CN102600768B - Indirect heating-type synthesis assembly for high-temperature and high-pressure artificial single crystal synthesis by using cubic press - Google Patents
Indirect heating-type synthesis assembly for high-temperature and high-pressure artificial single crystal synthesis by using cubic press Download PDFInfo
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Abstract
The invention relates to an indirect heating-type synthesis assembly for single crystal synthesis by using a cubic press. The indirect heating-type synthesis assembly comprises pyrophyllite powder pressing block which is internally lined with a dolomite casing. The indirect heating-type synthesis assembly is characterized in that a cylindrical metal cup made of metal niobium, tantalum, molybdenum or tungsten is arranged in the dolomite casing, an aluminum oxide ceramic high-temperature pipe is wrapped outside the cylindrical metal cup and the aluminum oxide ceramic high-temperature pipe is made of alpha-aluminum oxide and talc through high-temperature sintering; metal conducting strips are respectively arranged on the two sides of the metal cup and are connected with the metal cup; and the two ends of the dolomite casing are respectively sealed by composite conducting plugs and the composite conducting plugs are connected with the metal conducting strips. The indirect heating-type synthesis assembly uses high-melting-point metals to make the metal cup which is also used as an electric heating element, aluminum oxide ceramic materials are additionally used for making the high-temperature protection pipe, the indirect heating-type synthesis assembly is suitable for synthesizing artificial single crystals such as diamonds by using the cubic press, the requirements of higher temperature and longer heating time are satisfied, the stability of single crystal synthesis technology and equipment is improved, the losses of anvils are reduced and favorable conditions are provided for the synthesis of gem grade diamonds.
Description
Technical field
The invention belongs to diamond or the artificial synthesis technical field of other monocrystalline, relate to the synthetic assembling of a kind of monocrystalline, particularly relate to the indirect heating type synthetic assembling (synthetic piece) of the artificial monocrystalline of a kind of cubic hinge press HTHP in synthetic, can, for hexahedron top press high-pressure high temperature diamond synthesis, also can be applied to cubic boron nitride, single-crystal silicon carbide and gallium nitride single crystal growth.
Background technology
Artificial diamond industrial produces, and generally take high purity graphite as raw material, adds catalytic alloy (for example Fe, Ni, Mn, the alloy that Co etc. form), under HTHP, graphite part is converted into diamond.The adamantine synthetic cubic hinge press that conventionally adopts provides crystal growth required HTHP, and current most cubic hinge press diamond synthesis all adopt indirect mode.The heating of synthetic cavity is by tungsten carbide top hammer, to form with cavity heater element the form circuit of connecting with low-voltage and high-current.Take graphite matter tubing or electrothermal alloy as heating element heater indirect graphite synthetic rod.Graphite synthetic rod is wrapped among ferrous metal shell (metal cup), to reduce nonhomogeneous deformation.Between heating element heater and shell, install insulation tube additional, avoid electric current to pass through graphite synthetic rod and ferrous metal shell leakage conductance.Diamond synthesis briquetting used is the pyrophillite powder with waterglass bonding, in the middle of cube briquetting, is cylindrical synthetic chamber, the dolomite insulating tube that liner 3-4mm is thick.Pyrophyllite powder briquetting, insulating tube, heating element heater and conductive plug, insulation tube, metal cup (including synthetic rod) etc. are combined into the synthetic assembling of diamond (or synthetic piece), be placed in cubic apparatus synthesis press, by synthetic technological condition, pressure and temperature is raised to desirable value, after crystal growth certain hour, obtains artificially synthesizing diamond.
For example, ZL201020686676 discloses a kind of indirect heating device for diamond synthesis, comprise pyrophyllite composite block, conductive plug is installed respectively at the upper and lower two ends of pyrophyllite composite block, stem stem is installed in the centre of pyrophyllite composite block, stem stem periphery is installed metal cup, metal cup upper and lower surfaces are installing insulating sheet respectively, metal cup two sides are installing insulating pipe respectively, metal electric heating tube is installed respectively in insulation tube outer wall two sides, insulating trip is connected with sheet metal respectively, and sheet metal is connected with termination heating plate.CN200610017366.5 discloses a kind of outer indirect heating diamond synthesis block, comprise diamond synthesizing column, synthetic post two ends are provided with composite conducting heat-proof device, synthetic post and composite conducting heat-proof device outside are arranged with hermetical and pressure madium, are certainly disposed with outside to inside heater element, heat transfer element and isolated component between hermetical and pressure madium and composite conducting heat-proof device and synthetic post.Composite conducting heat-proof device comprises the metallic cylinder that conducting metal disk and one end join with it and diameter is less, closely embeds prefabricated insulation material cylinder in cylinder, and cylinder periphery is closely arranged with prefabricated thermal insulation material cylinder.
