WO1999010274A1 - Method for producing artificial diamonds - Google Patents

Abstract

The present invention relates to a method for producing artificial diamonds, wherein said method pertains to the techniques for producing materials with a high degree of hardness and more precisely to the synthesis of diamonds used in the production of diamond instruments. The method for producing artificial diamonds comprises applying an action on fullerene-containing graphite and on a catalyst by generating a pressure and heating within the diamond stability range and by maintaining the mixture at the synthesis temperature and pressure. This method is characterised in that the fullerene is introduced in an amount of between 10-2 and 6 x 10-1 wt.% of the graphite mass and in that the fullerene is distributed in said graphite mass. The fullerene can be introduced in the form of fullerene-containing soot or in the form of an extract of fullerenes. The method of the present invention allows for an increased yield of artificial diamonds at pressures not exceeding 5.5 GPa.

Description

 1

JOURNAL OF PRODUCTION ISSUES Κ LΧZΟΒ лас area of technology

The invention is available for the use of high-output materials.

5 materials, and, in particular, for the synthesis of diamonds, used, in particular, for the manufacture of diamond tools, as well as supplies and products for the business.

The prior art is that it has been developed and is currently used for

There are 10 different methods for the production of artificial diamonds from a group under conditions of high pressures and temperature.

However, the methods for producing artificial diamonds are known through the use of high pressure and temperature, which is a constant component mixture.

15 preset times (see ρeroshchagin L.F. - Selected labor. Synthetic diamonds and hydrothermal production. - Μ .: "Kauka", 1982. - S. 43-47, S. 78-86). To increase the degree of conversion of the group into diamond, alloying additives are introduced into the catalyst. increase pressure and synthesis time. However, the introduction of alloying additives complicates the technological process.

20 processes, therefore, as a rule, for the creation of economical processes, one type of catalyst is used. A change in the synthesis time in a wide range is limited by the temperature of the material of the on-line consumer. Pressure increase in order to increase the degree of heat loss of the panel into the diamond for the camera of a single volume

25 diets to reduce the number of its work cycles. which is not economically viable; isποlzοvanie same κameρ vysοκοgο pressure 7-10 GPa dρugοy κοn- sτρuκtsii πρi οdnοm and τοm same πρessοvοm οbορudοvanii sοπρyazhenο with decreasing οbema κameρy, chτο πρivοdiτ κ ποvyshennοmu ρasχοdu τveρdοgο sπlava, isποlzuemοgο for izgοτοvleniya κameρ pressures vysοκοgο

30 laziness.

The method of producing an artificial diamond is known, including the pulsed effect on the sample of the metal and the pressure and 2 nagρevοm πuτem προπusκaniya imπulsa eleκτρichesκοgο τοκa πο οbρaztsu, sοdeρzhaschemu meτall gρuππy of: copper, aluminum, niκel, zhelezο with vκlyucheniem melκοdisπeρsnyχ chasτits gρaφiτa, sρedny ρazmeρ κοτο- 5 ρyχ mκm 5-150, πρi following sοοτnοshenii κοmποnenτοv. Rev.%: group - 5-55, metal of the indicated group - 45-95 (see patent ΡΦ Νδ1820890, ΜPΚ С 01 Β 31/06. published 07.06.93).

The well-known method makes it possible to expedite the production technology of diamonds. Just for a well-known method, the low output is al-

10 mazov.

The method of producing diamonds is known, including exposure to carbon-bearing material with high pressure and heating in the region of stability of diamond. On the other hand, the carbon-friendly material used is al-ka-carbine in ammo. Larsa-karbin may

15 contain carbon in the amount of 99.0-99.9 wt.%, And heating leads to temperatures of 1400 - 700 ° С (see the automatic certificate СССΡ Νδ1533221. Ν Κ 02.03. 03/06.

A well-known method makes it possible to speed up the process and to increase the output of diamonds, but the same output rate still turns out to be short

20 hundred very high

Known for the production of polycrystalline diamond. including heating of carbon-containing material, separated from the catalyst by a separating layer, under pressure with the subsequent discharge and pressure. Material heating

25 Faster with a speed of 1500-2000 degrees with pressure and with a change in speed of 3-4 GPa. vydeρzhκu προvοdyaτ 0.5-5.0 s, πρi eτοm in κachesτ- vβ gιazdelya p'βgο slοα and π ^η lz ^{υ τ}

G / m and a dispersion of 1 -10 μm. Saving for production and synthesis are carried out at 1800 - - 2100Κ and a pressure of 7-8 GPa (see copyright certificate of the CCC)

30 Νδ1340030. ΚПΚ С 01 Β 31/06. Publicized 06/15/96.

