between 0.1 Nm /hour and 10 Nm3/hour. For example, the reaction is carried out at pressures that may range from medium vacuum (100's of Torr) to atmospheric and relatively high pressures (i.e. up to at least 300 psig). In this respect, for example, the reaction is carried out at a pressure of 150 psig. For example, once the plasma has been initiated, the system temperature is allowed to equilibrate to accommodate the small zone of very high (1000-1500°C) temperature in the plasma plume. For example, internal wall temperatures of the reactor 10 may be as high as 500°C. Depending on the reactant matter, the reactant matter of the plasma forming gaseous fluid is converted in the reaction zone 32 in accordance with any one of or any combination of the reaction steps described in Appendix "A".
[0055] In this respect, the conversion of the reactant matter of the plasma forming gaseous fluid results in product matter including solid particulate matter, wherein the solid particulate matter includes carbon.
[0056] In some embodiments, for example, the reactor 10 includes an outlet 22 configured for discharging the product matter. In some embodiments, the reaction vessel 12 also includes a heat exchanger disposed in thermal communication with the outlet 22 and configured for effecting heat transfer from the product matter discharging through the outlet 22. Such heat transfer effects cooling of the discharging product matter. For example, such heat transfer could effect heating of the plasma forming gaseous fluid before the plasma- forming gaseous fluid is introduced into the reaction vessel 12. In this respect, the heat exchanger is configured to receive the plasma-forming gaseous fluid and effect heat transfer from the discharging product matter and to the plasma-forming gaseous fluid.
[0057] Referring to Figure 10, in some embodiments, for example, an internal surface portion 96, of a downstream internal conduit surface 76, adjacent to the reaction zone 32, is disposed in thermal communication with a heat transfer medium 94 extending between the reaction zone adjacent internal surface portion 96 and an external surface 98 of the reactor for effecting dissipation of heat from the internal surface portion 96. In some embodiments, for example, the heat transfer medium 94 is steel wool.
(A) OPERATING AT HIGHER PRESSURES
[0058] One aspect is associated with a method of operating a plasma reactor 10. The plasma reactor 10 includes a reaction zone 32. The method includes contacting reactant matter with a plasma 102 in a reaction zone 32. For example, the plasma 102 is generated in the reaction zone 32. The pressure in the reaction zone 32 is at least 75 psig. In some embodiments, for example, the pressure in the reaction zone 32 is greater than 300 psig. In other embodiments, for example, the pressure in the reaction zone 32 is 150 psig. By providing the above-described pressure in the reaction zone 32, and amongst other things, there is effected a greater residence time for the reactant matter in the reaction zone 32, which effects a greater conversion of reactant matter into gaseous hydrogen and effects reduction in the amount of polycyclic aromatic hydrocarbons (PAH) associated with the solid particulate matter.
[0059] In some embodiments, the plasma 102 (see Figures 10 or 12) is generated by flowing a plasma forming fluid flow through a reaction zone 32 through which an electrical discharge is being effected. In some embodiments, the plasma forming fluid includes reactant matter. In some embodiments, the reactant matter includes natural gas. For example, the reactant matter includes methane. (B) ELECTRODE WITH RELATIVELY LOW RADIUS OF CURVATURE
[0060] Another aspect, which is provided, is associated with the manner by which the reactor 10 is configured for generating a plasma. The reactor 10 includes an electrode surface portion with a relatively low radius of curvature for, amongst other things, facilitating an electrical discharges at a relatively lower applied electrical potential difference.
[0061] Referring to Figure 2, the reactor 10 includes an internal space 26 including a reaction zone 32. The reactor 10 also includes a plasma generator 34. The plasma generator 34 includes a first electrode 36 and a second electrode. The first electrode 36 is configured for electrical coupling to a current and voltage source 44. The second electrode 52 is spaced apart from and disposed in electrical discharge communication with the first electrode 36 through the internal space 26, and includes an operative second electrode surface portion 54. For example, the second electrode 52 is a ground electrode. Referring specifically to Figure 5, the operative second electrode surface portion 54 is defined by a radius of curvature of less than 0.002 inches. In some embodiments, for example, the radius of curative is between 0.002 inches and 0.0055 inches. In some embodiments, for example, the radius of curvature is as small as permitted by existing manufacturing techniques so as to facilitate generation of a larger electric field, which eases the ignition process of the plasma. The reaction zone 32 is disposed between the first and second electrodes 36, 52.
[0062] Referring to Figures 5, 10, and 12, when a plasma forming gaseous fluid is disposed within the reaction zone 32 and a sufficient electrical potential difference is applied between the first electrode 36 and the operative second electrode surface portion 54, an electrical discharge is effected between the first electrode 36 and the operative second electrode surface portion 54 and through the reaction zone 32, and at least a fraction of the plasma forming gaseous fluid is converted into a plasma 102.
[0063] In some embodiments, the operative second electrode surface portion 54 is defined by an edge 58. For example, the reactor 10 includes an internal surface 28 defining the internal space 26, and the operative second electrode surface portion 54 is the conductive surface portion of the internal surface 28 which is closest to the first electrode 36.
[0064] In some embodiments, the reactor 10 includes a fluid passage which includes the reaction zone 32. Referring to Figure 5, for example, the fluid passage includes upstream and downstream fluid passage portions 66, 74, and the operative second electrode surface portion 54 defines an orifice 92 which effects fluid communication between the upstream fluid passage portion 66 and the downstream fluid passage portion 74.
[0065] In a related aspect, a method of operating any of the above-described embodiments of the reactor 10 in (B) is provided. The method includes contacting reactant matter with a plasma in a reaction zone 32, wherein the pressure in the reaction zone 32 is at least 75 psig.
[0066] In some embodiments, the plasma is plasma generated by providing a plasma forming fluid in the reaction zone 32, and applying a sufficient electrical potential difference between the first electrode 36 and the operative second electrode surface portion 54, so as to effect an electrical discharge between the first electrode 36 and the operative second electrode surface portion 54 and through the reaction zone 32. As a result, at least a fraction of the plasma forming gaseous fluid is converted into a plasma 102.
[0067] In some embodiments, the plasma forming fluid includes reactant matter. In some embodiments, the reactant matter includes natural gas. For example, the reactant matter includes methane.
(C) MITIGATING DEPOSITION OF PRODUCED SOLID PARTICULATE ON ELECTRODE MOUNTING STRUCTURE
[0068] A further aspect includes providing a reactor 10 configured for generating a plasma by virtue of an electrical discharge between first and second electrodes 36, 52, and providing a minimum distance between an operative second electrode surface portion 54 of the second electrode 52 and a mounting structure 46 for mounting the first electrode 36. Amongst other things, by providing this minimum distance, deposition of solid particulate, such as particulate carbon, generated by a reactive process effected by the generated plasma, upon the mounting structure 46 is mitigated. Such deposition could otherwise facilitate undesirable arcing between the mounting structure 46 and the first electrode 46.
[0069] Referring to Figure 2 the mounting structure 46 includes an internal mounting structure surface 48 defining a portion of the internal surface 28. The internal mounting structure surface 48 is defined by an electrically non-conductive material 49 of the mounting structure 46. With respect to the electrically non-conductive material 49, in some embodiments, for example, the electrically non-conductive material 49 defining the internal mounting structure surface 48 is disposed between the first electrode 36 and electrically conductive material, wherein such electrically conductive material is disposed within the reaction vessel 12 and in closer proximity to the first electrode 36 relative to the second electrode 52. For example, the electrically non-conductive material 49 includes a polymeric material, such as TEFLON™.