In the synthetic assembling that at present diamond is produced, metal cup (isolated component) arranges respectively with heating element heater, between install insulation tube additional; High-temperature insulation and insulation material adopt dolomite to make.The problem existing is: during (1) long-time heating, pyrophyllite powder briquetting (hermetical and pressure madium) temperature raises, easy quick-fried hammer.The temperature of synthetic chamber and heater element surpasses 1450 ℃, and adiabatic poor between pyrophyllite powder briquetting and heater element, long-time heating makes the rising of pyrophyllite powder briquetting temperature, and temperature causes that material generation volume changes suddenly during higher than phase transition temperature, thereby causes quick-fried hammer.(2) the easy quick-fried hammer of gas excretion producing when the high-temperature insulation that dolomite is made and insulation material high temperature.The water glass of binder that dolomite insulation and insulating tube add while making forms silica dioxide gel and does not fully react with dolomite, and at high temperature both react and produce water and carbon dioxide.Although pyrophillite is sheet crystal structure (being different from metal), allow part micro-molecular gas to overflow along inter-level diffusion, top hammer can safety relief.But the thickness of insulating tube used and insulation tube and size strengthen, the gas flow producing during heating increases, and has improved the risk of quick-fried hammer.(3) heater element poor stability when long-time heating: the indirect heater element generally using is at present cool molded graphite pipe or electrothermal alloy.Under high pressure deformation quantity is larger for the former, and poor stability, the process repeatability of resistance value are poor.The latter is irony alloy (the mixture 0.5-2 % of one or more in iron content 65-80%, chromium 13-27%, aluminium 4-7%, niobium, tantalum, molybdenum three), and fusing point is relatively low, is difficult to bear higher heating-up temperature.In addition, the reproducibility of iron, aluminium is strong, easily at high temperature oxidized, reacts with acidic oxide or the oxide that contains dithizone.And then resistance value changes.(4) the rear and front end temperature difference of top hammer becomes large during long-time heating, and swelling stress easily causes quick-fried hammer.
Aspect equipment, along with the technology innovation of China's diamond synthesis device, most enterprises has been eliminated old-fashioned supercharger systems, and adopts more efficiently high-pressure pump to carry out supercharging.Broken the generated time restriction that supercharger systems causes because oil cylinder piston stroke is limited, with high-pressure pump, carrying out supercharging can be without time limit pressurize.Therefore, improve the synthetic assembling of indirect heating type in cubic hinge press, improve the stability of the synthesis techniques such as diamond and equipment, meet the desired higher synthesis temperature of technique, extend the heat time, reduce top hammer loss, for the synthetic advantage that provides of gem grade diamond, significant for diamond industrial upgrading.
Summary of the invention
The present invention aims to provide the indirect heating type synthetic assembling of the artificial monocrystalline of a kind of cubic hinge press HTHP in synthetic, can overcome existing above-mentioned defect in prior art, improve the stability of the synthesis techniques such as diamond and equipment, meet higher synthesis temperature and extend the heat time, reduce top hammer loss, improve the quality of diamond synthesis, and then realize the synthetic of gem grade diamond.
In brief; the present invention makes metal cup and doubles as heating with refractory metal (niobium, tantalum, molybdenum, tungsten); additional alumina ceramic material is made high temperature protection pipe; with it, be assembled into the synthetic assembling of indirect stone (piece), be applicable to hexahedron synthetic diamond press high pressure-temperature synthetic gem grade diamond.This assembling also can be applied to cubic boron nitride, single-crystal silicon carbide and gallium nitride single crystal growth.
