WO1999019058A1 - Matrice synthetique a haute pression - Google Patents

Matrice synthetique a haute pression Download PDF

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Publication number
WO1999019058A1
WO1999019058A1 PCT/CN1998/000245 CN9800245W WO9919058A1 WO 1999019058 A1 WO1999019058 A1 WO 1999019058A1 CN 9800245 W CN9800245 W CN 9800245W WO 9919058 A1 WO9919058 A1 WO 9919058A1
Authority
WO
WIPO (PCT)
Prior art keywords
mold
pressure
medium
cavity
temperature
Prior art date
Application number
PCT/CN1998/000245
Other languages
English (en)
Chinese (zh)
Inventor
Weiping Wang
Original Assignee
Weiping Wang
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 Weiping Wang filed Critical Weiping Wang
Priority to AU95284/98A priority Critical patent/AU9528498A/en
Publication of WO1999019058A1 publication Critical patent/WO1999019058A1/fr

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Classifications

    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B30—PRESSES
    • B30B—PRESSES IN GENERAL
    • B30B11/00—Presses specially adapted for forming shaped articles from material in particulate or plastic state, e.g. briquetting presses, tabletting presses
    • B30B11/004—Presses specially adapted for forming shaped articles from material in particulate or plastic state, e.g. briquetting presses, tabletting presses involving the use of very high pressures
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J3/00—Processes of utilising sub-atmospheric or super-atmospheric pressure to effect chemical or physical change of matter; Apparatus therefor
    • B01J3/06—Processes using ultra-high pressure, e.g. for the formation of diamonds; Apparatus therefor, e.g. moulds or dies
    • B01J3/065—Presses for the formation of diamonds or boronitrides
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J2203/00—Processes utilising sub- or super atmospheric pressure
    • B01J2203/06—High pressure synthesis
    • B01J2203/065—Composition of the material produced
    • B01J2203/0655—Diamond