[0070] In some embodiments, for example, the reaction vessel 12 includes an internal reaction vessel wall 14, and the electrically non-conductive material 49 extends to the internal reaction vessel wall 14 such that a reaction zone remote electrically non- conductive material surface 481 is provided in abutting relationship with the internal reaction vessel wall 14. For example, the internal reaction vessel wall 14 includes an electrically conductive internal reaction vessel wall portion 16 and, in some embodiments, the electrically conductive internal reaction vessel wall portion 16 is disposed in closer proximity to the first electrode 36 relative to the second electrode 52. The electrically non-conductive material 49, in such cases, insulates the electrically conductive internal reaction vessel wall portion 16 from the first electrode 36.
[0071] In some embodiments, for example, the mounting structure 46 is the high voltage feedthrough assembly 300.
[0072] The reactor 10 includes an internal surface 28 defining an internal space 26 including a reaction zone 32. The reactor 10 also includes a plasma generator 34. The plasma generator 34 includes a first electrode 36 and a second electrode 52. The first electrode 36 is configured for electrical coupling to a current and voltage source 44. The second electrode 52 is spaced apart from and disposed in electrical discharge communication with the first electrode 36 through the internal space 26. The second electrode 52 further includes an operative second electrode surface portion 54. For example, the second electrode 52 is a ground electrode. The reaction zone 32 is disposed between the first electrode 36 and the operative second electrode surface portion 54.
[0073] The first electrode 36 is mounted within a reaction vessel 12 with a mounting structure 46. The internal mounting structure surface 48 includes an internal mounting structure surface portion 482 defining a portion of the internal surface 28. The internal mounting structure surface portion 482 is disposed in fluid communication with the reaction zone 32. Referring specifically to Figure 8, the minimum distance Dl between the operative second electrode surface portion 54 and the internal mounting structure surface portion 48 is at least two (2) inches. The minimum distance Dl varies depending on the fluid flow characteristics in the reaction zone 32.
[0074] Referring to Figures 5, 10, and 12, when a plasma forming gaseous fluid is disposed within the reaction zone 32 and a sufficient electrical potential difference is applied between the first electrode 36 and the operative second electrode surface portion 54, an electrical discharge is effected between the first electrode 36 and the operative second electrode surface portion 54 and through the reaction zone 32. At least a fraction of the plasma forming gaseous fluid disposed in the reaction zone 32 is converted into a plasma 102.
[0075] In some embodiments, for example, the operative second electrode surface portion 54 is the electrically conductive surface portion of the internal surface 28 which is closest to the first electrode 36.
[0076] In some embodiments, the internal mounting structure surface portion 48 is electrically non-conductive. For example, the mounting structure surface portion 48 includes a solid particulate deposition susceptible mounting surface portion 50 configured for becoming coupled to a solid particulate upon approach of the solid particulate to the solid particulate deposition susceptible mounting surface portion 50. For example, the solid particulate includes carbon-comprising particulate, such as particulate carbon.
[0077] For example, with respect to the upstream fluid passage portion 66, in some embodiments, the upstream fluid passage portion 66 is defined by an upstream conduit wall 68 disposed upstream of the reaction zone 32, wherein the upstream conduit wall 68 includes at least one electrically conductive upstream conduit wall surface portion 70. Further, any electrically conductive upstream conduit wall surface portion 70, which is disposed in electrical discharge communication with the first electrode 36, is disposed further from the first electrode 36 than the operative second electrode surface portion 54. Referring to Figure 4, in some embodiments, for example, any electrically conductive upstream conduit wall surface portion 70 of the upstream conduit wall 68 that is spaced apart from the mounting structure by a minimum distance of D6 of at least 1.118 inches is also spaced apart from the first electrode 36 by a minimum distance D7 that is greater than 0.5 inches . In some embodiments, for example, any electrically conductive upstream conduit wall surface portion 70 of the upstream conduit wall 68 that is spaced apart from the mounting structure by a minimum distance of D6 of 1.39 inches is also spaced apart from the first electrode 36 by a minimum distance D7 of 0.845 inches.
[0078] For example, with further respect to the upstream fluid passage portion 66, in some embodiments, the upstream conduit wall 68 includes an upstream solid particulate deposition susceptible conduit wall surface portion 72 configured for becoming coupled to a solid particulate upon approach of the solid particulate to the upstream solid particulate deposition susceptible conduit wall surface portion 72. For example, the solid particulate includes carbon-comprising particulate, such as particulate carbon.
[0079] For example, with further respect to the upstream fluid passage portion 66, in some embodiments, the upstream fluid passage portion 66 extends between the reaction zone 32 and the mounting structure 46.
[0080] In some embodiments, and with reference to Figure 2, the internal space 26 includes a fluid passage portion 64 for flowing a plasma forming gaseous fluid through the reaction zone 32. The fluid passage portion 64 includes an upstream fluid passage portion 66 disposed upstream of the reaction zone 32 and between the mounting structure 46 and the reaction zone 32. The fluid passage portion 64 also includes a downstream fluid passage portion 74 extending downstream from within the reaction zone 32. In some embodiments, for example, the downstream fluid passage portion 74 is defined by a downstream internal conduit surface 76 including a downstream solid particulate deposition susceptible conduit surface portion 78. The downstream solid particulate deposition susceptible conduit surface portion 78 is configured for becoming coupled to a solid particulate upon approach of the solid particulate to the downstream solid particulate deposition susceptible conduit surface portion 78.
[0081] In a related aspect, there is provided a method of operating any of the above- described embodiments of the reactor 10 in (C). The method includes contacting reactant matter with a plasma in a reaction zone 32 to effect production of product matter including solid particulate, such as carbon-comprising particulate. For example, the solid particulate is carbon particulate.
[0082] In some embodiments, the plasma is plasma generated by providing a plasma forming fluid in the reaction zone 32, and applying a sufficient electrical potential difference between the first electrode 36 and the operative second electrode surface portion 54, so as to effect an electrical discharge between the first electrode 36 and the operative second electrode surface portion 54 and through the reaction zone 32. As a result, at least a fraction of the plasma forming gaseous fluid is converted into a plasma 102.
[0083] With respect to the plasma forming fluid, in some embodiments, for example, the plasma forming fluid includes a plasma forming fluid flow.
[0084] With further respect to the plasma forming fluid, in some embodiments, for example, the plasma forming fluid includes reactant matter. In some embodiments, the reactant matter includes natural gas. For example, the reactant matter includes methane.
[0085] In some embodiments, there is provided a carrier fluid flow for sweeping produced solid particulate from the reaction zone 32. The downstream fluid passage portion 74 is defined by a downstream internal conduit surface 76 including a downstream solid particulate deposition susceptible conduit surface portion 78, wherein the downstream solid particulate deposition susceptible conduit surface portion 78 is configured for becoming coupled to the produced solid particulate upon approach of the produced solid particulate to the downstream solid particulate deposition susceptible conduit surface portion 78.
[0086] With respect to the carrier fluid flow, in some embodiments, for example, the minimum velocity of carrier fluid flow is 0.4 metres per second to 0.5 metres per second for flow through a circular fluid passage of a diameter of 0.4 inches. Further, in some embodiments, for example, the minimum velocity of carrier fluid flow is 0.5 metres per second to 0.6 metres per second for flow through a circular fluid passage of a diameter of 0.3 inches.
[0087] With further respect to the carrier fluid flow, in some embodiments, for example, at least a fraction of the carrier fluid flow is derived from the plasma forming fluid flow. In some embodiments, for example, the carrier fluid flow is entirely derived from the plasma forming fluid flow.
