HIGH-TEMPERATURE-HIGH-PRESSURE PROCESSING UNIT BY SOLVENT APPLICATION OF PRESSURE

Abstract

To provide a hydrostatic pressure type high temperature and high-pressure treatment apparatus by a wet method and a dry method for efficiently mass-producing high-quality and large-sized synthetic diamond. In the treatment apparatus, a high-pressure cell prevented from the intrusion of a pressure medium into the inside is housed in a high-pressure container, and hydrostatic pressurization is performed by the liquid pressure medium. At least one pressurizing mechanism 10 for the pressure medium 6 is provided, and a pressure medium having a known compressibility and volume change rate is used. A heating mechanism for the pressure medium and a measuring means for the average temperature in the vertical direction are provided, the pressure medium is heated to a predetermined temperature to be thermally expanded, treatment is continued while maintaining the pressure even after the pressurizing mechanism is stopped, and two or more high-pressure cells 9 can be simultaneously subjected to high-temperature and high-pressure treatment at uniform pressure without directionality.

Claims

1. A processing apparatus capable of high-temperature and high-pressure processing in which uniform pressure is applied without directionality simultaneously to two or more high-pressure cells, wherein: a high-pressure vessel is vertically or horizontally placed in a hydrostatic pressurization system in which outer surfaces of all materials inside the high-pressure vessel are isotopically pressurized by applying pressure to a liquid pressure medium that fills the high-pressure vessel; a high-pressure cell is accommodated inside the high-pressure vessel, the high-pressure cell having a surface provided with an elastic and fluid intrusion resistant sealing material having a deflection temperature under load of 200 C. or more; the pressure medium being used is a pressure medium whose compressibility due to pressure and volume change rate due to temperature are known; a heating mechanism heating the pressure medium, and a measurement means measuring an average temperature in a vertical direction of the pressure medium are provided inside the high-pressure vessel; a cooling mechanism is provided at a higher point than a center position in the vertical direction outside the high-pressure vessel; a pressurizing mechanism capable of pressurizing the pressure medium from outside the high-pressure vessel is operated first to pressurize the pressure medium to a certain pressure level; the pressure medium that has filled the high-pressure vessel is heated to a desired temperature to cause thermal expansion thereof; and the processing is continued while maintaining a desired pressure with continued measurement of pressure and temperature even after the pressurizing mechanism is stopped, wherein, when the pressure is low, a pressure regulation function operates the heating mechanism to increase the pressure by thermal expansion accompanying the heating of the pressure medium, and when the pressure is high, the pressure regulation function operates the cooling mechanism to reduce the pressure.

2. The processing apparatus capable of high-temperature and high-pressure processing in which uniform pressure is applied without directionality simultaneously to two or more high-pressure cells according to claim 1, wherein the processing apparatus comprises at least one pressure medium pressurizing mechanism that the processing apparatus can use first; the pressure medium being used is a liquid pressure medium having a ratio of volume expansion caused by heat at 150 C. greater than a ratio of volume compression caused by pressure at 500 MPa; the heating mechanism heating the pressure medium is provided inside the high-pressure vessel; the cooling mechanism is provided at a higher point than a center position in the vertical direction outside the high-pressure vessel; a means for measuring temperatures is provided for measuring an average temperature in the vertical direction through measurement of surface temperatures of a high thermal conductivity member that is attached to a surface along the vertical direction of a support plate that is installed over an entire length in the vertical direction of the high-pressure vessel; means for measuring temperatures are provided at positions of a highest point and a lowest point of the temperature determined by thermal flows of the pressure medium inside the high-pressure vessel; the temperature of the pressure medium that has filled the high-pressure vessel is controlled by the heating mechanism and the cooling mechanism for the pressure medium; and thermal expansion caused by heating the pressure medium is utilized to raise the pressure inside the high-pressure vessel to a higher level than a value reached by use of the pressurizing mechanism.

3. A processing apparatus that performs hydrostatic pressurization using a liquid pressure medium inside a horizontally placed high-pressure vessel, characterized in that the processing apparatus comprises a pair of molds that fit together at their lower and upper portions and have elastic and fluid intrusion resistant surfaces having a deflection temperature under load of 200 C. or more, the molds including an upper mold, which is a columnar vessel fixedly attached to a lower surface of a lid of the high-pressure vessel, with a pipe leading to a vessel for injecting the pressure medium and a pipe for collecting the pressure medium connected thereto, and a lower mold in a hollow cylindrical shape with a bottom, including a recess for accommodating a high-pressure cell and an opening thereabove, the lower mold being fixedly attached to an inner wall of a body of the high-pressure vessel, a pipe for injecting the pressure medium being connected to the body of the high-pressure vessel; wherein, after a high-pressure cell has been accommodated in the recess of the lower mold, the processing apparatus performs a first step, during lid tightening of the high-pressure vessel, in which the lid is lowered as the upper mold is inserted into the lower mold by remote control by means of a tapered guide mechanism in a lower portion of the upper mold, a second step in which an atmosphere in a space between the upper mold and the lower mold is evacuated to vacuum immediately before the lid and the body come into close contact with each other to bring both molds to close contact with each other, a third step in which the pressure medium that has filled the upper mold in advance is squeezed out and collected to a vessel installed above in a vertical direction when the lid and the body make close contact with each other, and a fourth step after lid tightening, in which an entire inner surface of the upper mold and an entire outer surface of the lower mold that are in liquid communication are hydrostatically pressurized simultaneously with the same pressure medium, whereby the processing apparatus is capable of hydrostatic pressurization in which two or more high-pressure cells are uniformly pressurized without contacting the pressure medium.