Definitions

  • the invention relates to a high-pressure chemical synthesis mold, which is suitable for manufacturing diamonds and other chemical substances that need to be prepared by using high-pressure bar.
  • graphite is transformed into diamond under the action of a catalyst for 3 to 5 minutes at a high temperature of 1500 to 1800K and a high pressure of 50,000 to 100,000 atm.
  • the catalyst and high temperature of 1500_1800K are relatively easy to achieve in the reaction.
  • the key to the reaction is high pressure.
  • the yield of diamond production is also directly related to the pressure. The higher the pressure, the higher the diamond yield.
  • the pressure required for industrial production of diamond is usually achieved by hard pressing machinery such as six-sided top, four-sided top, and two-sided top, and the die is mechanically pressed.
  • the mechanical hard pressing method is to directly squeeze the solid reactant with a mold.
  • the pressure achieved by this method has a large compressive stress due to the poor pressure transmission performance of the solid material, which poses a greater threat to the mold material and the pressure is not easy to reach.
  • the purpose of the present invention is to invent a thermal variable high pressure synthetic mold which can effectively reduce the decompression stress and thereby achieve a higher pressure, so as to produce high-quality diamond with high efficiency.
  • the solution of the present invention is as follows: It includes a press, a high-pressure mold, and the like.
  • the mold adopts a leak-proof close-fitting structure. After the mold is closed under pressure, a closed high-pressure chemical synthesis mold cavity is formed. The reason is that it fills and uses a pressure-varying medium in its high-pressure chemical synthesis mold cavity. Because the above technical scheme is adopted, compared with the existing technology, the present invention has the advantages of substantially reducing the mold compressive stress, thereby achieving higher pressure, more complete reaction, high product quality, large output, low cost, and the like.
  • FIG. 1 is a schematic structural diagram of Embodiment 1 of the present invention.
  • Fig. 2 is the pressure-volume of the pressure-varying medium in the cavity of the first embodiment shown in Fig. 1
  • -Temperature state change diagram that is, the P-V-T phase diagram of the medium, where P represents the pressure of the medium, V represents the volume of the medium, and T represents the temperature of the medium.
  • FIG. 3 is a schematic diagram of adding a pressure-variable medium in the half-clamped state of the mold in the first embodiment shown in FIG. 1.
  • FIG. 3 is a schematic diagram of adding a pressure-variable medium in the half-clamped state of the mold in the first embodiment shown in FIG. 1.
  • Fig. 4 is a schematic diagram of cooling of the composite column and recovery of the pressure-storing medium in the half-open state of the mold of the first embodiment shown in Fig. 1.
  • FIG. 3 and FIG. 4 are schematic diagrams of two other working states of the embodiment 1 shown in FIG. 1.
  • the names and meanings of the reference numerals in FIGS. 3 and 4 are the same as those in FIG.
  • the present invention includes:
  • the high-voltage mold MO is composed of an upper mold 2 and a lower mold 5.
  • the lower mold 5 is composed of a high-pressure-resistant metal outer cylinder 13, a high-temperature-resistant insulation inner cylinder 4, and a metal gland 3.
  • the lower mold structure here is a simplified model for the sake of simplicity. In practice, the lower mold is usually composed of multiple layers of high-strength materials and the structure is more complicated.
  • the synthesis column 7 is a piston type with a reactant inside. Sealed container,
  • the mold adopts a single-face top-type upper and lower mold structure.
  • the reason why the single-face top is used instead of the two-face top is because the single-face top structure is easier to achieve sealing.
  • the upper and lower molds are closely fitted. After the mold is closed, there is a filler 10 that is resistant to high temperature and pressure on the peripheral wall step between the head of the upper mold 2 and the inner cylinder 4 of the lower mold, as shown in a partially enlarged view A. Form a leak-proof tight fit structure.
  • the high-pressure mold MO is under the action of the strong pressure F of the pressure head 1 of the press M, and the upper and lower molds are tightly closed and closed to form a high-pressure chemical synthesis mold cavity 0.
  • the cavity Q is filled and used with a pressure varying medium 9, which is an inert fluid substance resistant to synthetic high pressure (here, "inertness” mainly refers to the chemical inertness of the mold material under synthetic high pressure, the same applies hereinafter).
  • a pressure varying medium 9 which is an inert fluid substance resistant to synthetic high pressure (here, "inertness” mainly refers to the chemical inertness of the mold material under synthetic high pressure, the same applies hereinafter).
  • it is usually a chemically inert substance that has a pressure that increases rapidly with increasing temperature in a static closed container (depending on the chemical composition and properties of the mold material, from carbon diamine (C0 2 ), inert gas (Ar gas, etc.), alkane compounds and other materials), this kind of materials in the present invention is called the first type of pressure swing medium-heat pressure swing medium.
  • the synthesis column 7 contains the reactants and is sealed and installed in the special "L" shaped slot on the head of the upper mold 2. It can move up and down with the upper mold 2. It can be removed and replaced after the mold is opened, which can achieve high efficiency. Continuous operation.
  • the surface of the head part of the upper mold 2 is covered with a heat insulation material 12 for heat insulation.
  • the cavity Q is provided with a heating resistor 6 connected to the wires c and d, a temperature-controlled thermocouple 8 connected to the wires a and b, and a composite column 7 connected to the wires e and f.
  • These wires are resistant to high temperatures, except that the wire f is
  • the other parts are sintered and planted on the bottom side of the inner cylinder 4 of the lower mold, which is laid out in a wavy or spiral shape to resist the high pressure of the cavity and lead out from the bottom side of the inner cylinder 4. After closing the mold, it is connected.