For achieving the above object, the present invention adopts following technical scheme:
The synthetic assembling of indirect heating type during the artificial monocrystalline of a kind of cubic hinge press HTHP is synthetic, comprise pyrophyllite powder briquetting (1), liner dolomite sleeve pipe (2), in dolomite sleeve pipe (2), it is cylindrical synthetic chamber, it is characterized in that, in dolomite sleeve pipe (2), comprise the cylindric metal cup (7) made from metal niobium, tantalum, molybdenum or tungsten, cylinder outer wrapping aluminium oxide ceramics high-temperature pipe (3), it is aggregate that described aluminium oxide ceramics high-temperature pipe (3) be take а-aluminium oxide and the talcum of mass percent 75～90%:10～25%, through 850-1200 ℃ of sintering, makes; Described metal cup (7) both sides arrange respectively metallic conduction sheet (5) and are connected with metal cup (7); Dolomite sleeve pipe (2) two ends are respectively by composite conducting plug (4) sealing, and composite conducting plug (4) is connected with metallic conduction sheet (5).
Described metal cup is by refractory metal, as niobium, tantalum, molybdenum, tungsten sheet metal are made by Sheet Metal Forming Technology or welding procedure.Metal cup can adopt the cup of one end sealing to add the form of metal bowl cover, or the form that the cup openend of two single-ended sealings fastens forms, its size can be determined according to the synthetic chamber of cubic hinge press size, be generally wall thickness 0.1-0.3mm, diameter 10-50mm, height 10-50mm.Synthetic assembling of the present invention, the synthetic stem stem of diamond (or other monocrystalline) is filled in metal cup, and while metal cup also doubles as heating, and the aluminium oxide ceramics high-temperature pipe of cup outer wrapping can be effectively by heating and the isolation of pyrophyllite powder briquetting.
Described aluminium oxide ceramics high-temperature pipe wall thickness is 3-8mm, and internal diameter and metal cup external diameter match, and height is identical with metal cup; External diameter and synthetic chamber diameter (dolomite casing inner diameter) match.
Described aluminium oxide ceramics high-temperature pipe adopts following methods preparation: according to mass percent а-aluminium oxide: talcum=75～90%:10～25% preparation aggregate, the binding agent polyvinyl alcohol that adds aggregate quality 1～4%, by wet ball grinding technique, make slurry, slurry mist projection granulating makes ceramic powder; Again that ceramic powder is compressing, 850-1200 ℃ of sintering, makes described ceramic high temperature pipe.
Described metallic conduction sheet is the disk that diameter is identical with aluminium oxide ceramics high-temperature pipe external diameter, adopts refractory metal, comprises metal niobium, tantalum, molybdenum or tungsten.
Described composite conducting plug comprises cylindrical conductive shell, or adopts low-carbon steel material punch forming, thickness to be >=3mm, external diameter identical with aluminium oxide ceramics high-temperature pipe external diameter (matching with the synthetic cavity diameter of briquetting).Described external conductive casing is connected with metallic conduction sheet conduction.In external conductive casing, fill heat Insulation film (energising end protection pad); preferably fill the heat Insulation film of two stacks; one piece material is identical with aluminium oxide ceramics high-temperature pipe; adopt the ceramic powder in above-mentioned aluminium oxide ceramics high-temperature pipe preparation; repressed moulding; the 850-1200 ℃ of aluminium oxide ceramics disk that sintering forms, another sheet is dolomite disk.Described aluminium oxide ceramics disk is thick is 3-8mm, diameter >=metal cup external diameter, and contact with metallic conduction sheet.
The synthetic assembling of indirect heating type of the present invention can be prepared by the following method:
(1) with niobium, tantalum, molybdenum, tungsten sheet metal, by Sheet Metal Forming Technology or welding procedure, be made into the metal cup (heater element) of wall thickness 0.1-0.3mm, diameter 10-50mm, height 10-50mm.
(2) take aluminium oxide and talcum (mass percent is 75～90%:10～25%) is aggregate; through high temperature 850-1200 ℃ of sintering, making wall thickness is 3-8mm; internal diameter and metal cup external diameter coupling, length identical with metal cup aluminium oxide ceramics high-temperature pipe (protective casing).
(3) take aluminium oxide and talcum (mass percent is 75～90%:10～25%), by the identical method of step (2), making thick be 3-8mm, the aluminium oxide ceramics heat Insulation film that diameter mate with composite conducting plug (switch on to holding and protect pad).
(4) adopt low-carbon steel material punch forming to make the external conductive casing of composite conducting plug, thickness is >=3mm that the cavity diameter of external profile diameter and briquetting matches.In external conductive casing, fill successively dolomite heat Insulation film and aluminium oxide ceramics heat Insulation film.