(D) DEFINING MAXIMUM DISTANCE BETWEEN ELECTRODES TO MITIGATE ELECTRICAL DISCHARGES AT NON-PREFERRED SURFACES
[0088] Another aspect, which is provided, is associated with a reactor 10 configured for generating a plasma. A maximum distance between electrodes is provided for, amongst other things, mitigating against the formation of a higher temperature environment at the electrodes during electrical discharge between the electrodes. Such higher temperatures would then effect formation of higher temperatures at non-preferred surfaces through heat transfer, and increase the likelihood of electrical discharge at these non-preferred surfaces.
[0089] Referring to Figure 2, the reactor 10 includes a fluid passage portion 64 for flowing a plasma forming gaseous fluid. The fluid passage portion 64 includes a reaction zone 32. The fluid passage portion 64 includes an upstream fluid passage portion 66 and a downstream fluid passage portion 74. The upstream fluid passage portion 66 is defined by an upstream conduit wall 68 disposed upstream of the reaction zone 32, wherein the upstream conduit wall 68 includes at least one electrically conductive upstream conduit wall 68 portion. The downstream fluid passage portion 74 extends downstream from within the reaction vessel 32.
[0090] The reactor 10 also includes a plasma generator 34. The plasma generator 34 includes a first electrode 36 and a second electrode 52. The first electrode 36 is configured for electrical coupling to a current and voltage source 44. The second electrode 52 is spaced apart from and disposed in electrical discharge communication with the first electrode 36 through the internal space 26. For example, the second electrode 52 is a ground electrode. The second electrode 52 includes an operative second electrode surface portion 54. The reaction zone 32 is defined between the first electrode 36 and the operative second electrode surface portion 54. Referring to Figure 9, the operative second electrode surface portion 54 is spaced apart from the first electrode 36 by a minimum distance D2 of less than 0.15 inches. For example, in some embodiments, the minimum distance D2 is greater than 0.075 inches. In this respect, in some embodiments, for example, if D2 is too small, power transfer in the plasma may be undesirably limiting. For example, in some embodiments, the minimum distance D2 is between 0.075 inches and 0.15 inches.
[0091] Referring to Figures 5, 10, and 12, when the plasma forming gaseous fluid is disposed in the reaction zone 32 and a sufficient electrical potential difference is applied between the first electrode 36 and the operative second electrode surface portion 54, an electrical discharge is effected between the first electrode 36 and the operative second electrode surface portion 54 and through the reaction zone 32, and at least a fraction of the plasma forming gaseous fluid is converted into a plasma 102.
[0092] The operative second electrode surface portion 54 is disposed in thermal communication with at least one electrically conductive upstream conduit wall portion 70. Any of the at least one electrically conductive upstream conduit wall portion 70, that is disposed in electrical discharge communication with the first electrode 36, is disposed further from the first electrode 36 than the operative second electrode surface portion 54. Amongst other things, disposition of the operative second electrode surface portion 54 from the first electrode 36 beyond the above-described maximum distance increases the likelihood that heat is generated during the electrical discharge at the operative second electrode surface portion 54 and effects heating of an electrically conductive upstream conduit wall portion 70 to a temperature which is effective to facilitate an electrical discharge between the first electrode 36 and the electrically conductive upstream conduit wall portion 70. It is preferred to effect electrical discharge further downstream, rather than upstream, so as to effect reduced residence time of any produced solid particulate in the reactor 10 and thereby mitigate against deposition, within the reactor 10, of the produced solid particulate.
[0093] With respect to the upstream conduit wall 68, in some embodiments, for example, the upstream conduit wall 68 includes an upstream solid particulate deposition susceptible conduit wall portion 72 configured for becoming coupled to the solid particulate upon approach of solid particulate to the upstream solid particulate deposition susceptible conduit wall portion 72.
[0094] With respect to the downstream fluid passage portion 74, in some embodiments, for example, the downstream fluid passage portion 74 is defined by a downstream internal conduit surface 76 including a downstream solid particulate deposition susceptible conduit surface portion 78. The downstream solid particulate deposition susceptible conduit surface portion 78 is configured for becoming coupled to solid particulate upon approach of the solid particulate to the downstream solid particulate deposition susceptible conduit surface portion 78.
[0095] In some embodiments, for example, the reaction zone 32 is provided in an internal space 26 defined by an internal surface 28 of the reactor 10, and the operative second electrode surface portion 54 is the electrically conductive surface portion of the internal surface 28 which is closest to the first electrode 36.
[0096] In some embodiments, for example, the upstream conduit wall 68 merges with the operative second electrode surface portion 54. [0097] In a related aspect, there is provided a method of operating any of the above- described embodiments of the reactor 10 in (D). The method includes contacting reactant matter with a plasma in a reaction zone 32 to effect production of product matter including solid particulate such as carbon-comprising particulate. For example, the solid particulate is carbon particulate.
[0098] In some embodiments, the plasma is plasma generated by providing a plasma forming fluid in the reaction zone 32, and applying a sufficient electrical potential difference between the first electrode 36 and the operative second electrode surface portion 54, so as to effect an electrical discharge between the first electrode 36 and the operative second electrode surface portion 54 and through the reaction zone 32. As a result, at least a fraction of the plasma forming gaseous fluid is converted into a plasma 102.
[0099] With respect to the plasma forming fluid, in some embodiments, for example, the plasma forming fluid includes a plasma forming fluid flow.
[00100] With further respect to the plasma forming fluid, in some embodiments, for example, the plasma forming fluid includes reactant matter. In some embodiments, the reactant matter includes natural gas. For example, the reactant matter includes methane.
[00101] In some embodiments, for example, there is further provided a carrier fluid flow for sweeping carbon from the reaction zone 32. In this respect, for example, the downstream fluid passage portion 74 is defined by a downstream internal conduit surface 76 including a downstream solid particulate deposition susceptible conduit surface portion 78. The downstream solid particulate deposition susceptible conduit surface portion 78 is configured for becoming coupled to the produced solid particulate upon approach of the produced solid particulate to the downstream solid particulate deposition susceptible conduit surface portion 78 Amongst other things, the carrier fluid flow mitigates against such deposition. In some embodiments, for example, the minimum velocity of carrier fluid flow is 0.5 metres per second to 0.6 metres per second for flow through the downstream fluid passage portion 74 having an internal diameter of 0.3 inches. In some embodiments, for example, at least a fraction of the carrier fluid flow is derived from the plasma forming fluid flow.
(E) PROVIDING SUFFICIENT ELECTRODE SURFACE AREA TO EFFECT COOLING OF THE ELECTRODE WHILE PROVIDING SUFFICIENT SPACE TO EFFECT DESIRED CONVERSION OF REACTANTS WHILE MITIGATING SOLID PARTICULATE DEPOSITION
[00102] Another aspect, which is provided, is associated with a reactor 10 configured for generating a plasma. This aspect provides, within a fluid passage within the reactor 10, an electrode with a defined electrode surface area which, amongst other things, effects cooling of the electrode while allowing sufficient space to effect desired conversion of reactants while mitigating against solid particulate deposition.
[00103] Referring to Figure 2, the reactor 10 includes a fluid passage portion 64 for flowing a plasma forming gaseous fluid. The fluid passage portion 64 includes an upstream fluid passage portion 66 and a downstream fluid passage portion 74. The reactor 10 also includes a plasma generator 34. The plasma generator 34 includes a first electrode 36 and a second electrode 52. The first electrode 36 is configured for electrical coupling to a current and voltage source 44. The second electrode 52 is spaced apart from and disposed in electrical discharge communication with the first electrode 36 through the internal space 26. For example, the second electrode 52 is a ground electrode.