  • P 3 is the pressure of the medium 9 after the reaction is completed.
  • P 3 can also be controlled within the pressure range required for the reaction, so that the reaction can be carried out more thoroughly (to save space, synthesis
  • the temperature control structure of column 7 is not shown and explained for the time being).
  • a pressure measurement element can be added in the mold cavity (to save space, it is not shown and explained for the time being).
  • the wall of the synthesis column 7 can also be made of an insulating material with good heat insulation properties, so that only the reactants in the synthesis column 7 can be controlled to be heated to the reaction temperature, and the temperature of the medium can be changed with The pressure or the protection of the cavity material needs to be adjusted up and down, which will be easier to control.
  • the press head 1 and the upper die 2 of the high-pressure die should be raised as soon as possible to the half-open state shown in FIG. Variations affect yield.
  • the high-temperature and high-pressure medium 9 in the mold cavity is in a gaseous state, and is recovered by the collecting tube 15 on the upper side of the mold.
  • the low-temperature medium 9 is controlled by the feeding tube 14 to be added to the mold to control the speed of the synthesis column 7 to reduce the temperature.
  • the feeding tube 14 should be closed, and the medium 9 in the mold cavity should be evacuated through the receiving tube 15 to avoid wasting the medium and polluting the environment, and then the pressure can be raised.
  • Head 1 allows the mold to be fully opened, remove the synthesis column that has completed the reaction, and replace it with a new synthesis column, and then proceed to the next synthesis process.
  • the feeding tube 14 of the high-pressure mold can be easily connected to the machine (feeder) for adding the medium 9; similarly, the collecting tube 15 can be easily connected to the machine (feeder) for recycling the medium 9;
  • the up and down change of column 7 is simple and repetitive, and it is easy to complete with a robotic hand. In this way, in practice, the addition and recovery of the variable pressure medium 9 and the up and down replacement of the composite column 7 can be automatically completed by the corresponding machine.
  • the fully automatic operation of diamond synthesis is realized, the efficiency is greatly improved, and the cost is greatly reduced.
  • the composite column 7 can also be rapidly cooled outside the mold.
  • the pressure changing medium 9 is firstly a fluid substance and is a good pressure transmitting medium, which effectively reduces the compressive stress in any direction in the high-pressure chemical synthesis mold cavity Q. Secondly, it serves as a pressure changing medium, which can make high pressure
  • the mold is first closed under a low pressure. After the heads of the upper mold 2 all enter the mold cavity of the lower mold cover 3 and the inner cylinder 4 and are protected by them, the heat is used to raise the pressure to a high pressure P 2 state. This is equivalent to effectively suppressing the axial compressive stress of the mold on the mold by using the pressure change effect. Due to these effects, the variable pressure medium 9 can substantially reduce the main compressive stress in the high-pressure chemical synthesis mold so that the achievable pressure can reach a higher value, which is also the main basis of the present invention.
  • the pressures P 2 and P 3 of the pressure-storage medium 9 at a high temperature 2 can reach very high values, so that the reaction tends to be complete. High-quality products.
  • the larger the cavity Q volume, the larger the volume of the synthetic column 7 that can be accommodated, the higher the diamond output per mold, and the larger composite mold output can greatly exceed the existing technology.
  • This mold can also be used for high-pressure recrystallization of diamond powder.
  • the volume change of the diamond before and after the recrystallization process is negligible. Therefore, the state change process of the pressure-varying medium during recrystallization can be roughly regarded as 0 ⁇ A ⁇ B shown in Figure 2 Process, it does not require a large cavity Q volume V to run smoothly. Therefore, this mold does not need to be made very large and is also suitable for high-pressure recrystallization of diamond powder. Because the pressure achieved by this mold is higher, recrystallization can be performed at higher temperatures, the corresponding crystallization speed is accelerated, and the crystallization time can be shortened.
  • FIG. 5 is a schematic structural diagram of Embodiment 2 of the present invention.
  • FIG. 6 is a schematic structural diagram of Embodiment 3 of the present invention.
  • Embodiment 2 is basically the same as that of Embodiment 1.
  • the names and meanings of the same reference numerals in the figures are the same as those in FIG. 1.
  • the difference is that in Embodiment 2, an ultrasonic oscillating structure 6 is provided in the cavity Q, which can generate ultrasonic waves. , The pressure of the pressure swing medium 9 is raised.
  • the ultrasonic oscillating structure 6 can be used alone or in combination with a heating resistor (the heating resistor is not shown because it is covered by 6 in FIG. 5) to achieve the pressure required for the reaction.
  • the third embodiment is also a variation from the first embodiment.
  • the names and meanings of the same reference numerals in the figure are the same as those in FIG.
  • the high-voltage or high-voltage discharge excites the transformer 9 to generate the required high voltage.
  • the discharge structure 6 can also be used alone or with a heating resistor (the heating resistor is covered by 6 "in Figure 6, so it is not shown) ).
  • the pressure-change medium 9 used in this embodiment may be the first type of pressure-change medium in Embodiment 1-the heat-pressure-change medium, or the second type of pressure-change medium.
  • Pressure medium inert fluid material resistant to synthetic high pressure can be used. In use, the constant pressure medium does not need to be heated to a high temperature state, which can reduce a part of the energy consumption for heating and cooling the heat pressure medium.