(5) in metal cup, fill synthetic stem stem, be assembled into synthetic assembling.
Above-mentioned synthetic assembling can be used for the artificial monocrystalline such as diamond in cubic hinge press HTHP is synthetic.
Beneficial effect of the present invention: the present invention makes metal cup and doubles as heating with refractory metal (niobium, tantalum, molybdenum, tungsten); additional alumina ceramic material is made high temperature protection pipe; with it, be assembled into the synthetic assembling of indirect (piece), be applicable to the artificial monocrystalline such as hexahedron top press high-pressure high temperature diamond synthesis.Synthetic assembling of the present invention can improve the stability of synthesis technique and equipment in the cubic hinge press such as diamond, meets the desired higher temperature of technique and longer heat time, reduces top hammer loss, is the synthetic advantage that provides of gem grade diamond.Beneficial effect of the present invention comprises:
(1) fusing point of the metal such as niobium, tantalum, molybdenum, tungsten is high, and the metal cup made from refractory metal doubles as heater element, and the heating-up temperature that can bear significantly improves; And the good stability of long-time heating.
(2) metal cup doubles as heater element, can reduce the use of high temperature insulating material, and the aluminium oxide ceramics high-temperature pipe of cup outer wrapping can, effectively by heating (metal cup) and the isolation of pyrophyllite powder briquetting, reduce quick-fried hammer risk.
(3) adopt the corundum of high temperatures to make earthenware, and it is carried out to high annealing, avoided the air release of material in monocrystalline building-up process.The high-temperature insulating quality of the alumina ceramic tube made from а-aluminium oxide and talcum and aluminium oxide ceramics heat Insulation film (energising end pad) is good, does not at high temperature undergo phase transition, and cubical expansivity changes little, the pressurize good stability of cavity.In addition, this ceramic material has during higher than 1450 ℃ a small amount of liquid phase to produce in temperature, be conducive to pressure transmission, and the pressure uniformity in cavity is good, thereby can improve the distributing homogeneity of single crystal grain in synthetic stem stem and the concentration degree of a footpath distribution.
(4) the alumina ceramic material density making by sintering is larger, and intensity is high, is difficult for fragmentation, is conducive to the assembling of synthetic assembling; Metal cup and heating element heater unite two into one, and make the structure of the synthetic assembling of indirect of the present invention compacter, and the transport performance of assembled product improves, and has reduced breakage rate.
Below in conjunction with specific embodiment, describe the present invention.Protection scope of the present invention is not limited with the specific embodiment, but is limited by claim.
Accompanying drawing explanation
The structural representation of the synthetic assembling of Fig. 1 indirect heating type of the present invention.
1, pyrophyllite powder briquetting, 2, dolomite sleeve pipe, 3, aluminium oxide ceramics high-temperature pipe, 4, composite conducting plug, 5, metallic conduction sheet, 6, synthetic stem stem, 7, metal cup (heater element of holding concurrently).
The specific embodiment
Below in conjunction with specific embodiment, describe the present invention.Protection scope of the present invention is not limited with the specific embodiment, but is limited by claim.
The synthetic assembling of indirect heating type during the artificial monocrystalline of cubic hinge press HTHP of the present invention is synthetic, equally applicable to synthetic other the artificial monocrystalline of cubic hinge press HTHP, as cubic boron nitride, single-crystal silicon carbide and gallium nitride single crystal etc., below in conjunction with accompanying drawing, so that diamond is synthetic, is assembled into example and is described in detail.
According to the synthetic assembling of cubic hinge press indirect heating type diamond of the present invention, referring to Fig. 1, comprise pyrophyllite powder briquetting 1, dolomite sleeve pipe 2, aluminium oxide ceramics high-temperature pipe 3, composite conducting plug 4, metallic conduction sheet 5, metal cup (heater element of holding concurrently) 7.Pyrophyllite powder briquetting 1 liner dolomite sleeve pipe 2, in dolomite sleeve pipe 2, it is cylindrical synthetic chamber, the synthetic stem stem 6 of diamond is placed in synthetic chamber, synthetic stem stem 6 is filled in metal cup 7, and certainly synthetic stem stem 6 is respectively metal cup 7, aluminium oxide ceramics high-temperature pipe 3, dolomite sleeve pipe 2 and pyrophyllite powder briquetting 1 from inside to outside.
