WO1994018550A1 - A method for measuring temperature, molecular composition or molecular densities in gases - Google Patents

A method for measuring temperature, molecular composition or molecular densities in gases Download PDF

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Publication number
WO1994018550A1
WO1994018550A1 PCT/SE1994/000100 SE9400100W WO9418550A1 WO 1994018550 A1 WO1994018550 A1 WO 1994018550A1 SE 9400100 W SE9400100 W SE 9400100W WO 9418550 A1 WO9418550 A1 WO 9418550A1
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WO
WIPO (PCT)
Prior art keywords
molecular
temperature
densities
lines
process room
Prior art date
Application number
PCT/SE1994/000100
Other languages
French (fr)
Inventor
Lars B. BÅÅTH
Original Assignee
Mefos, Stiftelsen För Metallurgisk Forskning
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 Mefos, Stiftelsen För Metallurgisk Forskning filed Critical Mefos, Stiftelsen För Metallurgisk Forskning
Priority to CA002155339A priority Critical patent/CA2155339C/en
Priority to EP94906423A priority patent/EP0698205B1/en
Priority to KR1019950703205A priority patent/KR100469208B1/en
Priority to JP6517956A priority patent/JPH08508338A/en
Priority to DE69429261T priority patent/DE69429261T2/en
Priority to AT94906423T priority patent/ATE209783T1/en
Priority to AU60130/94A priority patent/AU688302B2/en
Publication of WO1994018550A1 publication Critical patent/WO1994018550A1/en
Priority to US09/152,853 priority patent/US6084415A/en
Priority to US09/595,957 priority patent/US6244743B1/en

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Classifications

    • G—PHYSICS
    • G01—MEASURING; TESTING
    • G01N—INVESTIGATING OR ANALYSING MATERIALS BY DETERMINING THEIR CHEMICAL OR PHYSICAL PROPERTIES
    • G01N22/00—Investigating or analysing materials by the use of microwaves or radio waves, i.e. electromagnetic waves with a wavelength of one millimetre or more