A well-known method of operation uses a measurement of high temperature and pressure and does not prevent the production of diamonds in the form of 3 install

The method of producing diamond is known, including the compression of carbon-containing material for a good value and its heating with a pressure of 5 after that. On the other hand, the material used is different for different weight (see otherwise). At a depth of sample, a pressure gradient above 1 GPa / mm may be generated. The value of the main pressure reaches 15-25 GPa. Sample Compression May Happen As

10 hydrostatic, so also in non-hydrostatic conditions. The pressure must be reduced by heating below 1000 ° C (see international application \ Λ / Ο Νδ93 / 02012. ΜPΚ C 01 Β 31/00, published 04.02.93).

The well-known method of producing diamonds of high quality. in

15 parts are partly crystalline, but it does not require the use of excessive pressure and / or the creation of a pressure gradient. which complicates the use of the equipment.

The method of acquiring diamonds from the original raw materials containing the carbon components, including the main components, is known.

20 sistent vοzdeysτvie on νκazanny ma ^τ eρial pressure πρedelaχ 2-50 GPa πρi πρilοzhenii κ maτeρialν pressure gρadienτa and οdnοvρemen- nοe nagρevanie οblucheniem chasτi maτeρiala, κ κοτοροmu πρilοzhenο maκsimalnοe pressure lazeρnym radiation. For the most part, the most commercially available materials are sulleren C <i> or carbon

25 local microcircuits (latent of the USA Αδ 5360477. ΜPΜ C 30 Β 29/00. Published 01.11.1994).

The well-known method allows you to maintain a constant temperature of the receiver for a long time. However, the use of this equipment is significantly complicated.

30 The closest to the claimed method of production of artificial ^x diamonds are the methods of production of diamonds. Taken for just because it coincides with the claimed method for the largest number 4 facts The method includes operating on a fully-integrated vehicle located between two layers of a total mass of about 10% of the total mass. a pressure of 6.7 GPa and heating to a temperature of 5 parts 200-1850 ° C with catalysts: nickel. The balance and the κ-ο аль ((((((((Β .. αοααеΒοη Θ .. αοαιсеνιе S. ΡаЬге С, Яаззаϊ Α.- С _βη ΡиΙΙегеηез СагЬοη Зоигсе ϊοг Οιатοηα ¹ δνηϊз.η.η. 1993. 12927).

A well-known method of production allows to increase the output of diamonds up to 10% of the order of 90%;

DISCLOSURE OF THE INVENTION The objective of the present invention was to develop a cost-effective way of producing artificial diamonds, which would increase the pressure to a higher pressure.

The task posed is solved in that way in the process of making artificial diamonds. vκlyuchayuschegο vοzdeysτvie on Φνlleρen with gρaφi- 20 τοm and κaτalizaτοο pressure nagρevοm in οblasτi sτabilnοsτi al MAZ with ποsledνyuschey vydeρzhκοy πρi τemπeρaτνρe sinτeza, Φνlleρen vdηdατ in ΚΌLI -ΙΡΓΤ _^ ΠΡZHYAΙ Ι ΙΡΜ IΗΤΡPΒYA ΠΡ L 1 ^"- 6" ^* 0 ¹ ΜESS% Ο ^{τ the} softnesses of the group and distribute it in the mass of the group. Fullerene may be introduced in the form of emitting soot or as an extract of Φνl-25 lerenes.

Unexpectedly, it was found that if you enter into the full list not in the quality of the basic component. and as a small addition in quantity

1 P - β 10 ^" me - g — g% _ η _τ me _ yyyy gη, yag_itya _ and πη _g and h _τη _m η, yyg _π, η —ρ _π_, ρ_-pithy _. Ρ_ΓΠ_ Β_ mass of group . It is possible that a comparatively small 30 pressures (4.5-5.5 GPa) are significantly higher than the result of diverging temperatures. ϊ ^η and the content of <"* ™. pasture in the group <+> and τβ, π" β increases ^t βm 6 0 'wt.%, the output of diamonds will stop and we will exit with the exit of diamonds from the bulk.

5 П ^η AND СДДЖЖЕИИ πЧνл π ПЗЗ ИЖβ 10 Μ ЗСС.% ΟΤ ΜESCES Г ^Τ > Э '+> IEE There is also no increase in diamond output.

The above experiments are shown. A nec- essary condition for the production of increased diamond output is the separation of fullerene in the bulk of the group.

10 The discovered effect, for the most part, is visible. οbuslοvlen τem οbsτοyaτel- sτvοm, chτο in uκazannοm above κοlichesτvennοm inτeρvale mοleκuly φulleρena veduτ itself πρi οbρazοvanii diamond κaκ κaτalizaτορ, πο- dοbnο neκοτορym meτallam, on account οbρazοvaniya, naπρimeρ, κaρbidοv πρi lesτρuκτuρizaiii φulleρenοv πρi τemπeρaτuρe above 800 ° C or

15 is high, perhaps, in the center of diamond marketing.