Metal cup 7 is by aluminium oxide ceramics high-temperature pipe 3 parcels, and height is identical with metal cup 7; Both sides arrange respectively metallic conduction sheet 5.Metallic conduction sheet 5 one sides are connected with metal cup 7, and opposite side is connected with composite conducting plug 4.Aluminium oxide ceramics high-temperature pipe 3 external diameters, metallic conduction sheet 5 diameters are identical with composite conducting plug 4 external diameters, and match with dolomite sleeve pipe 2 internal diameters, and dolomite sleeve pipe 2 both sides are respectively by 4 sealings of composite conducting plug.
Metal cup 7 is made with metal niobium, tantalum, molybdenum or tungsten, and it is aggregate that aluminium oxide ceramics high-temperature pipe 3 be take а-aluminium oxide and the talcum of mass percent 75～90%:10～25%, through 850-1200 ℃ of sintering, makes.Metallic conduction sheet 5 adopts metal niobium, tantalum, molybdenum or tungsten material, and composite conducting plug 4 comprises hollow cylindrical mild steel external conductive casing, and external conductive casing is filled dolomite heat Insulation film and aluminium oxide ceramics heat Insulation film from inside to outside successively.
Above-mentioned its manufacturing process of synthetic assembling comprises the steps:
(1) the refractory metal cup 7(heating of holding concurrently) make
By metallic plate punchings such as niobium, tantalum, molybdenum, tungsten or to be welded into thickness be 0.1-0.3mm, the cup-shaped heater element of diameter 10-50mm, height 10-50mm.
(2) aluminium oxide ceramics dry powder preparation
By а-aluminium oxide and the talcum powder preferred 85%:15% of 75～90%:10～25%(by mass percentage) mix, be loaded in ball grinder, take water as medium, with corundum ball, be ground into particle diameter and be less than 200 object slurries, again by aluminium oxide and talcum powder quality 1～4%(preferably 3%) add polyvinyl alcohol (PVA molecular weight >=10000, polyvinyl alcohol water solution concentration is 5-10%), with atomizing granulating technology, be prepared into the powder ball of particle diameter 0.3-0.7mm.
(3) aluminium oxide ceramics high-temperature pipe 3 is made
It is 3-8mm that the repressed moulding of ceramic powder, the high temperature sintering of preparation in step (2) are made to wall thickness, the protective casing of internal diameter and length and above-mentioned cup-shaped heater element external diameter and matched.Ceramic powder is pressed into required tubular blank with wolfram steel mould, tubular blank is embedded in coarse granule alumina powder, in 850-1200 ℃ of sintering 1-3 hour, (preferably 3.5 ℃/min was warmed up to 550 ℃ of insulations and comes unstuck for 1 hour; With 5 ℃/min, be warmed up to 1000 ℃ again sintering 1 hour) become aluminium oxide ceramics high-temperature pipe.The shrinkage factor of pottery in sintering process is 5-8%, and therefore, the design of mould should be done corresponding size by actual shrinkage factor and amplify.By tubular blank landfill sintering in alumina powder, buried powder has limited earthenware in sintering process and, along diametric contraction deformation, has guaranteed diameter uniformity and the caliber size of pipe on the one hand; On the other hand, high temperature sintering has been removed volatile material (as the hydroxyl in raw material, moisture and binding agent), has avoided prepared high-temperature pipe to produce gas under the high pressure-temperature condition of diamond synthesis; The 3rd, by sintering process, the density of earthenware is larger, and intensity is high, is difficult for broken.
(4) composite conducting plug 4 is made
The external conductive casing of composite conducting plug plug is low-carbon steel material punch forming, and thickness is at least 3mm, and the cavity diameter of external profile diameter and briquetting matches.In external conductive casing, fill two heat Insulation films, a powder aluminium oxide ceramics disk dry-pressing formed and that form in 850-1200 ℃ of (preferably 1000 ℃) sintering 1-3 hour for making in above-mentioned steps (2).Another piece is dolomite disk.Its common manufacture craft of dolomite disk is: the mass percent of dolomite powder (particle diameter 100-300 order), waterglass (modulus 2.3) and polyvinyl alcohol (molecular weight is greater than 10000) is that to be mixed with in use concentration be 5% aqueous solution to 84%:13%:3%(polyvinyl alcohol), above-mentioned material is stirred in agitator, with dry pressuring forming process, be pressed into disk, then in 450 ℃ of heating 1-2 hour.Dolomite heat Insulation film and aluminium oxide ceramics heat Insulation film are filled in external conductive casing successively, make composite conducting plug.