Definitions

  • a method for measuring temperature, molecular composition or molecular densities in gases is a method for measuring temperature, molecular composition or molecular densities in gases.
  • Tliis invention relates to a method for measuring temperature, molecular densities and molecular composition or any combination thereof, in gases and/or flames in melting and/or combustion processes.
  • None of the above patents discloses, discusses, or makes possible the simultaneous determination of a multiple of molecular lines and species or can determine molecular densities and temperature in a working melting process or combustion process without any interaction with the gas flow.
  • Electromagnetic waves may penetrate media of varying physical properties, changing its amplitude and phase in a way which is specific to the content of the media.
  • molecular gas will emit or absorb electromagnetic radiation mainly depending on its density, the physical temperature, or the radiation field in the area where the gas resides.
  • Continuum radiation will also be affected when penetrating a media in the sense that the amplitude will be attenuated and the propagation velocity will change, resulting in a sudden change of phase in the interface area.
  • the radioband is of particular interest in that here waves can penetrate deeper into dusty areas and also detect and measure complicated molecules by their rotational transitions.
  • Fig 1 shows an experimental set up.
  • Fig 2 shows schematically a more sofisticated apparatures.
  • Fig 3 is a top view of the apparatures in fig 2.
  • Each molecular species has its own fingerprint in the form of a spectrum of lines, in the radio domain mainly determined by the quantified transitions between vibrational- and/or rotational states.
  • Molecular lines in the atmosphere are very much broadened due to the relatively high pressure. The most significant exception is if the molecular flow is highly directive, e.g. if we are looking through the flow at an angle perpendicular to that of the flow. In that case the pressure broadening will be much less and molecular lines can be well separated. This exception is the case for the gas flow in chimneys or through the gas flow from any burning process if viewed across the flow.
  • a chimney (11) is made out of ceramic material, chrome-magnesite and charmotte, and covered with steel.
  • the chimney has an opening (12) for an oil burner.
  • the steel cover has two opposite windows (13), with intact ceramic materiel. Outside the windows (13) and in line with the windows are two parabolic antennas (14,15).
  • One of the parabola is connected to a transmitter (16) and the other parabola (15) is connected to a receiver (17).
  • the transmitter consists of a signal generator which is stepped in frequency over a wide frequency band.
  • the received signal is compared with the transmitted signal in a cross-correlator (18) connected to a computer (19).
  • the received signal consists of a number of spectral lines emitted from the gas inside the chimney overlaid on the background transmitted signal.
  • the transmitted signal is used to calibrate the frequency response of the system and the attenuation through the chimney walls by looking at the received signal between the molecular lines. This baseline will then be subtracted from the received signal and the intensities of the molecular spectral lines can be determined as calibrated inside the chimney.
  • the system is further calibrated by measuring the signal transmitted through the chimney as a function of frequency when the chimney is emty.
  • the registered spectrum is stored in a computer.
  • a database is searched for known lines which coincides in frequency with maxima within the observed spectrum. Thereafter a Gaussian model fit is made to the line in order to determine the amplitude, frequency, and line width.
  • a line is considered to be detected if the amplitude of the Gaussian fitted line is more than three times the calculated noise level.
  • the measured amplitudes are then calibrated to an absolute temperature scale.
  • N u /g u N rot /Q(T rot ) e" Eu ⁇ rot
  • N u is the number of molecules in the upper energy level of the transition
  • g u is the statistical weight of the transition
  • E u is the energy of the upper energy level in Kelvin
  • Q is the rotational constant.
  • T rol is physical temperature, in the case of burning processes where the excitation is dominated by collisions due to the high temperature
  • N rot is the column density of the molecules of this particular specie.
  • N u /g u is directly proportional to the intensity integrated over the spectral line and can therefore be measured. If a number of spectral lines from a molecule are available, then both the density (if the path length is known) and the physical temperature (if the molecule is predominantly collision excited) can be determined simultaneously. If lines from other molecules are also present, then also the densities of these molecules may be measured from the intensity of a single molecular line.
  • the radio antenna can also consist of an interferometer where the elements are radio horn antennas mounted in a plane (31,32) and with properly adjusted delay lines as shown in Figure 2. Then the two dimensional distribution of molecular densities and temperature can be reconstructed by transforming from the aperture (u,v) plane to the image plane.
  • the system consists of interferometers (32) which are looking into the processroom or exhaust channel from different angles as is shown in Figure 3, then the densities and the temperature may also be recovered in three dimensions by a Radon transform, similar to what is used in computer tomography.
  • a Radon transform similar to what is used in computer tomography.
  • Such a system can recover the temperature distribution in three dimensions within a hot gas (or a flame). It can also, which will be more important, simultaneously recover the three dimensional density distribution of each delectable molecular specie.
  • FIG. 4 shows the spectrum observed in the radioband 20-40 GHz through the flow in the chimney. Most of these lines come from SO 2 , some others from NH 3 and other molecules. It is therefore clearly possible to detect molecules within the radioband in gas flows on earth. As a consequence it is then also possible to make images of such a flow.
  • Fig. 5 shows the identifications of some of the lines from one observations. Using SO2 as a tracer it was possible to determine the temperature as well as the density of SO 2 as function of time.

Abstract

A measuring technique and method are provided to simultaneously determine the molecular density of several molecular species and the temperature within a closed process room in a melting or combustion process. In such processes in the industry, e.g. in metallurgic process industry, it is important to determine the temperature and the contents within the gas or flame without physically connect to or disturb the process. This has shown to raise large problems especially at high temperatures. The radio signal over a frequency band is measured on the outside of the process room through a window in the mantel covering as a function of frequency and registered on a computer as a radio spectrum. The system is calibrated by using a known signal transmitted through the process room. The spectral lines are identified by their frequency from a database. The temperature is determined from several lines of the same molecular specie and the molecular densities are determined from the intensities of the lines. The method is suitable to determine vibrational and rotational excitation of molecular species in the radio wavelength range of 500 m et 30 νm. The densities of molecular species and the temperature can be imaged in three dimensions inside the process room or exhaust channel if interferometers are used for simultaneous two dimensional imaging from several azimuth directions.