The inventive method for the production of artificial diamonds is as follows. PREPARES A SHILE FROM A GROUP WITH ADDITION

NOW υ π π π ии ии ии ес ес ^{2 2 2 2} - 6 10 ¹ СС ESS.% Ο ^τ Μ Essentials and catalysts, for example, alloy of nickel and nickel, alloy with copper and manganese mixed with manganese and manganese. Received the bandwidth, it is supplied with pressure and placed in the bulk of the electrically isolated container, by filling the bulk with the product in the bulk of the product. Equipped with such a device, it places 25 high pressure in the device and compresses it to pressure. sοοτveτsτvuyuschegο οb- lasτi usτοychivοgο οbρazοvaniya diamond, and on account zaτem nagρevayuτ προ- πusκaniya eleκτρichesκοgο τοκa cheρez shiχτu dο τemπeρaτuρy, sοοτveτ- sτvuyuschey eτοmu pressure zaτem vydeρzhivayuτ πρi eτiχ τemπeρaτuρe and pressure τechenie zadannοgο vρemeni. After cutting off 30 electrical current, relieve pressure and extract the product of diamond synthesis. Then, it produces chemical enrichment, disperses the diamonds that are diverted to the grain, and for every grain distillation 6 mechanical value, according to the values that are assigned to the brand of diamonds.

Quick description of the drawing

5 The resulting effect is clearly traceable from the graph shown in Fig. 1. some results are shown for a simple separation of the proportion of the aggregate in the diamond (Ν), in weight%, it is only 1.5%. (κρiva 2).

10 BEST MODES FOR CARRYING OUT THE INVENTION

The following methods are used to study the method of producing artificial diamonds. EXAMPLE 1. PREPARING A SHILE FROM A GROUP WITH THE ADDITION OF FULLERIES

15 С ₆ ο + С ₇₀ in the amount of 0.15 wt.% Of the mass of the filter, entering them from the fullerene extract and the catalyst from the nickel alloy with manganese. Mixing of the ingredients is carried out in the mixer. achieving a division of the territory in the volume of the group. Then they flash. πο doubling its pressure of 10 ΜPa. and place in a cylindrical tank

20 Spare parts of a thermo-electric isolating tank, closing with burnt-down powder pouches from a mixture of slab and lime. The charged container places high pressure in the appliance of the type "very hot", compresses to 4.5 GPa, and heats up at a constant speed.

25 maintain ηρ and data for 10 minντ. After extracting it, it turns off the heat, relieves pressure and removes the synthesis product. After chemical enrichment, the group transfers the output to diamond, which made up 33.7% of the average aggregate in the average. For example, 2.

30 They perform the same operations and pressure and the same pressure, time of the discharge and temperature. and that in Example 1. we add C ₆ ο + C ₇₀ fullerenes in a quantity of 0.01 wt.% of the mass of the aggregate, introducing χ from ful - 7 Lorenogo extract. For the transition to diamond, it averaged 30.3% of the total sintering. Pρimeρ 3. 5 Βyποlnyayuτ Te same οπeρatsii and πρi τeχ same davleniyaχ, vρemeni You are a deρzhκi and τemπeρaτuρe, chτο and πρimeρe 1. dοbavleniem with φulleρenοv ο + C ₆ C ₇ ο κοlichesτve to 0.12 wt.% Οτ gρaφiτa weight of vvοdya iχ Φνl- Loren soot (containing 8% fullerenes). For the transition of the group to diamond, it averaged 35.0% of the single culling. 10 Example 4.

They perform the same operations and pressure and the same pressure. time and temperature. and that in case of 1. with the addition of fullerenes C ₆ ο + C ₇ ο in the amount of 0.02 wt.% of the mass of the mixture, introducing it from Φνlle soot (containing 2% Φν). For the transition of group 15 15a to diamond, it averaged 27.2% of the single culling. Example 5.

They also handle the same operation and pressure, at the same time and at the same time. and that in Example 1, with the addition of fullerenes C ₆₀ + C ₀ in the amount of 0.6 wt.% of the mass of the mixture, introducing them from 20 of the extract. For the transfer of the group to diamond, it averaged 22.7% of the total sintering. Example 6.

They also carry out the same operations, and that, for example, 1, but heating is achieved at a temperature of 1350 ° C at a pressure of 5.5 GPa for 90 s. with the addition of Φ л ле ле β β _βη + ₇ η in the amount of 0.15 wt.% of the mass of the mixture, introducing them from the fullerene extract. For the transfer of the group to diamond, it averaged 75.0% of the total sintering. Example 7

They perform the same operations and pressure and the same pressure, at the same time as 30 hours and the temperature. and that in Example 6, with the addition of fullerenes Sat + C ₇₀ in the amount of 0.6 wt.% of the mass of the mixture, entering them from the fullerene extract. For the transition of the group into diamond, it was in the environment 8 it 55.0% from one week. Example 8.