[00104] A reaction zone 32 is defined within the fluid passage portion 64 between the first electrode 36 and the second electrode 52. The downstream fluid passage portion 74 extends downstream from within the reaction zone 32. The upstream fluid passage portion 66 is disposed upstream of the reaction zone 32.
[00105] Referring to Figures 5, 10, and 12, when the plasma forming gaseous fluid is disposed within the reaction zone 32 and a sufficient electrical potential difference is applied between the first electrode 36 and the second electrode 52, an electrical discharge is effected between the first electrode 36 and the second electrode 52 and through the reaction zone 32, and at least a fraction of the plasma forming gaseous fluid is converted into a plasma 102.
[00106] Referring to Figures 10 and 1 1 , the first electrode 36 is at least partially disposed in the downstream fluid passage portion 74 and is spaced apart from an internal conduit wall 76, which defines the downstream fluid passage portion 74 to define a fluid flow space 741 in the downstream fluid passage portion 74 between the first electrode 36 and the internal conduit wall 76. In any plane 200 which intersects that portion of the first electrode 36 disposed in the downstream fluid passage portion 74, and which is disposed in a normal orientation relative to an axis 741 1 of the downstream fluid passage portion 74 being intersected, the ratio of the diameter D3 of the first electrode 36 to the diameter D4 of the downstream fluid passage portion 74 is between two (2) and five (5). For example, in some embodiments, this ratio is three (3).
[00107] With respect to the second electrode 52, in some embodiments, for example, the second electrode 52 includes an operative second electrode surface portion 54. When the plasma forming gaseous fluid is disposed within the reaction zone 32 and a sufficient electrical potential difference is applied between the first electrode 36 and the operative second electrode surface portion 54, the effected electrical discharge is between the first electrode 36 and the operative second electrode surface portion 54 and at least a fraction of the plasma forming gaseous fluid is converted into a plasma 102.
[00108] In some embodiments, for example, the reaction zone 32 is provided in an internal space 26 defined by an internal surface 28 of the reactor 10, and the operative second electrode surface portion 54 is the electrically conductive surface portion of the internal surface 28 which is closest to the first electrode 36.
[00109] With respect to the upstream fluid passage portion 66, in some embodiments, for example, the upstream fluid passage portion 66 is defined by an upstream conduit wall 68 disposed upstream of the reaction zone 32. The upstream conduit wall 68 includes at least one electrically conductive upstream conduit wall portion 70. Any electrically conductive upstream conduit wall portion 70, which is disposed in electrical discharge communication with the first electrode 36, is disposed further from the first electrode 36 than the operative second electrode surface portion 54.
[00110] With further respect to the upstream fluid passage portion 66, in some embodiments, for example, the upstream conduit wall 68 includes an upstream solid particulate deposition susceptible conduit wall portion 72 configured for becoming coupled to solid particulate upon approach of the solid particulate to the upstream solid particulate deposition susceptible conduit wall portion 72.
[00111] With respect to the downstream fluid passage portion 74, in some embodiments, for example, the downstream fluid passage portion 74 is defined by a downstream internal conduit surface 76 including a downstream solid particulate deposition susceptible conduit surface portion 78. The downstream solid particulate deposition susceptible conduit surface portion 78 is configured for becoming coupled to solid particulate upon approach of the solid particulate to the downstream solid particulate deposition susceptible conduit surface portion 78.
[00112] In a related aspect, there is provided a method of operating any of the above- described embodiments of the reactor 10 in (E). The method includes contacting reactant matter with a plasma in a reaction zone 32 to effect production of product matter including solid particulate such as carbon-comprising particulate. For example, the solid particulate is carbon particulate.
[00113] In some embodiments, the plasma is plasma generated by providing a plasma forming fluid in the reaction zone 32, and applying a sufficient electrical potential difference between the first electrode 36 and the operative second electrode surface portion 54, so as to effect an electrical discharge between the first electrode 36 and the second electrode 52 (and, in some embodiments, the operative second electrode surface portion 54) and through the reaction zone 32. As a result, at least a fraction of the plasma forming gaseous fluid is converted into a plasma 102.
[00114] With respect to the plasma forming fluid, in some embodiments, for example, the plasma forming fluid includes a plasma forming fluid flow. [00115] With further respect to the plasma forming fluid, in some embodiments, for example, the plasma forming fluid includes reactant matter. In some embodiments, the reactant matter includes natural gas. For example, the reactant matter includes methane.
[00116] In some embodiments, for example, there is further provided a carrier fluid flow for sweeping carbon from the reaction zone 32. In this respect, for example, the downstream fluid passage portion 74 is defined by a downstream internal conduit surface 76 including a downstream solid particulate deposition susceptible conduit surface portion 78. The downstream solid particulate deposition susceptible conduit surface portion 78 is configured for becoming coupled to the produced solid particulate upon approach of the produced solid particulate to the downstream solid particulate deposition susceptible conduit surface portion 78 Amongst other things, the carrier fluid flow mitigates against such deposition. In some embodiments, for example, the minimum velocity of carrier fluid flow is 0.5 metres per second to 0.6 metres per second for flow through the downstream fluid passage portion 74 having an internal diameter of 0.3 inches. In some embodiments, for example, at least a fraction of the carrier fluid flow is derived from the plasma forming fluid flow.
(F) INCREASING SERVICE LIFE OF ELECTRODE
[00117] Another aspect is provided associated with a reactor 10 configured for generating a plasma, which, amongst other things, effects increased service life of the electrode.
[00118] Referring to Figure 2, the reactor 10 includes an internal space 26 defining a fluid passage portion 64 for flowing a plasma forming gaseous fluid. The fluid passage portion 64 includes a reaction zone 32. The reactor 10 also includes a plasma generator 34. The plasma generator 34 includes a first electrode 36 and a second electrode 52. The first electrode 36 is configured for electrical coupling to a current and voltage source 44, and includes an operative first electrode surface portion 38. The second electrode 52 is spaced apart from and disposed in electrical discharge communication with the first electrode 36 through the internal space 26, and includes an operative second electrode surface portion 54. For example, the second electrode 52 is a ground electrode. The reaction zone 32 is disposed between the first and second electrodes 36, 52.
[00119] When a plasma forming gaseous fluid is disposed within the reaction zone 32 and a sufficient electrical potential difference is applied between the operative first electrode surface portion 38 and the operative second electrode surface portion 54, an electrical discharge is effected between the operative first electrode surface portion 38 and the operative second electrode surface portion 54 and through the reaction zone 32, and at least a fraction of the plasma forming gaseous fluid is converted into a plasma 102.
[00120] Referring to Figure 12, an operative distance D5 is defined along the longitudinal axis 36 of the first electrode 36 between: (i) a plane in which is disposed an axis normal to the operative first electrode surface portion 38, and (ii) a tip 100 of the first electrode 36, disposed downstream of the operative first electrode surface portion 38, wherein the operative distance D5 is at least 0.25 inches. For example, in some embodiments, the operative distance D5 is less than 1.25 inches. For example, in some embodiments, the operative distance D5 is one inch. By providing this minimum operative distance, amongst other things, the reactor 10 is able to operate for longer durations before requiring replacement of the first electrode 36.
[00121] In some embodiments, for example, the reaction zone 32 is provided in an internal space 26 defined by an internal surface 28 of the reactor 10, and the operative second electrode surface portion 54 is the electrically conductive surface portion of the internal surface 28 which is closest to the first electrode 36.