4. The processing apparatus that performs hydrostatic pressurization using a liquid pressure medium inside a horizontally placed high-pressure vessel according to claim 1, characterized in that the processing apparatus comprises a pair of molds that fit together at their lower and upper portions and have elastic and fluid intrusion resistant surfaces having a deflection temperature under load of 200 C. or more, and at least one pressure medium pressurizing mechanism that the processing apparatus can use first; the pressure medium being used is a pressure medium whose compressibility due to pressure and volume change rate due to temperature are known; a heating mechanism heating the pressure medium, and a measurement means measuring an average temperature in the vertical direction of the pressure medium are provided inside the high-pressure vessel; a cooling mechanism is provided at a higher point than a center position in the vertical direction outside the high-pressure vessel; an upper mold, which is a columnar vessel, is fixedly attached to a lower surface of a lid of the high-pressure vessel, with a pipe for injecting the pressure medium and a pipe leading to a vessel for collecting the pressure medium connected thereto; a lower mold in a hollow cylindrical shape with a bottom, including a recess for accommodating a high-pressure cell and an opening thereabove, is fixedly attached to an inner wall of a body of the high-pressure vessel; a pipe for injecting the pressure medium is connected to the body of the high-pressure vessel; after a high-pressure cell has been accommodated in the recess of the lower mold, the processing apparatus performs a process comprising a first step, during lid tightening of the high-pressure vessel, in which the lid is lowered as the upper mold is inserted into the lower mold by remote control by means of a tapered guide mechanism in a lower portion of the upper mold, a second step in which an atmosphere in a space between the upper mold and the lower mold is evacuated to vacuum immediately before the lid and the body come into close contact with each other to bring both molds into close contact with each other, a third step in which the pressure medium that has filled the upper mold in advance is squeezed out and collected to a vessel installed above in a vertical direction when the lid and the body make close contact with each other, and a fourth step after lid tightening, in which an entire inner surface of the upper mold and an entire outer surface of the lower mold that are in liquid communication are hydrostatically pressurized simultaneously with the same pressure medium, whereby the pressure medium that has filled the high-pressure vessel is heated to a desired temperature to cause thermal expansion thereof, whereby the processing is continued while maintaining the pressure even after the pressurizing mechanism is stopped, and whereby hydrostatic pressurization is performed in which two or more high-pressure cells are uniformly pressurized without contacting the pressure medium.

5. The processing apparatus according to claim 3, wherein the pair of molds is made of a material that is any of a silicone rubber, nitrile rubber, fluor rubber, heat-resistant fluorine resin, or a composite material including these.

6. The processing apparatus according to claim 3, further comprising a mesh-like or porous medium flow mechanism that supports the high-pressure cells weighing 10 kg or more in the direction of gravity via the lower mold to allow for the high-temperature and high-pressure processing without obstructing flows of the pressure medium.

7. The processing apparatus according to claim 1, wherein high-pressure cells of two or more kinds of shapes can be subjected to simultaneous high-temperature and high-pressure processing, provided that the two or more high-pressure cells each have a totally symmetric shape.

8. The processing apparatus according to claim 1, wherein the two or more high-pressure cells are one or more of a regular hexahedron, a regular octahedron, a hexahedron/octahedron with all their corners cut off to form faces, or a segmented sphere.

9. The processing apparatus according to claim 1, wherein one or more of toluene, ethanol, methanol, benzene, acetone, and a liquid mixture of these organic solvents is used for the pressure medium.

10. The processing apparatus according to claim 1, wherein the pressure medium is a liquid mixture of one or more of ethanol, methanol, and acetone, and water, with a controlled mixing ratio, for more refined thermal expansion rate control, which enables more accurate pressure control through measurement and control of temperatures.

11. The processing apparatus according to claim 1, wherein heat sources inside the high-pressure vessel that is cylindrical are aligned and placed in a central position from a lower portion to a middle portion in the vertical direction, while a cooling function provided by a cooling medium is placed outside the high-pressure vessel in an upper portion in the vertical direction, with a partition plate made of a low thermal conductivity material blocking flows of the pressure medium therebetween, whereby a structure is configured in which a thermosiphon is created in vertical opposite directions, to enable more exact determination of positions of a highest point and a lowest point of temperature that are determined by the thermosiphon, and to enhance temperature measurement and control accuracy by measurement of a maximum temperature and a minimum temperature.