Description

A method for measuring temperature, molecular composition or molecular densities in gases.
Tliis invention relates to a method for measuring temperature, molecular densities and molecular composition or any combination thereof, in gases and/or flames in melting and/or combustion processes.
Conventional gas analysis methods using IR-paramagnetic- and masspectrometer technology need a psychical contact with the gas to be analysed. This means that the gas have to be cooled before entering the analyser which may affect the results of the measurements. .Another disadvantage with conventional gas analysers is that they can not simultaneously measure the temperature of the gas and analyse the gas.
It is known that the attenuation of a continuum radio signal can be used to recover the amount of black smoke in exhaust fumes, .JP 60-64234. This patent method does not determine any molecular content, nor does it determine any temperature.
It is also known that the changes in refractive index of flying ash can be used to determine the carbon content therein, WO 90/03568. This patent method does not distinguish between molecular species and does not measure any spectral lines or determine molecular densities, configuration, or temperature.
It is also known attenuation and reflection in the exhaust fumes from a reaction engine can be used to determine changes in the exhaust fume composition, WO 90/03568. This method does not determine any molecular species or temperature.
It is also known that the existence of a specific molecular specie can be decided if the molecular gas is first mixed with a drive gas and then injected into a cavity chamber, patent US-A-5124 653. The cavity is then adjusted to the wavelength of the molecular transition and the molecular gas is excited by injecting a radio signal. The radio transmitter is then turned off .and the molecule will emit at its specific frequency if it is present. This method measures a single molecular line at the time and can only detect the molecular species for which it is specifically adjusted. This method does not measure the temperature or the molecular density within the process since the molecular gas has to be taken out of the process-room to the special cavity and the gas is also contaminated with a drive gas.
None of the above patents discloses, discusses, or makes possible the simultaneous determination of a multiple of molecular lines and species or can determine molecular densities and temperature in a working melting process or combustion process without any interaction with the gas flow.
Changes in the pattern of electromagnetic wave fronts represent the most sensitive probes in physics. Electromagnetic waves may penetrate media of varying physical properties, changing its amplitude and phase in a way which is specific to the content of the media. Thus molecular gas will emit or absorb electromagnetic radiation mainly depending on its density, the physical temperature, or the radiation field in the area where the gas resides. Continuum radiation will also be affected when penetrating a media in the sense that the amplitude will be attenuated and the propagation velocity will change, resulting in a sudden change of phase in the interface area. The radioband is of particular interest in that here waves can penetrate deeper into dusty areas and also detect and measure complicated molecules by their rotational transitions.
It is an object of the invention to provide an accurate and reliable method to analyse a gas and to determine the temperature of a gas directly in an industrial process without physical contact with the gas that is being analysed and without disturbing the gas and the process.
The invention will be described more closely with reference to the drawings.
Fig 1 shows an experimental set up.
Fig 2 shows schematically a more sofisticated apparatures.
Fig 3 is a top view of the apparatures in fig 2.
Each molecular species has its own fingerprint in the form of a spectrum of lines, in the radio domain mainly determined by the quantified transitions between vibrational- and/or rotational states. Molecular lines in the atmosphere are very much broadened due to the relatively high pressure. The most significant exception is if the molecular flow is highly directive, e.g. if we are looking through the flow at an angle perpendicular to that of the flow. In that case the pressure broadening will be much less and molecular lines can be well separated. This exception is the case for the gas flow in chimneys or through the gas flow from any burning process if viewed across the flow.
The invention can be best described with an experimental set-up shown in Figure 1. Here a chimney (11) is made out of ceramic material, chrome-magnesite and charmotte, and covered with steel. The chimney has an opening (12) for an oil burner. The steel cover has two opposite windows (13), with intact ceramic materiel. Outside the windows (13) and in line with the windows are two parabolic antennas (14,15). One of the parabola is connected to a transmitter (16) and the other parabola (15) is connected to a receiver (17). The transmitter consists of a signal generator which is stepped in frequency over a wide frequency band. The received signal is compared with the transmitted signal in a cross-correlator (18) connected to a computer (19).
The received signal consists of a number of spectral lines emitted from the gas inside the chimney overlaid on the background transmitted signal. The transmitted signal is used to calibrate the frequency response of the system and the attenuation through the chimney walls by looking at the received signal between the molecular lines. This baseline will then be subtracted from the received signal and the intensities of the molecular spectral lines can be determined as calibrated inside the chimney.
The system is further calibrated by measuring the signal transmitted through the chimney as a function of frequency when the chimney is emty.
The registered spectrum is stored in a computer. A database is searched for known lines which coincides in frequency with maxima within the observed spectrum. Thereafter a Gaussian model fit is made to the line in order to determine the amplitude, frequency, and line width. A line is considered to be detected if the amplitude of the Gaussian fitted line is more than three times the calculated noise level. The measured amplitudes are then calibrated to an absolute temperature scale.
SUBSTITUTE SHEET If a number of lines from the same molecular specie can be detected, then the relative population of the various energy levels may be determined. This relation is mainly determined by the physical temperature of the gas and the density of the molecular specie as: Nu/gu = Nrot/Q(Trot) e"Eu τrot where Nu is the number of molecules in the upper energy level of the transition, gu is the statistical weight of the transition, Eu is the energy of the upper energy level in Kelvin, Q is the rotational constant. Trol is physical temperature, in the case of burning processes where the excitation is dominated by collisions due to the high temperature, and Nrot is the column density of the molecules of this particular specie. Nu/gu is directly proportional to the intensity integrated over the spectral line and can therefore be measured. If a number of spectral lines from a molecule are available, then both the density (if the path length is known) and the physical temperature (if the molecule is predominantly collision excited) can be determined simultaneously. If lines from other molecules are also present, then also the densities of these molecules may be measured from the intensity of a single molecular line.
The radio antenna can also consist of an interferometer where the elements are radio horn antennas mounted in a plane (31,32) and with properly adjusted delay lines as shown in Figure 2. Then the two dimensional distribution of molecular densities and temperature can be reconstructed by transforming from the aperture (u,v) plane to the image plane.
If then the system consists of interferometers (32) which are looking into the processroom or exhaust channel from different angles as is shown in Figure 3, then the densities and the temperature may also be recovered in three dimensions by a Radon transform, similar to what is used in computer tomography. Such a system can recover the temperature distribution in three dimensions within a hot gas (or a flame). It can also, which will be more important, simultaneously recover the three dimensional density distribution of each delectable molecular specie. These measurement are also performed without any physical probe since the radio signal may, as indeed was the case in our pilot experiment, that will be described penetrate through the ceramic wall of the chimney.
In the apparatus shown in Fig 2, an experiment was carried out. An oxy/oil burner was installed and was burning in a steady state.
BSTBTUTE SHEET Fig. 4 shows the spectrum observed in the radioband 20-40 GHz through the flow in the chimney. Most of these lines come from SO2, some others from NH3 and other molecules. It is therefore clearly possible to detect molecules within the radioband in gas flows on earth. As a consequence it is then also possible to make images of such a flow. Fig. 5 shows the identifications of some of the lines from one observations. Using SO2 as a tracer it was possible to determine the temperature as well as the density of SO2 as function of time.
SUBSTITUTE SHEET