[00122] In a related aspect, there is provided a method of operating any of the above- described embodiments of the reactor 10 in (F). The method includes contacting reactant matter with a plasma in a reaction zone 32 to effect production of product matter including solid particulate.
[00123] Referring to Figures 5, 10, and 12, in some embodiments, the plasma is plasma generated by providing a plasma forming fluid in the reaction zone 32, and applying a sufficient electrical potential difference between the first electrode 36 and the operative second electrode surface portion 54, so as to effect an electrical discharge between the first electrode 36 and the operative second electrode surface portion 54 and through the reaction zone 32. As a result, at least a fraction of the plasma forming gaseous fluid is converted into a plasma 102.
[00124] With respect to the plasma forming fluid, in some embodiments, for example, the plasma forming fluid includes a plasma forming fluid flow.
[00125] With further respect to the plasma forming fluid, in some embodiments, for example, the plasma forming fluid includes reactant matter. In some embodiments, the reactant matter includes natural gas. For example, the reactant matter includes methane.
[00126] In some embodiments, for example, the plasma 102 is generated in the reaction zone 32, and the pressure in the reaction zone 32 is at least 75 psig. By providing this pressure in the reaction zone 32, and amongst other things, there is effected a greater residence time for the reactant matter in the reaction zone, which effects a greater reaction conversion of reactant matter, and which, as a corollary, effects greater generation of heat, and thereby effects creation of conditions which could, amongst other things, acceleration electrode erosion. In this respect, and amongst other things, the operative distance D5 is provided to mitigate against these consequences.
(G) HEAT EXCHANGER FOR EFFECTING HEATING OF PLASMA FORMING FLUID BEING INTRODUCED INTO REACTION ZONE
[00127] Another aspect, which is provided, is associated with a reactor 10 configured for generating a plasma, which, amongst other things, includes a heat exchanger 18 for effecting heating of plasma forming fluid being introduced into the reactor 10.
[00128] Referring to Figure 7, there is provided a reactor 10 including an internal space 26 including a reaction zone 32. The reactor includes an inlet 20 fluidly coupled to the reaction zone 32 with a fluid introduction passage 24 for introducing a plasma forming gaseous fluid into the reaction zone 32. The reactor 10 also includes a plasma generator 34. The plasma generator 34 includes a first electrode 36 and a second electrode 52. The first electrode 36 is configured for electrical coupling to a current and voltage source 44. The second electrode 52 is spaced apart from and disposed in electrical discharge communication with the first electrode 36 through the internal space 26. The reaction zone 32 is disposed between the first and second electrodes 36, 52.
[00129] When a plasma forming gaseous fluid is disposed within the reaction zone 32 and a sufficient electrical potential difference is applied between the first electrode 36 and the second electrode 52, an electrical discharge is effected between the first electrode 36 and the second electrode 52 and through the reaction zone 32, and at least a fraction of the plasma forming gaseous fluid is converted into a plasma.
[00130] The reaction vessel 12 includes a heat exchanger 18 disposed in heat transfer communication with the fluid introduction passage 24 for effecting heat transfer to plasma forming gaseous fluid being introduced to the reaction zone 32.
[00131] In some embodiments, for example, the heat exchanger 18 includes an induction heater.
[00132] In a related aspect, there is provided a method of operating any of the above- described embodiments of the reactor 10 in (G). The method includes contacting reactant matter with a plasma in a reaction zone 32 to effect production of product matter.
[00133] In some embodiments, the plasma is plasma generated by providing a plasma forming fluid in the reaction zone 32, and applying a sufficient electrical potential difference between the first electrode 36 and the second electrode 52, so as to effect an electrical discharge between the first electrode 36 and the second electrode 52 and through the reaction zone 32. As a result, at least a fraction of the plasma forming gaseous fluid is converted into a plasma. The plasma forming fluid is heated by the heat exchanger 18. In some embodiments, the plasma forming fluid is heated by the heat exchanger 18 to a temperature of between 400°C and 700°C from any defined temperature.
[00134] With respect to the plasma forming fluid, in some embodiments, for example, the plasma forming fluid includes a plasma forming fluid flow. [00135] With further respect to the plasma forming fluid, in some embodiments, for example, the plasma forming fluid includes reactant matter. In some embodiments, the reactant matter includes natural gas. For example, the reactant matter includes methane.
(H) OPERATING A REACTOR AT ELEVATED TEMPERATURES
[00136] Another aspect is provided relating to the method of operating a plasma reactor 10. Amongst other things, this aspect effects heat transfer from an electrode at a sufficiently desirable rate so as to mitigate against providing high temperatures at the electrode which would facilitate deposition of solid particulate at the electrode.
[00137] Referring to Figure 2, a plasma reactor 10 is provided including an internal surface 28 defining an internal space 26 including a reaction zone 32. The plasma reactor also includes a plasma generator 34. The plasma generator 34 includes a first electrode 36 and a second electrode 52. The first electrode 36 is configured for electrical coupling to a current and voltage source 44. The second electrode 52 is spaced apart from and disposed in electrical discharge communication with the first electrode 36 through the internal space 26. For example, the second electrode 52 is a ground electrode. The reaction zone 32 is disposed between the first and second electrode 36, 52.
[00138] A plasma forming gaseous fluid is provided within the reaction zone 32.
[00139] Referring to Figure 10, when an electrical potential difference is applied between the first electrode 36 and the second electrode 52 sufficient to effect an electrical discharge between the first electrode 36 and the second electrode 52 and through the reaction zone 32, at least a fraction of the provided plasma forming gaseous fluid is converted into plasma 102.
[00140] Referring to Figure 10, the plasma reactor 10 includes a pressure boundary 960, which includes an internal surface portion 96 adjacent to and in thermal communication with the reaction zone 32, and which also defines an extemalmost surface 962 which is disposed in heat transfer relationship with the outside environment 1000 (ie. the atmosphere). In some embodiments, for example, the internal surface portion 96 is defined by the second electrode 52. The material of the pressure boundary 960 is characterized by an average heat transfer coefficient of at least 100 W / (meter-Kelvin). In some embodiments, for example, this average heat transfer coefficient is between 100 W / (meter-Kelvin) and 200 W / (meter-Kelvin). In some embodiments, for example, this average heat transfer coefficient is 173 W / (meter-Kelvin).
[00141] In some embodiments, for example, the pressure boundary 960 includes a heat transfer medium 94. In some embodiments, for example, the heat transfer medium 94 includes steel wool. In other embodiments, for example, the heat transfer medium includes copper.
[00142] With respect to the plasma forming fluid, in some embodiments, for example, the plasma forming fluid includes a plasma forming fluid flow.
[00143] With further respect to the plasma forming fluid, in some embodiments, for example, the plasma forming fluid includes reactant matter. In some embodiments, the reactant matter includes natural gas. For example, the reactant matter includes methane.