12. The processing apparatus according to claim 11, wherein a thin, elongated plate-like material having a high thermal conductivity is attached on a surface of the partition plate over an entire length in the vertical direction, and temperatures of this surface are measured to enable more accurate measurement of an average temperature in the vertical direction of the pressure medium.

13. The processing apparatus according to claim 1, wherein a selection of thermal conductivity of an anvil made of an ultra-hard material inside the high-pressure cells enables pressurizing speeds and target pressures of the pressure medium inside the high-pressure vessel to be changed.

14. The processing apparatus according to claim 13, wherein the anvil inside the high-pressure cells is made of a material having a low thermal conductivity to allow itself to be used in a control of reducing pressurizing speed, including zirconia, silicon nitride, cermet, boron carbide, and materials mainly composed of these.

15. The processing apparatus according to claim 1, further comprising a check valve that operates in a direction in which a piping path of the pressure medium is closed when a temperature rise of the pressure medium has led to a higher pressure inside the high-pressure vessel than pressure inside the pressurizing mechanism, which makes it possible to disconnect the piping path from the pressurizing mechanism to the high-pressure vessel on a pressurizing mechanism side of the check valve during the high-temperature and high-pressure processing.

16. The processing apparatus according to claim 1, wherein a piping path extending from the pressurizing mechanism is connectable to another high-pressure vessel to enable shared use of the one pressurizing mechanism among a plurality of high-pressure vessels.

17. The processing apparatus according to claim 1, wherein the high-temperature and high-pressure processing can be continued for over 8 hours or more even after the pressurizing mechanism is disconnected, with the two or more high-pressure cells inside taking up the high-pressure vessel.

Description

BRIEF DESCRIPTION OF THE DRAWINGS

[0107] FIG. 1 shows the schematic diagram of the pressurization device and the high-pressure cell in the conventional hydrostatic pressurization method for academic research; (The hydraulic pressure device is integrated with the high-pressure cell).

[0108] FIG. 2 shows the configuration flow of the high-temperature and high-pressure processing apparatus (pressure medium contact type: wet process) using liquid medium hydrostatic pressurization.

[0109] FIGS. 3A and 3B show an example of the binding mechanism (a. vertical installation, b. horizontal installation) in the high-pressure vessel in the pressure medium contact type (wet process).

[0110] FIG. 4 shows an example of the processing apparatus in which one pressurizing mechanism is shared by a plurality of high-pressure vessels.

[0111] FIGS. 3A and 3B a schematic diagram of the high-temperature and high-pressure processing apparatus using liquid medium hydrostatic pressurization of the pressure medium non-contact type (dry process).

[0112] FIG. 6 shows an example of the configuration flow of the high-temperature and high-pressure processing apparatus using hydrostatic pressurization of the liquid medium for dry process in a preparatory stage.

[0113] FIG. 7 shows an example of the configuration flow of the liquid medium pressurized high temperature/high-pressure processing apparatus for dry process after the preparatory stage.

[0114] FIGS. 8A to 8C show an enlarged view of the upper molding die 40 for the fluid-proof [heat-resistant]elastic material and an explanatory view of its effect. This material is used in the dry process equipment described in FIG. 6 and FIG. 7.

[0115] FIGS. 9A to 9B show a schematic diagram of the circulation situation of the pressure medium due to heat convection by a thermosiphon in the high-pressure vessel (a. wet treatment, b. dry treatment).

[0116] FIG. 10 shows a comparison of compressibility of pure alcohol and aqueous alcohol solution.

MODE FOR CARRYING OUT THE INVENTION

[0117] Here, as a mode for carrying out the present invention, the following items of the high-temperature and high-pressure processing apparatus using the liquid medium hydrostatic pressurization method will be described with reference to the drawings. 1) is an overview of the structure of the pressure medium contact type (wet process). 2) is the structure of pressure medium non-contact type (dry process) and its mold structure and operation procedure. In addition, the common points of the above two will be explained in detail as follows. 3) is the processing equipment in which one pressurizing mechanism is shared by multiple high-pressure vessels. 4) is the structure in which the pressure medium is circulated by the thermosiphon in the high-pressure vessel. It should be noted that FIGS. 2-9 are merely examples and are not intended to limit the present invention.

[0118] FIG. 2 is the configuration flow of the high-temperature and high-pressure processing apparatus (pressure medium contact type: wet process) using liquid medium hydrostatic pressurization according to the present invention. This schematically shows an example of the configuration.