(5) pyrophyllite powder briquetting 1, dolomite sleeve pipe 2, aluminium oxide ceramics high-temperature pipe 3, metal cup 7(are included to synthetic stem stem 6), metallic conduction sheet 5, composite conducting plug 4 be assembled into synthetic assembling, becomes that indirect heating type is synthetic to be assembled by said structure assembling (as Fig. 1).
When described synthetic assembling synthesizing for gem grade diamond, the interior material filling mode of metal cup (heating of holding concurrently) is: the gem grade diamond micro mist and the chip catalyst that particle diameter are less than to 50 microns are loaded in metal cup with overlapped way, densified under 200-400MPa pressure, be then assembled into synthetic assembling.
Synthetic assembling after assembling can be used for the synthetic of gem grade diamond: the synthetic assembling by after assembling, be positioned in cubic apparatus synthesis press, and follow procedure is raised to desirable value by pressure and temperature, keeps 10-240 hour.Gained synthetic rod gets final product to obtain product through electrolysis, fragmentation, screening.
Embodiment 1
Synthetic assembling in the hexahedron synthetic diamond press of cavity diameter 23mm, comprising:
Pyrophyllite powder briquetting, size 38mm
3; Liner dolomite sleeve pipe, centre is the cylindrical synthetic chamber of diameter 23mm
Aluminium oxide ceramics high temperature protection pipe: wall thickness 5mm, outer through 23mm, interior through 13mm, height 11.6 mm
Metal cup: metal molybdenum, wall thickness 0.2mm, outer through 13mm, height 11.6mm
Refractory metal conducting strip: metal molybdenum, thickness 0.2mm, diameter 23mm
Composite conducting plug: box hat: thickness 3mm, outer through 23mm, height 13mm
In box hat, fill: aluminium oxide ceramics disk, diameter 17mm, thickness 5mm
Dolomite disk: diameter 17mm, thickness 5mm
Be assembled into synthetic assembling, in metal cup, fill synthetic stem stem.
Synthetic assembling is positioned in cubic hinge press, and follow procedure is raised to pressure and temperature desirable value and is retained to generated time.Gained synthetic rod gets final product to obtain product through electrolysis, fragmentation, screening.
Synthesis condition: 1450 ℃ of temperature; Pressure 52000 atmospheric pressure (with bismuth silk phase transformation estimation); Generated time 55 hours.
Synthetic stem stem: use raw material is W14 diadust 2.8g, 4 of iron-nickel accelerant sheets; By overlapped way, load in metal cup, densified under 200-400MPa pressure.
Products obtained therefrom: 1.61 grams of the above diamond single crystals of diameter 1mm, the largest particles diameter 2.8mm.
Embodiment 2
Synthetic assembling in the hexahedron synthetic diamond press of cavity diameter 23mm, comprising:
Pyrophyllite powder briquetting, size 38mm
3; Liner dolomite sleeve pipe, centre is the cylindrical synthetic chamber of diameter 23mm
Aluminium oxide ceramics high temperature protection pipe: wall thickness 5mm, outer through 23mm, interior through 13mm, height 11.6 mm
Metal cup: metal molybdenum, wall thickness 0.2mm, outer through 13mm, height 11.6mm
Refractory metal conducting strip: metal molybdenum, thickness 0.2mm, diameter 23mm
Composite conducting plug: box hat: thickness 3mm, outer through 23mm, height 13mm
In box hat, fill: aluminium oxide ceramics disk: diameter 17mm, thickness 5mm
Dolomite disk: diameter 17mm, thickness 5mm
Be assembled into synthetic assembling, in metal cup, fill synthetic stem stem.
Synthetic assembling is positioned in cubic hinge press, and follow procedure is raised to pressure and temperature desirable value and is retained to generated time.Gained synthetic rod gets final product to obtain product through electrolysis, fragmentation, screening.
Synthesis condition: 1450 ℃ of temperature; Pressure 52000 atmospheric pressure (with bismuth silk phase transformation estimation); Generated time 76 hours.