[00144] In the above description, for purposes of explanation, numerous details are set forth in order to provide a thorough understanding of the present disclosure. However, it will be apparent to one skilled in the art that these specific details are not required in order to practice the present disclosure. In other instances, well-known electrical structures and circuits are shown in block diagram form in order not to obscure the present disclosure. Although certain dimensions and materials are described for implementing the disclosed example embodiments, other suitable dimensions and/or materials may be used within the scope of this disclosure. All such modifications and variations, including all suitable current and future changes in technology, are believed to be within the sphere and scope of the present disclosure. All references mentioned are hereby incorporated by reference in their entirety. APPENDIX "A" - REACTIONS
The dominant reactions that initiate the process
Figure imgf000038_0001
e + CH => CH3 + H + e
e + CH4 => CH2 + H2 + e
e + CH4=> CH + H2 + H + e
e + CH4 => CH3 + H* + e
Other reactions include:
Figure imgf000038_0002
Reaction
Figure imgf000039_0001
e + CH4 => CH3 + H* + e
Figure imgf000039_0002
e + CH4 => CH* + H2 + H + e
Figure imgf000039_0003
e + CH4 =>CH3 + + H + 2e
e + CH4 =>CH2 + + H2 + 2e
Figure imgf000039_0004
e + CH4 =>C+ + 4H* + 2e
e + C2H4 =>C2H4 + + 2e
e + C2H6 => C2H4 + + H2 + 2e e + C2H2 =>C2H2 + + 2e
e + C3H8=> C2H5 + + CH3 + 2e
Figure imgf000039_0005
Electron-impact reactions of Hydrogen e + H2 => H2 + e
e + H2 => H2 + e
e + H2 => H2 + e
e + H2 => H + H + e
e + H2 => H2 + + 2e
e + H => H + e
e + H => H+ + 2e
II. Ion-Molecule Reaction
C+ + CH4 => C2H2 + +H2
C+ + CH4 => C2H3 + +H
CH+ + CH4 =>C2H2 + +H2 + H
CH+ + CH4 => C2H3 + +H2
CH+ + CH4 => C2H4 + + H
CH+ + H2 => CH2 + + H
CH2 + + CH4 => C2H4 + + H2
CH2 + + CH4 => C2H5 + + H
CH2 + + H2 => CH3 + + H
CH2 + + CH4 => CH3 + +CH3 Reaction
Figure imgf000040_0001
CH2 + + CH4=>C2H3 + + H + H2
CH3 + + CH4 => CH4 + + CH3
Figure imgf000040_0002
CH4 + + CH4 => CH5 + + CH3
CH4 + + H2 => CH5 + + H
CH5 + +C2H6=>C2H5 + +H2+CH4
Figure imgf000040_0003
C2H2 + + CH4 => C2H3 + + CH3
C2H2 + + CH4 => C3H5 + + H
C2H3 + + CH4 => C3H5 + + H2
C2H3 + + C2H4=>C2H5 + + C2H2
C2H3 + + C2H2 => C4H5 +
C2H4 + + C2H4 =>C3H5 + + CH3
C2H4 + + C2H4 => CH8 +
C2H4 + + C2H6 =>C3H6 + + CH4
C2H4 + + C2H6 =>C3H7 + + CH3
C2H5 + + C2H4 =>C3H5 + + CH4
C2H5 + + C2H3 => C4H8 +
H2 + +H2=>H3 + + H
H3 + +CH4=>CH5 + + H2
H3 + +C2H2=>C2H3 + + H2
H3 + +C2H4=>C2Hs+ + H2
III. Neutral - Neutral Reactions
CH3 + CH3 = C2H6
CH3 +CH3 = C2H4 +H2
CH3 + H = CH4
CH3 + CH2 = C2H4 + H
CH3 + H2 = CH4 + H
CH3 + CH3 = C2H5 + H
CH3 + C2H6 = CH4 + C2H5
Figure imgf000040_0004
CH + C2H4 = C3H5
Figure imgf000041_0001
Figure imgf000042_0001
Figure imgf000043_0001
Figure imgf000044_0001
Figure imgf000045_0001
Figure imgf000046_0001

Claims

CLAIMS:
1. A method of operating a plasma reactor including a reaction zone comprising: generating a plasma in the reaction zone; and contacting reactant matter with the plasma in the reaction zone wherein the pressure in the reaction zone is at least 75 psig.
2. The method as claimed in claim 1 , wherein the reactant matter includes natural gas
3. The method as claimed in claim 1 , wherein the plasma is generated by flowing a plasma forming fluid flow through a reaction zone through which an electrical discharge is being effected.
4. The method as claimed in claim 3, wherein the plasma forming fluid includes reactant matter
5. Contacting reactant matter with a plasma in a reaction zone, wherein the pressure in the reaction zone is at least 75 psig.
6. A reactor, defining an internal space including a reaction zone, comprising: a plasma generator including: a first electrode, configured for electrical coupling to a current and voltage source; and a second electrode, spaced apart from and disposed in electrical discharge communication with the first electrode through the internal space, and including an operative second electrode surface portion; wherein the reaction zone is disposed between the first and second electrodes; such that, when a plasma forming gaseous fluid is disposed within the reaction zone and a sufficient electrical potential difference is applied between the first electrode and the operative second electrode surface portion, an electrical discharge is effected between the first electrode and the operative second electrode surface portion and through the reaction zone, and at least a fraction of the plasma forming gaseous fluid is converted into a plasma; and wherein the operative second electrode surface portion is defined by a radius of curvature of less than 0.002 inches.
7. The reactor as claimed in claim 6, wherein the operative second electrode surface portion is defined by an edge.
8. The reactor as claimed in claim 6, wherein the internal space includes a fluid passage portion including upstream and downstream fluid passage portions, wherein the operative second electrode surface portion defines an orifice which effects fluid communication between the upstream fluid passage portion and the downstream fluid passage portion.
9. The reactor as claimed in claim 6, further comprising an internal surface defining the internal space, wherein the operative second electrode surface portion is the conductive surface portion of the interior surface which is closest to the first electrode.
10. A method of operating a plasma reactor as claimed in claim 6, comprising: generating a plasma in the reaction zone; and contacting reactant matter with the plasma in the reaction zone wherein the pressure in the reaction zone is at least 75 psig.
1 1. The method as claimed in claim 10, wherein the reactant matter includes natural gas.
12. The method as claimed in claim 10, wherein the plasma is generated by flowing a plasma forming fluid flow through a reaction zone through which an electrical discharge is being effected
13. The method as claimed in claim 12, wherein the plasma forming fluid includes reactant matter
14. A method of operating a plasma reactor as claimed in claim 6, comprising: contacting reactant matter with a plasma in a reaction zone, wherein the pressure in the reaction zone is at least 75 psig.
15. A reactor, including an internal surface defining an internal space including a reaction zone, comprising: a plasma generator including: a first electrode, configured for electrical coupling to a current and voltage source; and a second electrode, spaced apart from and disposed in electrical discharge communication with the first electrode through the internal space, and including an operative second electrode surface portion; wherein the reaction zone is disposed between the first electrode and the operative second electrode surface portion; such that, when a plasma forming gaseous fluid is disposed within the reaction zone and a sufficient electrical potential difference is applied between the first electrode and the operative second electrode surface portion, an electrical discharge is effected between the first electrode and the operative second electrode surface portion and through the reaction zone, and at least a fraction of the plasma forming gaseous fluid is converted into a plasma; and wherein the first electrode is mounted within a reaction vessel with a mounting structure including an internal mounting structure surface defining a portion of the internal surface, wherein the mounting surface is disposed in fluid communication with the reaction zone; and wherein the minimum distance between the operative second electrode surface and the mounting structure is at least two (2) inches.
16. The reactor as claimed in claim 15, wherein the operative second electrode surface portion is the electrically conductive surface portion of the interior surface which is closest to the first electrode.
17. The reactor as claimed in claim 15, wherein the internal mounting structure surface is electrically non-conductive.
18. The reactor as claimed in claim 17, wherein the upstream fluid passage portion is defined by an upstream conduit wall disposed upstream of the reaction zone, wherein the upstream conduit wall includes at least one electrically conductive upstream conduit wall surface portion; and wherein any electrically conductive upstream conduit wall surface portion, which is disposed in electrical discharge communication with the first electrode, is disposed further from the first electrode than the operative second electrode surface portion;
19. The reactor as claimed in claim 18, wherein the upstream conduit wall includes an upstream solid particulate deposition susceptible conduit wall surface portion configured for becoming coupled to a solid particulate upon approach of the solid particulate to the upstream solid particulate deposition susceptible conduit wall surface portion.