[0119] In this processing apparatus, the closed space surrounded by the high-pressure vessel body 7 and the lid 8 is filled with the liquid pressure medium 6, and two or more High-pressure cells 9 are installed therein. The high-pressure cells 9 have symmetrical shape of a regular hexahedron or a regular octahedron. Or these High-pressure cells are of the type in which all these protruding end faces are cut flat. Alternatively, the high-pressure cells are of the split-sphere type. In the case of the pressure medium contact type (wet process), the outer surfaces of all the High-pressure cells 9 are covered with seals 19 made of the heat- and fluid-resistant elastic material, so that the pressure solvent does not enter. Their interior is evacuated prior to installation in this processing equipment. The pressure medium in the closed space surrounded by the body 7 and the lid 8 of the high-pressure vessel is connected to the pressurizing mechanism 10 through the piping line. The fluid having a known compressibility due to pressure and a coefficient of volume change or volume expansion due to temperature and having a maximum specification temperature of 250 C. or more is used as the pressure medium. The check valve 11 and the gate valve 12 are installed in the middle of the pipeline.

[0120] The liquid pressure medium 6 in the closed space is pressurized by the pressurizing mechanism 10 at the beginning of the treatment. This pressure (for example, 500 MPa) is the value that can be achieved by the inherent performance of the pressurizing mechanism 10 at room temperature.

[0121] On the other hand, in the high-pressure cells 9, processed material 13, the internal heating source 14, and the anvil 15 are installed in this order from the inside. The mass of each high-pressure cells 9 weighs over 10 kilograms (Kg). A power line for the internal heating source 14 is connected to the waterproof pressure connector 18 in the high-pressure vessel protruding from the outer surface of the high-pressure cells 9. The same applies to the connection cable 17 such as the measurement line of the internal thermocouple 16 for measuring the temperature of the processed material 13.

[0122] The plurality of High-pressure cells 9 is also fixed or suspended within the high-pressure vessel by the binding mechanism 20 so that all outer surfaces do not directly contact the inner wall of the high-pressure vessel. The maximum operating pressure of this device is the designed compressive strength of the high-pressure vessel. In recent years, there are also high-pressure devices with the pressure of several GPa. Also, the maximum temperature of the device is determined by the maximum operating temperature of the seal. At this temperature, the heat- and fluid-resistant elastic material does not deform significantly.

[0123] The high-pressure vessel 7 may be either vertical or horizontally placed. Further, the pressurized mechanism 10 may be the motor-type pump or the piston-type pump. Furthermore, although FIG. 2 shows three types and four pieces of High-pressure cells, there are no restrictions on the type and number of High-pressure cells as long as they are two or more.

[0124] Here, the operation following pressurization of the pressure medium by the pressurizing mechanism 10 will be described. In FIG. 2, the internal heat source 12 connected to source power supply of the internal heating 21 is heated. Next, the processed material 13 is heated to 1300 C. or higher. Over time, heat conduction heats the pressure medium 6 to the predetermined temperature (eg 150 C.). When the pressure medium 6 is heated, its pressure fluctuates due to the volume change caused by the temperature. The temperature change of the pressure medium 6 is detected by the high-pressure vessel thermocouple 22. The thermocouple 22 is installed in an exposed state on the inner surface of the high-pressure vessel. Also, the change in temperature is monitored by the temperature detecting function 23. The high-pressure vessel thermocouple 22 is classified into three types: TC1 (highest point), TC2 (lowest point), and TC3 (average point). TC3 is used to measure steady state average temperature. TC1 for the maximum temperature and TC2 for the minimum temperature are used for temperature control during start-up, rapid heating, and cooling. If the compressibility and volume change rate of the pressure medium are unknown, data are acquired. The DAC device and the calibration device may be connected to the gate valve 12 in the processing apparatus to acquire these physical property data before actual processing.

[0125] Here, the case where the temperature rises of the pressure medium 6 causes the pressure rise due to the change in volume to exceed the set value will be described. Upon receiving the signal from the temperature detecting function 23, the pressure regulation function 24 determines that the pressure of the pressure medium 6 should be reduced.

[0126] The signal from the pressure regulation function 24 is transmitted to the temperature decrease mechanism 25. The refrigerant cooler 26 then operates. The coolant is sent to the cooling jacket 27. The pressure medium 6 is now cooled. The returned coolant is cooled again by the coolant cooler 26.

[0127] This prevents the pressure in the high-pressure vessel from increasing in the random fashion. The processing equipment can control the pressure by accurately detecting the temperature of the pressure medium 6 with the high-pressure vessel thermocouple 22. In addition, the working pressure of the pressure medium 6 can be accurately controlled to the desired processing pressure (for example, 500 MPa).

[0128] Conversely, the case will be described in which the rise of the temperature of the pressure medium 6 increases the pressure as the volume changes. This case provides higher pressure compared to what the pressurizing mechanism 10 performance achieves. Again, the pressure regulation function 24 receives the signal from the temperature detecting function 23. The pressure regulation function 24 determines that the pressure medium 6 should be pressurized.