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  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Mechanical Engineering (AREA)
  • Organic Chemistry (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Carbon And Carbon Compounds (AREA)

Abstract

L'invention concerne une matrice synthétique à haute pression qui se prête à la fabrication de diamants et autres matériaux analogues devant être synthétisés à haute pression. Cette matrice est caractérisée en ce qu'elle présente une cavité (Q) qui est remplie d'un fluide expansible (9). Ainsi, on peut assurer une pression plus élevée, une réaction plus complète, une meilleure qualité, un rendement plus élevé et un coût inférieur par rapport à l'art antérieur.
PCT/CN1998/000245 1997-10-13 1998-10-13 Matrice synthetique a haute pression WO1999019058A1 (fr)

Priority Applications (1)

Application Number Priority Date Filing Date Title
AU95284/98A AU9528498A (en) 1997-10-13 1998-10-13 High pressure synthetic die

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
CN97227496.0 1997-10-13
CN97227496 1997-10-13

Publications (1)

Publication Number Publication Date
WO1999019058A1 true WO1999019058A1 (fr) 1999-04-22

Family

ID=5198970

Family Applications (1)

Application Number Title Priority Date Filing Date
PCT/CN1998/000245 WO1999019058A1 (fr) 1997-10-13 1998-10-13 Matrice synthetique a haute pression

Country Status (2)

Country Link
AU (1) AU9528498A (fr)
WO (1) WO1999019058A1 (fr)

Cited By (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US7160423B2 (en) 2002-03-05 2007-01-09 Caliper Life Sciences, Inc. Mixed mode microfluidic systems
CN106914622A (zh) * 2017-03-13 2017-07-04 中国科学技术大学 一种超高等静压静温环境生成装置及方法
CN115041097A (zh) * 2022-06-14 2022-09-13 中南钻石有限公司 一种超硬材料合成用复合型密封传压结构及成型工艺

Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US3249964A (en) * 1963-09-09 1966-05-10 Stackpole Carbon Co Producing dense articles from powdered carbon and other materials
US3490344A (en) * 1967-07-10 1970-01-20 Western Electric Co Pressure vessel
US4251488A (en) * 1978-11-16 1981-02-17 Estanislao Antonio J Means for high pressure production of diamonds

Patent Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US3249964A (en) * 1963-09-09 1966-05-10 Stackpole Carbon Co Producing dense articles from powdered carbon and other materials
US3490344A (en) * 1967-07-10 1970-01-20 Western Electric Co Pressure vessel
US4251488A (en) * 1978-11-16 1981-02-17 Estanislao Antonio J Means for high pressure production of diamonds

Cited By (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US7160423B2 (en) 2002-03-05 2007-01-09 Caliper Life Sciences, Inc. Mixed mode microfluidic systems
CN106914622A (zh) * 2017-03-13 2017-07-04 中国科学技术大学 一种超高等静压静温环境生成装置及方法
CN106914622B (zh) * 2017-03-13 2019-02-01 中国科学技术大学 用超高等静压静温环境焊接的方法
CN115041097A (zh) * 2022-06-14 2022-09-13 中南钻石有限公司 一种超硬材料合成用复合型密封传压结构及成型工艺

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Publication number Publication date
AU9528498A (en) 1999-05-03

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