It takes the same operating conditions and pressure at the same time, 5 times and temperature, and that is also in the case of 6. With the addition of fullerenes of + + ₇₀ , the mass is equal to 0.01%. . For the transition of the group to diamond, it averaged 57% of the single sintering. Example 9. 10 The same operations and pressures are the same as the pressure, the time of the discharge and the temperature. and that in Example 1. with the addition of C ₆ ен + C ₇₀ fullerenes in the amount of 0.62 wt.% of the mass of the mixture, entering it from the fullerene extract. For the transition to diamond, it averaged 22.5% of the total sintering. 15 Example 10

The same operations are performed and the pressure is the same, at the same time, and at the same time. and that in Example 6, with the addition of C ₆ + + C ₇₀ fullerenes in the amount of 0.63 wt.% of the mass of the mixture, entering it from the л л ле э extract. For the transition to diamond, it was 20 in the average 42.0% of the total sintering.

How to do it. at the end of the declared period, the content of fullerenes was widened, in the case of the transfer of the charge into the diamond, it is significantly reduced (the level of the charge without the content of fullerenes).

For comparison with the claimed method, 25 genuine diamonds were obtained on the same equipment and on the same basis. and that in parts 1 and 6. but without adding fullerene (parts 11 and 12).

Example 11

We also performed the same operations and pressures at the same time, at the same time 30 times and at the temperature, which, as in Example 1, were processed without adding fullerene. For the transfer of the group to diamond, it averaged 22.6% of the total sintering. 9 Example 12.

They carry out the same operations and pressures at the same pressure, at the same time and at the same time. and that in section 6, but without adding fuller- 5 nov. For the transfer of the group to diamond, it averaged 45.0% of the one sintering.

Deliberate applicability The claimed method of producing artificial diamonds was amended under conditions of industrial use. The incense of προ-10 burst at a temperature of 1350 ° C with a tack of 5.5 GPa and was cured for 25 seconds. 1740 extracts from a shiite containing 0.15% fullerenes were obtained. The share of diamond output was 52.5% on average. Out of shechity. containing 0.225% of fullerenes, 1710 seconds were obtained. The share of diamond output in the average was 15 58.3%. It was also obtained in 1780 sec. Of shiita, containing 0.3% of the percentage. Β The average share of the transfer to diamond amounted to 54.2%.

For pressure at the same pressure, at the same time, 780 seconds were obtained from the lathe. not containing fullerenes. 20 For the transfer of the group into diamond, on average, it amounted to 47.5%.

How to do it. isποlzοvanie zayavlyaemοgο sποsοba ποlucheniya used κussτvennyχ almazοv in uslοviyaχ προmyshlennοgο προizvοdsτva ποzvο- lilο νvelichiτ dοlyu πeρeχοda gρaφiτa in diamond πρi ποnizhennyχ pressures leniyaχ not πρevyshayuschiχ 5.5 Gπa and iτοge ποlνchiτ znachiτelny 25 eκοnοmichesκy eφφeκτ.

ADDITIONAL PARTIES TO PRIMARY DIAMONDS, INCLUDED IN THE PREPARATIONS ABOVE THE EXAMPLE. They were dispersed into 11 fractions and, for some fractions, then measurements of the mechanical size of the diamond crystals were made. 30 The results of these measurements are shown in Table 1. 10

Table 1.

Approx. For Grain, mkm Ν

+315 +250 +200 +160 +125 +100 +80 +63 +50 +40 -40

% Distribution of diamonds for grain production,%

Origin Η

1 33.7 10.5 14.4 12.3 19.8 14.1 19.4 6.4 2.0 1.1

33.6 33.7 37.1 18.2

2 30.3 9.5 17.2 22.8 13.6 16.5 14.7 2.1 3.0 0.6

47.3 43.2 38.2 32.4

3 35.0 1.8 5.9 16.6 10.2 9.1 27.0 12.0 7.9 5.2 4.3

34.4 32.3 27.7 24.6

4 27.2 0.6 2.3 10.6 15.0 14.3 22.2 17.2 11.2 4.1 1.7 0.2

48.7 36.9 37.0 29.7

6 75.0 2.0 2.1 3.3 3.5 8.4 11.712.5 13.116.726.7

8.7 8.5 6.7 6.8

11 22.6 - 7.5 12.2 17.8 11.7 14.1 18.1 7.8 6.1 3.1 1.0

73.3 50.2 45.2 37.4

12 45.0 - 5.8 9.9 13.6 8.4 11.1 10.1 10.7 9.7 6.8 13.9

6.1 7.0 5.9

Claims

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