Claims

CLAIMSWe claim:
1. A method for measuring temperature, molecular composition or molecular densities or any combination thereof in gases and/or flames in melting and/or combustion processes, characterized in that it comparises measurning electromagnetic radiation in the radio range defined as wavelengts between 500 m and 30 μ with a radio antenna positioned outside a process room and/or exhaust shannel, performing the measurements during a continuous melting and /or combustion process, and measuring spectral lines emitted by the high temperature collision excited molecules, and absorbed from a background signal when the population of energy levels for the collision excited molecule permits this.
2. A method as claimed in claim 1 characterised in that molecular species are identified from the measured spectrum by comparing the detected spectral lines with molecular lines from an identification data base.
3. A method as claimed in claim 2, characterised in that the temperature is measured inside the process room and/or exhaust channel by measuring the relative intensities of several lines from the same molecular specie and compmng with a theoretical relation calculated for the expected population of energy levels as a function of temperature.
4. A method as claimed in claim 3, characterised in that the density of the molecular species are determined by measuring the absolute intensity of a spectral line from that specie and compare with the theoretically expected intensity for the already determined temperature.
5. A method as claimed in claim 1 or 4 characterised in that the electromagnetic radiation is measured in narrow frequency channels resulting in a frequency spectrum which is compared with a known reference signal and is calibrated against the back of the process room and/or exhaust channel transmitted copy of the reference signal.
SUBSTITUTE SHEET
6. A method as claimed in claim 5, characterised in that the reference and background signal is created in steps of narrow frequency channels by stepping a signal generator in frequency.
7. A method as claimed in claims 1, 2, 3, 4, 5, or 6, characterised in that the receiving antenna is an interferometer and that the two dimensional distribution of densities and temperature are reconstructed from the cross correlation of the signal of the individual interferometer elements.
8. A method as claimed in claim 7, characterised in that the signal is received simultaneously by interferometers placed at several azimuth angles around the processroom and/or exhaust channel and the three dimensional distribution of densities and temperature are reconstructed by projections.
SUBSTITUTE SHEET
PCT/SE1994/000100 1993-02-03 1994-02-03 A method for measuring temperature, molecular composition or molecular densities in gases WO1994018550A1 (en)