20. The reactor as claimed in claim 18, wherein the downstream fluid passage portion is defined by a downstream internal conduit surface including a downstream solid particulate deposition susceptible conduit surface portion, wherein the downstream solid particulate deposition susceptible conduit surface portion is configured for becoming coupled to a solid particulate upon approach of the solid particulate to the downstream solid particulate deposition susceptible conduit surface portion.
21. The reactor as claimed in claim 15, wherein the mounting surface includes a solid particulate deposition susceptible mounting surface portion configured for becoming coupled to a solid particulate upon approach of the solid particulate to the solid particulate deposition susceptible mounting surface portion
22. The reactor as claimed in claim 18, wherein the upstream fluid passage portion extends between the reaction zone and the mounting structure.
23. A method of operating the reactor as claimed in claim 15, comprising: generating a plasma in the reaction zone; and contacting reactant matter with the plasma in the reaction zone to effect production of product matter..
24. The method as claimed in claim 23, wherein the product matter includes solid particulate.
25. The method as claimed in claim 24, further comprising providing a carrier fluid flow for sweeping carbon from the reaction zone, wherein the downstream fluid passage portion is defined by a downstream internal conduit surface including a downstream solid particulate deposition susceptible conduit surface portion, wherein the downstream solid particulate deposition susceptible conduit surface portion is configured for becoming coupled to the produced solid particulate upon approach of the produced solid particulate to the downstream solid particulate deposition susceptible conduit surface portion
26. The method as claimed in claim 25, wherein the minimum velocity of the carrier fluid flow is one (1) cubic metre per hour..
27. The method as claimed in claim 23, wherein the reactant matter includes natural gas.
28. The method as claimed in claim 23, wherein the plasma forming fluid includes the reactant matter.
29. The method as claimed in claim 23, wherein the plasma forming fluid is a plasma forming fluid flow
30. The method as claimed in claim 23, wherein at least a fraction of the carrier fluid flow is derived from the plasma forming fluid flow.
31. A reactor, defining a fluid passage portion for flowing a plasma forming gaseous fluid, wherein the fluid passage portion includes an upstream fluid passage portion and a downstream fluid passage portion, comprising: a plasma generator including: a first electrode, configured for electrical coupling to a current and voltage source; and a second electrode, spaced apart from and disposed in electrical discharge communication with the first electrode through the internal space, and including an operative second electrode surface portion; wherein a reaction zone is defined between the first electrode and the operative second electrode portion, and the downstream fluid portion extends downstream from within the reaction zone; such that, when the plasma forming gaseous fluid is disposed in the reaction zone and a sufficient electrical potential difference is applied between the first electrode and the operative second electrode surface portion, an electrical discharge is effected between the first electrode and the operative second electrode surface portion and through the reaction zone, and at least a fraction of the plasma forming gaseous fluid is converted into a plasma; wherein the operative second electrode surface portion is spaced apart from the first electrode by a minimum distance of less than 0.15 inches; and wherein the upstream fluid passage portion is defined by an upstream conduit wall disposed upstream of the reaction zone, wherein the upstream conduit wall includes at least one electrically conductive upstream conduit wall portion; and wherein any electrically conductive upstream conduit wall portion, which is disposed in electrical discharge communication with the first electrode, is disposed further from the first electrode than the operative second electrode surface portion; and wherein the operative second electrode surface portion is disposed in thermal communication with at least one electrically conductive upstream conduit wall portion.
32. The reactor as claimed in claim 31 , wherein the upstream conduit wall includes an upstream solid particulate deposition susceptible conduit wall portion configured for becoming coupled to solid particulate upon approach of the solid particulate to the upstream solid particulate deposition susceptible conduit wall portion.
33. The reactor as claimed in claim 31 , wherein the downstream fluid passage portion is defined by a downstream internal conduit surface including a downstream solid particulate deposition susceptible conduit surface portion, wherein the downstream solid particulate deposition susceptible conduit surface portion is configured for becoming coupled to solid particulate upon approach of the solid particulate to the downstream solid particulate deposition susceptible conduit surface portion
34. The reactor as claimed in claim 31 , wherein the reaction zone is provided in an internal space defined by an internal surface of the reaction vessel; and wherein the operative second electrode surface portion is the electrically conductive surface portion of the interior surface which is closest to the first electrode.
35. The reactor as claimed in claim 34, wherein the upstream conduit wall merges with the operative second electrode surface portion
36. A method of operating the reactor as claimed in claim 31 , comprising: generating a plasma in the reaction zone; and contacting reactant matter with the plasma in the reaction zone to effect production of product matter;
37. The method as claimed in claim 36, wherein the product matter includes solid particulate.
38. The method as claimed in claim 37, further comprising providing a carrier fluid flow for sweeping carbon from the reaction zone, wherein the downstream fluid passage portion is defined by a downstream internal conduit surface including a downstream solid particulate deposition susceptible conduit surface portion, wherein the downstream solid particulate deposition susceptible conduit surface portion is configured for becoming coupled to the produced solid particulate upon approach of the produced solid particulate to the downstream solid particulate deposition susceptible conduit surface portion
39. The method as claimed in claim 38, wherein the minimum flow rate of carrier fluid flow is one (1) cubic metre per hour.
40. The method as claimed in claim 36, wherein the reactant matter includes natural gas.
41. The method as claimed in claim 36, wherein the plasma forming fluid includes the reactant matter.
42. The method as claimed in claim 36, wherein the plasma forming fluid is a plasma forming fluid flow
43. The method as claimed in claim 38, wherein at least a fraction of the carrier fluid flow is derived from the plasma forming fluid flow.
44. A reactor, defining a fluid passage portion for flowing a plasma forming gaseous fluid, wherein the fluid passage portion includes an upstream fluid passage portion and a downstream fluid passage portion, comprising: a plasma generator including: a first electrode configured for electrical coupling to a current and voltage source; and a second electrode spaced apart from and disposed in electrical discharge communication with the first electrode through the internal space; wherein a reaction zone is defined between the first electrode and the second electrode, and the downstream fluid passage portion extends downstream from within the reaction zone, and the upstream fluid passage portion is disposed upstream of the reaction zone; such that, when the plasma forming gaseous fluid is disposed within the reaction zone and a sufficient electrical potential difference is applied between the first electrode and the second electrode, an electrical discharge is effected between the first electrode and the second electrode and through the reaction zone, and at least a fraction of the plasma forming gaseous fluid is converted into a plasma; wherein the first electrode is at least partially disposed in the downstream fluid passage portion and is spaced apart from an internal conduit wall of the downstream fluid passage portion to define a fluid flow space in the downstream fluid passage portion, wherein, in any plane which intersects that portion of the first electrode disposed in the downstream fluid passage portion, and which is disposed in a normal orientation relative to an axis of the downstream fluid passage portion being intersected, the ratio of the diameter of the first electrode to the diameter of the downstream fluid passage portion is between two (2) and five (5).
45. The reactor as claimed in claim 44, wherein the second electrode includes an operative second electrode surface portion, and wherein, when the plasma forming gaseous fluid is disposed within the reaction zone and a sufficient electrical potential difference is applied between the first electrode and the operative second electrode surface portion, the effected electrical discharge is between the first electrode surface and the operative second electrode surface portion and at least a fraction of the plasma forming gaseous fluid is converted into a plasma.