[0129] The signal from the pressure regulation function 24 is transmitted to the heating mechanism 28. The heating mechanism 28 operates the hydraulic-medium heating heater (hereinafter referred to as pressure medium heater)30. The pressure medium heater 30 is installed in the high-pressure vessel. As a result, the pressure medium 6 is heated (eg 250 C.). Even in this case, the temperature of the pressure medium 6 is detected by the high-pressure vessel thermocouple 22. The processing pressure is controlled with high accuracy, and the pressure does not continue to exceed the pressure resistance limit of the high-pressure vessel. Should the pressure become too high, the temperature decrease mechanism 25 reduces the pressure to an appropriate processing pressure. As a result, the pressure of the pressure medium (eg 700 MPa) can be maintained. The pressure of this pressure medium makes it possible to obtain the high working pressures necessary to produce large size synthetic diamond products. (e.g., 7 GPa).

[0130] As the heating of the pressure medium 6 progresses, the pressure inside the high-pressure vessel becomes higher than the pressure (for example, 500 MPa) pressurized by the pressurizing mechanism 10. Therefore, the piping route leading to the high-pressure vessel can be removed from the flange surface of the check valve 11 on the pressurizing mechanism side. Thus, even if the pressurizing mechanism 10 is stopped or removed from the pressurizing mechanism 10, the processing apparatus of the present invention can continue high-temperature and high-pressure processing. In addition, when disconnecting the piping of the pressurizing mechanism 10 from the processing apparatus, the piping path can be closed by the gate valve 12. Moreover, the pressurizing mechanism 10 may be stopped when disconnecting the pipe or may be operated with its output reduced.

[0131] As another function, the decompressing mechanism 55 is installed. The decompressing mechanism 55 consists of the valve type such as the needle valve or the diaphragm valve. This valve is used when stopping the operation of the processing equipment or when there is an overpressure problem. The pressure of the pressure medium in the high-pressure vessel can be reduced by discharging the minute volume of the fluid that propagates the pressure of the pressure medium, on the order of several to several tens of cubic centimeters (cm{circumflex over ()}3), to the outside of the system.

[0132] On the other hand, since pressure gauges have poor measurement accuracy in this pressure range, they often cannot be used for pressure control. Therefore, the piezoelectric sensor 32 such as the load cell is installed for rough pressure monitoring.

[0133] FIGS. 3A and 3B a the diagram schematically showing an example of the binding mechanism 20 (a. vertical installation, b. horizontal installation) in the high-pressure vessel in the pressure medium contact type (wet process) of the present invention. Also, the appropriate shape of the high-pressure cells 9, that is, the shape of the anvil 15, varies depending on the size and shape of the product. However, in the processing apparatus of the present invention, the high-pressure cells 9 can process any shape if it has the symmetrical shape.

[0134] In FIGS. 3A and 3B, the binding mechanism 20 has the shape suspended from the lid 8 in both vertical and horizontal placement. In this figure the axial forces exerted by the pressure medium 6 on the lid 8 are supported by the press frame 33. A plurality of High-pressure cells 9 installed in the high-pressure vessel is required to propagate pressure from the pressure medium 6 to all surfaces. As such, the body 7 of the high-pressure vessel should not meet the inner surface of the sidewalls and the bottom surface. The high-pressure cells 9 should expose substantially the entire surface. In addition, they must be fixed or suspended in the high-pressure vessel while maintaining the internal vacuum state. Therefore, the binding mechanism 20 has the shape and structure that reduces the area in contact with the high-pressure cells 9 as much as possible.

[0135] Also, the case where isotropic pressure cannot be obtained due to the influence of the binding mechanism 20 and product quality is affected will be described. In this case, the pressure medium circulation layer 48, which will be described later, may be provided in the portion that inevitably meets the high-pressure cells 9.

[0136] In addition, FIGS. 3A and 3B have the shape in which the binding mechanism 20 is suspended from the lid 8. However, the shape of this may be one supported from the floor surface or wall surface of the high-pressure cylinder, or one fixed. This is regardless of vertical or horizontal orientation. It may be possible to place or suspend several High-pressure cells with one securing device. Also, the structure for supporting the axial force may be the method other than the press frame 33, such as bolt fastening or loading.

[0137] FIG. 4 shows an example of the processing apparatus of the present invention in which a plurality of vertically placed high-pressure vessels shares one pressurizing mechanism. As described above (0052), after the initial stage of pressurizing the pressure medium therein in any one high pressure vessel, the processing equipment can deactivate the pressurizing mechanism 10. Nevertheless, high temperature and high-pressure processing can be continued. Also, the check valve 11 can be removed from the piping route connected to the high-pressure vessel at the position on the pressurizing mechanism 10 side. By connecting the removed piping route to another high-pressure vessel, another processing apparatus can be started up. Thus, the pressurization of the pressure medium in the pressure vessel of another processing unit can be started. FIG. 4 is the diagram for explaining the state in which a pressurization pump 36, which is one hydraulic pump type pressurizing mechanism 10, is shared by the bodies 7 and lids 8 of eight high pressure vessels (A to H).