Priority Applications (9)

Application Number Priority Date Filing Date Title
CA002155339A CA2155339C (en) 1993-02-03 1994-02-03 A method for measuring temperature, molecular composition or molecular densities in gases
EP94906423A EP0698205B1 (en) 1993-02-03 1994-02-03 A method for measuring temperature, molecular composition or molecular densities in gases
KR1019950703205A KR100469208B1 (en) 1993-02-03 1994-02-03 Method for measuring temperature, molecular composition or molecular density in gas
JP6517956A JPH08508338A (en) 1993-02-03 1994-02-03 Method for measuring gas temperature, molecular composition or molecular density
DE69429261T DE69429261T2 (en) 1993-02-03 1994-02-03 METHOD FOR MEASURING TEMPERATURE, MOLECULAR COMPOSITION OR MOLECULAR DENSITY IN GASES
AT94906423T ATE209783T1 (en) 1993-02-03 1994-02-03 METHOD FOR MEASURING TEMPERATURE, MOLECULAR COMPOSITION OR MOLECULAR DENSITIES IN GASES
AU60130/94A AU688302B2 (en) 1993-02-03 1994-02-03 A method for measuring temperature, molecular composition or molecular densities in gases
US09/152,853 US6084415A (en) 1993-02-03 1998-09-14 Method for measuring molecular composition or molecular densities in gases
US09/595,957 US6244743B1 (en) 1993-02-03 2000-06-19 Method for measuring temperature, molecular composition or molecular densities in gases

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
SE9300347A SE501473C2 (en) 1993-02-03 1993-02-03 Ways of determining the state of gases and flames in melt and combustion processes
SE9300347-3 1993-02-03

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US08/510,444 Continuation-In-Part US5829877A (en) 1993-02-03 1995-08-02 Method for measuring temperature of at least one of a gas and a flame in a combustion process

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EP (1) EP0698205B1 (en)
JP (1) JPH08508338A (en)
KR (1) KR100469208B1 (en)
AT (1) ATE209783T1 (en)
AU (1) AU688302B2 (en)
DE (1) DE69429261T2 (en)
ES (1) ES2169066T3 (en)
SE (1) SE501473C2 (en)
WO (1) WO1994018550A1 (en)

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US4693614A (en) * 1983-06-20 1987-09-15 Sumitomo Metal Industries, Ltd. Apparatus for detecting slag outflow
US5124653A (en) * 1989-09-01 1992-06-23 Uwe Andresen Method and apparatus for determining the concentration of compounds in a gas mixture by microwave gas analysis

Cited By (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP0829020A2 (en) * 1995-03-17 1998-03-18 The Regents Of The University Of California Narrow field electromagnetic sensor system and method
EP0829020A4 (en) * 1995-03-17 1998-07-08 Univ California Narrow field electromagnetic sensor system and method
WO2001050114A2 (en) * 1999-12-29 2001-07-12 Sebacur Ag Device for detecting munitions, drugs, explosives etc. using molecular spectroscopy in the radio frequency range
WO2001050114A3 (en) * 1999-12-29 2002-07-25 Sebacur Ag Device for detecting munitions, drugs, explosives etc. using molecular spectroscopy in the radio frequency range

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DE69429261D1 (en) 2002-01-10
KR100469208B1 (en) 2005-04-19
US6244743B1 (en) 2001-06-12
AU6013094A (en) 1994-08-29
DE69429261T2 (en) 2002-07-25
US5829877A (en) 1998-11-03
SE9300347L (en) 1994-08-04
JPH08508338A (en) 1996-09-03
AU688302B2 (en) 1998-03-12
SE501473C2 (en) 1995-02-27
SE9300347D0 (en) 1993-02-03
ES2169066T3 (en) 2002-07-01
EP0698205B1 (en) 2001-11-28
ATE209783T1 (en) 2001-12-15
US6084415A (en) 2000-07-04
KR960701359A (en) 1996-02-24
EP0698205A1 (en) 1996-02-28

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