46. The reactor as claimed in claim 45, wherein the reaction zone is provided in an internal space defined by an internal surface of the reaction vessel; and wherein the operative second electrode surface portion is the electrically conductive surface portion of the interior surface which is closest to the first electrode.
47. The reactor as claimed in claim 44, wherein the upstream fluid passage portion is defined by an upstream conduit wall disposed upstream of the reaction zone, wherein the upstream conduit wall includes at least one electrically conductive upstream conduit wall portion; and wherein any electrically conductive upstream conduit wall portion, which is disposed in electrical discharge communication with the first electrode, is disposed further from the first electrode than the operative second electrode surface portion;
48. A method of operating the reactor as claimed in claim 44, comprising: generating a plasma in the reaction zone; and contacting reactant matter with the plasma in the reaction zone to effect production of product matter;
49. The method as claimed in claim 48, wherein the product matter includes solid particulate (includes carbon-comprising particulate).
50. The method as claimed in claim 49, further comprising providing a carrier fluid flow for sweeping carbon from the reaction zone, wherein the downstream fluid passage portion is defined by a downstream internal conduit surface including a downstream solid particulate deposition susceptible conduit surface portion, wherein the downstream solid particulate deposition susceptible conduit surface portion is configured for becoming coupled to the produced solid particulate upon approach of the produced solid particulate to the downstream solid particulate deposition susceptible conduit surface portion
51. The method as claimed in claim 50, wherein the minimum flow rate of carrier fluid flow is one (1) cubic metre per hour.
52. The method as claimed in claim 48, wherein the reactant matter includes natural gas.
53. The method as claimed in claim 48, wherein the plasma forming fluid includes the reactant matter.
54. The method as claimed in claim 48, wherein the plasma forming fluid is a plasma forming fluid flow
55. The method as claimed in claim 50, wherein at least a fraction of the carrier fluid flow is derived from the plasma forming fluid flow.
56. A reactor, including an internal space defining a fluid passage portion for flowing a plasma forming gaseous fluid, wherein the fluid passage portion includes a reaction zone, comprising: a plasma generator including: a first electrode, configured for electrical coupling to a current and voltage source, and including an operative first electrode surface portion; and a second electrode, spaced apart from and disposed in electrical discharge communication with the first electrode through the internal space, and including an operative second electrode surface portion; wherein the reaction zone is disposed between the first and second electrodes; such that, when a plasma forming gaseous fluid is disposed within the reaction zone and a sufficient electrical potential difference is applied between the operative first electrode surface portion and the operative second electrode surface portion, an electrical discharge is effected between the operative first electrode surface portion and the operative second electrode surface portion and through the reaction zone, and at least a fraction of the plasma forming gaseous fluid is converted into a plasma; wherein an operative distance is defined along the longitudinal axis of the first electrode between: (i) a plane in which is disposed an axis normal to the operative first electrode surface portion and (ii) a tip of the first electrode downstream of the operative first electrode surface portion, wherein the operative distance is at least 0.25 inches.
57. The reactor as claimed in claim 56, wherein the reaction zone is provided in an internal space defined by an internal surface of the reaction vessel; and wherein the operative second electrode surface portion is the electrically conductive surface portion of the interior surface which is closest to the first electrode.
58. A method of operating the reactor as claimed in claim 56, comprising: generating a plasma in the reaction zone; and contacting reactant matter with the plasma in the reaction zone to effect production of product matter;
59. The method as claimed in claim 58, wherein the product matter includes solid particulate.
60. The method as claimed in claim 59, further comprising providing a carrier fluid flow for sweeping carbon from the reaction zone, wherein the downstream fluid passage portion is defined by a downstream internal conduit surface including a downstream solid particulate deposition susceptible conduit surface portion, wherein the downstream solid particulate deposition susceptible conduit surface portion is configured for becoming coupled to the produced solid particulate upon approach of the produced solid particulate to the downstream solid particulate deposition susceptible conduit surface portion
61. The method as claimed in claim 60, wherein the minimum velocity of the carrier fluid flow is one (1) cubic metre per hour.
62. The method as claimed in claim 58, wherein the reactant matter includes natural gas.
63. The method as claimed in claim 58, wherein the plasma forming fluid includes the reactant matter.
64. The method as claimed in claim 58, wherein the plasma forming fluid is a plasma forming fluid flow
65. The method as claimed in claim 60, wherein at least a fraction of the carrier fluid flow is derived from the plasma forming fluid flow.
66. A reactor, defining an internal space including a reaction zone, and including an inlet fluidly coupled to the reaction zone with a fluid introduction passage for introducing a plasma forming gaseous fluid into the reaction zone, comprising: a plasma generator including: a first electrode configured for electrical coupling to a current and voltage source; and a second electrode spaced apart from and disposed in electrical discharge communication with the first electrode through the internal space; wherein the reaction zone is disposed between the first and second electrodes; such that, when a plasma forming gaseous fluid is disposed within the reaction zone and a sufficient electrical potential difference is applied between the first electrode and the second electrode, an electrical discharge is effected between the first electrode and the second electrode and through the reaction zone, and at least a fraction of the plasma forming gaseous fluid is converted into a plasma; and wherein the reaction vessel includes a heat exchanger disposed in heat transfer communication with the fluid introduction passage for effecting heat transfer to plasma forming gaseous fluid being introduced to the reaction zone.
67. The reactor as claimed in claim 66, wherein the heat exchanger includes an induction heater.
68. A method of operating the reactor as claimed in claim 66, comprising: generating a plasma in the reaction zone from a plasma forming fluid; and contacting reactant matter with the plasma in the reaction zone to effect production of product matter, wherein the plasma forming fluid is heated to a temperature of at least 400°C by a heat exchanger of the reactor.
69. The method as claimed in claim 68, wherein the reactant matter includes natural gas.
70. The method as claimed in claim 68, wherein the plasma forming fluid includes the reactant matter.
71. The method as claimed in claim 68, wherein the plasma forming fluid is a plasma forming fluid flow.
72. A method of operating a plasma reactor comprising: providing a reactor including a reaction zone, and also including: a plasma generator including: a first electrode configured for electrical coupling to a current and voltage source; and a second electrode spaced apart from and disposed in electrical discharge communication with the first electrode through the internal space; wherein the reaction zone is disposed between the first and second electrodes; and wherein the reactor further includes a pressure boundary, wherein the pressure boundary defines, and is in thermal communication with, an internal space including the reaction zone, and wherein the pressure boundary includes an extemalmost surface that is exposed to, and in thermal communication with the outside environment; providing a plasma forming gaseous fluid within the reaction zone; applying an electrical potential difference between the first electrode and the second electrode sufficient to effect an electrical discharge between the first electrode and the second electrode and through the reaction zone, and to convert at least a fraction of the provided plasma forming gaseous fluid into plasma; wherein the material of the pressure boundary is characterized by an average heat transfer coefficient of at least 100 W / (meter-Kelvin).
73. The method as claimed in claim 72; wherein the reactant matter includes natural gas.
74. The method as claimed in claim 72; wherein the plasma forming fluid includes the reactant matter.
75. The method as claimed in claim 72; wherein the plasma forming fluid is a plasma forming fluid flow
76. The method as claimed in claim 72; wherein the plasma is characterized by a temperature of at least 2000 degrees Celsius.
PCT/CA2012/000029 2011-01-14 2012-01-13 Plasma reactor and method of operation thereof WO2012094743A1 (en)

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