Synthetic stem stem: use raw material is W14 diadust 2.8g, 4 of iron-nickel accelerant sheets; By overlapped way, load in metal cup, densified under 200-400MPa pressure.
Products obtained therefrom: 1.79 grams of the above diamond single crystals of diameter 1mm, the largest particles diameter 3.0mm.
Embodiment 3
Synthetic assembling is identical with embodiment 1, extends generated time to 96 hour.
Synthesis condition: 1450 ℃ of temperature; Pressure 52000 atmospheric pressure (with bismuth silk phase transformation estimation); Generated time 96 hours.
Synthetic stem stem: use raw material is W14 diadust 2.8g, 4 of iron-nickel accelerant sheets; By overlapped way, load in metal cup, densified under 200-400MPa pressure.
Products obtained therefrom: the above diamond single crystal of diameter 1mm: 1.91 grams, the largest particles diameter 3.2mm.
Embodiment 4
Synthetic assembling in the hexahedron synthetic diamond press of cavity diameter 23mm, comprising:
Briquetting size: 38mm
3; Liner dolomite sleeve pipe, centre is the cylindrical synthetic chamber of diameter 23mm
Aluminium oxide ceramics high temperature protection pipe: wall thickness 5mm, outer through 23mm, interior through 13mm, height 11.6 mm
Metal cup: metal tantalum, wall thickness 0.2mm, outer through 13mm, height 11.6mm
Refractory metal conducting strip: metal tantalum, thickness 0.2mm, diameter 23mm
Composite conducting plug: box hat: thickness 3mm, outer through 23mm, height 13mm
In box hat, fill: aluminium oxide ceramics disk, diameter 17mm, thickness 5mm
Dolomite disk: diameter 17mm, thickness 5mm.
Synthesis condition is identical with embodiment 1, products obtained therefrom: 1.62 grams of the above diamond single crystals of diameter 1mm, the largest particles diameter 2.8mm.The electrolytic treatments speed of synthetic piece is very slow, needs electrolysis of fluorides matter to do electrolyte.
Embodiment 5
Substantially the same manner as Example 4, metal cup and metallic conduction sheet adopt niobium.Because metal niobium is relatively soft, the easy moulding of metal cup.
Synthesis condition is identical with embodiment 1, products obtained therefrom: 1.60 grams of the above diamond single crystals of diameter 1mm, the largest particles diameter 2.8mm.Metal tube present situation remains intact, and deformation is even, the electrolytic treatments speed of synthetic piece.
Embodiment 6
Substantially the same manner as Example 4, metal cup and metallic conduction sheet adopt tungsten.Because tungsten hardness is large, metal cup can not be used punch forming.Adopt argon arc welding technique to make metal cup.
In synthesis condition, except temperature is 1700 ℃, other condition is identical with embodiment 1, products obtained therefrom: 1.80 grams of the above diamond single crystals of diameter 1mm, the largest particles diameter 3.0 mm.Metal tube present situation remains intact, and deformation is even, the electrolytic treatments speed of synthetic piece.Electrolyte is favourable to improving electrolytic speed containing organic acid.
Claims (6)
1. the artificial monocrystalline of the cubic hinge press HTHP synthetic assembling of indirect heating type in synthetic, comprise pyrophyllite powder briquetting (1), liner dolomite sleeve pipe (2), in dolomite sleeve pipe (2), it is cylindrical synthetic chamber, it is characterized in that, dolomite sleeve pipe comprises with metal niobium in (2), tantalum, the cylindric metal cup (7) that molybdenum or tungsten are made, cylindric metal cup (7) outer wrapping aluminium oxide ceramics high-temperature pipe (3), it is aggregate that described aluminium oxide ceramics high-temperature pipe (3) be take а-aluminium oxide and the talcum of mass percent 75～90%:10～25%, through 850-1200 ℃ of sintering, make, described metal cup (7) both sides arrange respectively metallic conduction sheet (5) and are connected with metal cup (7), dolomite sleeve pipe (2) two ends are respectively by composite conducting plug (4) sealing, and composite conducting plug (4) is connected with metallic conduction sheet (5).
2. the synthetic assembling of indirect heating type according to claim 1, is characterized in that, described aluminium oxide ceramics high-temperature pipe (3) wall thickness is 3-8mm, and internal diameter and metal cup (7) external diameter matches, and height is identical with metal cup (7); External diameter and dolomite sleeve pipe (2) internal diameter match.