[0138] One pressurization pump 36 is mounted on the movable cart 35 and can be moved to the predetermined position on the rails 34. After stopping and fixing at the predetermined position, the high-pressure hose 37 is attached to the pressurizing mechanism side of the check valve 11 of the high-pressure vessels from A to H. By operating the pressurization pump 36 here, the pressure medium is pressurized to the certain pressure (for example, 500 MPa) that its performance allows under normal temperature. Further, the pressure medium tank 38 is installed below the pressurization pump 36 of the movable cart 35.

[0139] In FIG. 4, eight high pressure vessels are connected to one pressurizing mechanism 10. However, the number of bodies 7 and lids 8 of the high-pressure vessels to be connected may be greater or less than this. The growth time depends on the size of the synthetic diamond product to be manufactured, and the time to be held at high temperature and high pressure may extend to several days. However, the retention time is mainly proportional to the size of the synthetic diamond product to be manufactured. First, the plan for the operation schedule of the processing equipment, which is determined by the size of the product to be manufactured, is formulated, and the number of high-pressure vessels that can be handled by one pressurizing mechanism is calculated. Based on these results, the business operator decides on plant equipment and layout plans, operation schedules, the number of operating personnel, and so on. This procedure is reasonable.

[0140] In FIG. 4, the pressurizing mechanism 10, the high-pressure vessel, the press frame 33, and the like are arranged in the plane, but alternatively, they may be arranged in another arrangement. That is, the moving means of the pressurizing mechanism 10 may be arranged vertically in the three-dimensional manner by using another form such as an elevator. These arrangements may be combined. Alternatively, the pressurizing mechanism 10, the high-pressure vessel, the press frame 33, etc. may be fixed, and the piping system may relate to the long high-pressure hose 37, although this may slightly reduce the work efficiency during treatment. By these methods, one pressurizing mechanism 10 can be shared by the bodies 7 and lids 8 of a plurality of high-pressure vessels.

[0141] FIGS. 5A and 5B the schematic diagram of the configuration (a. before lid tightening, b. after lid tightening) of the pressure medium non-contact type (dry process) high-temperature and high-pressure processing apparatus using liquid medium hydrostatic pressurization. This is the schematic diagram of the preparatory stage. In the case of the pressure medium contact type (wet process), work efficiency is remarkably deteriorated due to dealing with the contamination of the pressure medium 6 adhering to the seal 19 made of the heat- and fluid-resistant elastic material and the high-pressure cells 9. This is as described in the second half of Means for Solving Problems above. One of the reasons is that the high-pressure cells 9 are heavy objects that may weigh more than 10 kilograms and weigh several tons. Therefore, the pressure medium non-contact type (dry process) liquid medium hydrostatic pressurization method is required. However, due to the structure of the apparatus, the seal 19 made of the heat- and fluid-resistant elastic material is necessary to obtain a plurality of products in one high-temperature and high-pressure treatment. Also, considerable ingenuity is required for the mechanism for feeding the pressure medium 6 there.

[0142] As shown in FIG. 5A, the hollow cylindrical upper molding die 40 is fixed to the lower portion of the lid 8 of the high-pressure vessel via the upper molding die mounting jig 41. The notching 53 serving as the guide mechanism is provided at the lower end of the upper molding die 40. The heat-resistant penetrating tube 43 is installed in the central hollow cylindrical portion of the upper molding die 40. The folded-type vacuum exhaust port 49 is installed around it. The metallic net spring pipe 57 like the medical stent is installed inside the folded-type vacuum exhaust port 49. The heat-resistant penetrating tube 43 has the heat-resistant and pressure-resistant structure. It houses current and instrumentation leads 5 and the internal thermocouple 16 inside. The high-pressure cell-cooling water pipe 44 is also accommodated if necessary.

[0143] On the other hand, the folded-type vacuum exhaust port 49 maintains its shape and outer diameter during vacuum suction. However, when the pressure medium presses the upper molding die 40, it closes due to the external force. The heat-resistant penetrating tube 43 and the atmospheric escape pipe 45 are connected to the suction pipe-connection box 54 existing in the space recessed from the surface of the lid 8. The connection nozzle with the vacuum suction line is provided there. The heat-resistant penetration tube 43 must be prepared for thermal expansion and interference with the high-pressure cells 9. Therefore, the penetration tube 43 is fixed to the suction pipe-connection box 54 via the spline bearing having the gap through which fluid can flow. In addition, the penetration tube 43 is movable several centimeters in the vertical direction. A flexible pipe leading to the vacuum pump 50 is connected to this connection nozzle. On the other hand, the heat-resistant penetrating tube 43 in the suction pipe-connection box 54 is notched in half Current and Instrumentation Lead 5, internal thermocouple 16, and high-pressure cell cooling water piping 44 now turn to the outer periphery of lid 8. After the direction change, wiring and piping are also installed in the space recessed from the surface of the lid 8. Therefore, the surface of the lid 8 has no projections, and the press frame 33 can be attached by sliding the surface of the lid 8.