3. the synthetic assembling of indirect heating type according to claim 1, it is characterized in that, described aluminium oxide ceramics high-temperature pipe (3) adopts following methods preparation: according to mass percent а-aluminium oxide: talcum=75～90%:10～25% preparation aggregate, the binding agent polyvinyl alcohol that adds aggregate quality 1～4%, by wet ball grinding technique, make slurry, slurry mist projection granulating makes ceramic powder; Again that ceramic powder is compressing, 850-1200 ℃ of sintering, makes described ceramic high temperature pipe.
4. the synthetic assembling of indirect heating type according to claim 1, is characterized in that, described metallic conduction sheet (5) adopts metal niobium, tantalum, molybdenum or tungsten, is the diameter disk identical with aluminium oxide ceramics high-temperature pipe (3) external diameter.
5. the synthetic assembling of indirect heating type according to claim 1, it is characterized in that, described composite conducting plug (4) comprises cylindrical conductive shell, thickness >=3mm, external diameter is identical with aluminium oxide ceramics high-temperature pipe (3) external diameter, fills heat Insulation film in external conductive casing; External conductive casing is connected with metallic conduction sheet (5) conduction.
6. the synthetic assembling of indirect heating type according to claim 5, it is characterized in that, described heat Insulation film is the heat Insulation film of two stacks, a slice is aggregate for take а-aluminium oxide and the talcum of mass percent 75～90%:10～25%, the 850-1200 ℃ of aluminium oxide ceramics disk that sintering forms, another sheet is dolomite disk, wherein aluminium oxide ceramics disk is thick is 3-8mm, diameter >=metal cup (7) external diameter, and contact with metallic conduction sheet (5).
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| CN201210087887.3A CN102600768B (en) | 2012-03-30 | 2012-03-30 | Indirect heating-type synthesis assembly for high-temperature and high-pressure artificial single crystal synthesis by using cubic press |
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| CN201210087887.3A CN102600768B (en) | 2012-03-30 | 2012-03-30 | Indirect heating-type synthesis assembly for high-temperature and high-pressure artificial single crystal synthesis by using cubic press |
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| CN102600768B true CN102600768B (en) | 2014-03-05 |
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| CN201210087887.3A Expired - Fee Related CN102600768B (en) | 2012-03-30 | 2012-03-30 | Indirect heating-type synthesis assembly for high-temperature and high-pressure artificial single crystal synthesis by using cubic press |
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| CN103585930B (en) * | 2013-11-27 | 2015-09-23 | 南通国谊锻压机床有限公司 | A kind of tungsten alloy top hammer automatic molding process and device thereof |
| CN108940125A (en) * | 2018-06-13 | 2018-12-07 | 燕山大学 | It is a kind of to prepare Al13Fe3The method of single crystal grain |
| CN111659318B (en) * | 2020-06-15 | 2023-10-27 | 山东聊城君锐超硬材料有限公司 | Assembled block for high-temperature high-pressure modification of CVD cultivated diamond and modification method |
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| JPH06165929A (en) * | 1992-11-30 | 1994-06-14 | Sumitomo Electric Ind Ltd | Method for synthesizing diamond single crystal |
| ES2258919B2 (en) * | 2005-02-21 | 2007-04-01 | Instituto De Monocristales, S.L. | CAPSULE AND ELEMENTS FOR THE PRODUCTION OF DIAMOND SYNTHESIS. |
| CN101007251A (en) * | 2006-01-23 | 2007-08-01 | 郑州人造金刚石及制品工程技术研究中心 | Outer indirect heating diamond synthesis block |
| CN101279223B (en) * | 2008-05-05 | 2010-11-17 | 江苏工业学院 | Use of electrothermal alloy in six-side top high-temperature high-pressure synthetic cavity |
| US8021639B1 (en) * | 2010-09-17 | 2011-09-20 | Diamond Materials Inc. | Method for rapidly synthesizing monolithic polycrystalline diamond articles |
| CN201906593U (en) * | 2010-12-29 | 2011-07-27 | 山东聊城昌润超硬材料有限公司 | Indirect heating device for diamond synthesis |
| CN202052523U (en) * | 2011-05-11 | 2011-11-30 | 晶日金刚石工业有限公司 | Energy-saving diamond synthesis assembly block |
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