[0144] Inside the lid 8, the atmospheric escape pipe 45 surrounds the heat-resistant through pipe 43. The folded-type vacuum exhaust port 49 is provided at the lower portion of the atmospheric escape pipe 45. The folded-type vacuum exhaust port 49 is connected by the spigot structure (the structure in which uneven parts mesh with each other) that can be freely contracted in the diameter direction. The metallic net spring pipe 57 is located inside the folded-type vacuum exhaust port 49.

[0145] As shown in FIG. 5A, the body 7 of the high-pressure vessel, which is placed horizontally, has an opening for the lid 8 at the top of the high-pressure cylinder. The lower mold 39 is fixed to this opening. The lower mold 39 is concave with bottom and has an open cylinder at the top with an opening for loading and unloading the high-pressure cells 9. The high-pressure cells 9 are housed in the recess, and the bottoms of the heavy high-pressure cells 9 are supported by the lower support mechanism 47 via the lower molding die 39. At the contact portion between the support mechanism 47 and the high-pressure cells 9 via the lower molding die 39, the net having the shape conforming to the outer shape of the high-pressure cells 9 is provided on the support mechanism side. This mesh may be the porous pressure medium distribution layer 48. These structures allow the pressure medium 6 to flow freely even after the high-pressure cells 9 are fixed.

[0146] As shown in FIG. 5B, the pipe leading to the vacuum pump 50 is connected to the suction pipe-connection box 54 before and after the body 7 and the lid 8 of the high-pressure vessel are brought into close contact with each other. Also, as the lid 8 descends, the lid 8 is guided to the notching at the lower end of the upper molding die 40. Next, the upper mold 40 and the lower mold 39 are fitted together. In this state, the high-pressure cells 9 are sandwiched and wrapped. Before body 7 and lid 8 are brought into close contact, the air in the space between upper mold 40 and lower mold 39 is drawn to vacuum. In addition to the effect of the negative pressure, the pressure medium 6 is supplied from the gravity equation pressure-medium equalizing tank 42 into the upper molding die 40 to fill it. However, the operations at this stage, that is, the operations corresponding to the first to third steps described in (0040) are considerably complicated due to the opening and closing of valves. FIG. 5B illustrates the state in which the upper mold 40 and the lower mold 39 for one processing pit 46 have already been assembled. Therefore, it cannot be explained only by the state shown in FIG. 5B. Therefore, the configuration and operation thereof will be described with reference to FIG. 6, FIG. 7 and FIGS. 8A and 8C from the next section.

[0147] FIG. 6 is an example of the configuration flow of the pressure medium non-contact type (dry process) high-temperature and high-pressure treatment apparatus using liquid medium hydrostatic pressurization in the preparatory stage of the present invention. FIG. 7 is an example of the configuration flow of the dry process apparatus before processing after going through the preparatory stage of FIG. 6. FIGS. 8A to 8C are an enlarged view of the upper molding die 40 for the heat- and fluid-resistant elastic material used in the dry process apparatus described in FIG. 6 and FIG. 7, and an explanatory view of the effect thereof.

[0148] Note that FIG. 6 and FIG. 7 do not show the overall configuration of the liquid medium pressurized high-temperature and high-pressure processing apparatus. FIG. 6 and FIG. 7 explain the difference in the structure of the equipment when the pressure medium non-contact type (dry process) is used. The overall configuration including these control systems was explained in FIG. 2 of the pressure medium contact type (wet process).

[0149] FIG. 6 shows the preparatory stage in which the high-pressure cells 9 are installed in the body 7 of the high-pressure vessel placed horizontally, and then the lid 8 is lowered to seal the body 7 in the dry process apparatus.

[0150] The pressure medium 6 in the body 7 of high-pressure vessel is confined by the inner wall surface of the body 7 and the lower molding die 39, and there is no portion where the pressure medium 6 is exposed to the atmosphere. The partition plate 31 is arranged in the pressure medium 6 in the body 7 and has an elongated copper plate 65 for measuring the average temperature on its surface. The high-pressure cells 9 are brought into close contact with the molding die by fitting the lower molding die 39 and the upper molding die 40 made of heat- and fluid-resistant elastic material. The High-pressure cells 9 in FIG. 6 have three types of shapes, and the number of them is four. One of the High-pressure cells, the regular octahedral type, is the high-pressure cell 56 of which all tip portions are cut off. The support mechanism 47 is installed immersed in the pressure medium 6. That is, FIG. 6 shows an example in which four processing pits 46 are formed in one high-pressure vessel.

[0151] On the other hand, the upper molding die 40 for the heat- and fluid-resistant elastic material shown in FIG. 6 is bag-like elastic material. The upper molding die 40 is fixed to the lower portion of the lid 8 by the upper molding die mounting jig 41. Its interior is filled with pressure medium 6. The pressure medium 6 inside the bag-shaped upper mold 40 is not exposed to the atmosphere.

[0152] The lower end of the upper molding die 40 has the notching 37 that serves as the guide mechanism. The upper molding die 40 has the shape along the high-pressure cells 9. In FIG. 6, the four-split upper molding die 40 is shown as an example, and the pipe for the pressure medium 6 is connected to each split bag. The gravity equation pressure-medium equalizing tank 42 is installed above the lid 8 and is of an open-top type and balanced with the atmosphere. In FIG. 6, the piping route of the pressure medium 6 is connected via the hydraulic-medium equalizing tank slice valve 59 in the open state. Also, the hydraulic-medium equalizing tank slice valve 62 of the gravity equation pressure-medium equalizing tank 42 is in an open state. On the other hand, the upper hydraulic-medium slice valve 58 on the pressurizing mechanism 10 side is closed.

[0153] The heat-resistant penetrating tube 43 penetrating the lid 8 is installed at the center of the upper molding die 40. Outside the heat-resistant penetrating tube 43 is the atmospheric escape pipe 45. The atmospheric escape pipe 45 also serves as an evacuation port for evacuating to vacuum. Also, this atmospheric escape pipe 45 is positioned inside the upper molding die 40. The metallic net spring pipe 57 is housed inside the folded-type vacuum exhaust port 49 below the atmospheric escape pipe 45. The upper ends of the heat-resistant penetrating tube 43 and the atmospheric escape pipe 45 are connected to the suction pipe-connection box 54 installed in the recess on the surface of the lid 8. The heat-resistant penetrating tube 43 has the pressure-resistant and heat-resistant structure. The heat-resistant and pressure-resistant current/instrumentation lead wire 5 and the internal thermocouple 16 are installed in the heat-resistant penetrating tube 43. The pressure-resistant high-pressure cell cooling water pipe 44 is installed here as required. The current/instrumentation lead wire 5 is connected to the high voltage cell 9 by the flexible connection cable 17 via the pressure-resistant connector. Note that not all figures are shown in FIG. 6.

[0154] FIG. 7 shows the state after the preparation stage of FIG. 6. FIG. 7 shows the state immediately after the lid 8 meets the body 7 of the high-pressure vessel after the lid 8 has been lowered. This is the pre-processing stage. However, at this stage, the pressurizing mechanism 10 is not yet in operation. Moreover, all the heating means are not in operation. The right side of FIG. 7 shows the cross-sectional view taken along line A-A.

[0155] When the lid 8 is lowered, the upper molding die 40 fixed to the lower portion of the lid 8 is lowered. During the descent, the inner wall of the lower mold 39 guides the notching 53 at the lower end of the upper mold 40. After that, this lower end eventually hits the upper part of the high-pressure cells 9. The lower end of the upper molding die 40 has the shape along the high-pressure cells 9. Furthermore, the lid 8 is lowered by remote control by means of the notching 53 at the lower end of the upper molding die 40 and the tapered guide mechanism at the bottom. As it descends, the upper molding die 40 is inserted into the lower molding die 39 (first step).

[0156] In the first step of the former stage, the upper molding die 40 enters into the concave portion of the lower molding die 39 by remote control and is fitted therewith. Next, in FIG. 7, the lid 8 of the high-pressure vessel is further lowered. However, the lowering of the lid 8 is temporarily stopped just before the lid 8 comes in close contact with the body 7. This is when the heat-resistant penetrating tube 43 approaches the position closest to the high-pressure cells 9. At this point, the closed space is formed by the lower mold 39, the high-pressure cells 9, and the upper mold 40. The vacuum pump 50 is now operated. As a result, the air in the gap between the lower molding die 39 and the upper molding die 40 is discharged by vacuum suction through the heat-resistant penetrating tube 43. At the same time, the atmosphere remaining in the high-pressure cells 9 is also discharged by vacuum suction. By evacuating residual atmospheric air, the gap between lower mold 39 and upper mold 40 is eliminated. In addition, the upper mold 40 stretched by vacuum pressure fills the space. As a result, both molding dies are in close contact with each other without any wrinkles. As a result, all the outer surfaces of the high-pressure cells 9 can be sandwiched between both molding dies without gaps. (Second step).

[0157] In the preceding second step, the upper molding die 40 is stretched and pulled by the vacuum pressure to increase the inner volume. This is the situation in which more fluid can be drawn into it. Here, in FIG. 7, the following operations are performed. First, the pressure medium adjustment tank gate valve 59 and the hydraulic-medium atmospheric release valve 60 of the piping connected to the gravity equation pressure-medium equalizing tank 42 are opened. Subsequently, the pressure medium 6 is supplied to the upper mold 40. As a result, the pressure medium 6 is loaded with atmospheric pressure and gravity. Therefore, the pressure medium 6 has no residual air, and air bubbles, voids, and the like are not mixed. Thereby, the inside of the upper mold 40 can be filled with the pressure medium 6.

(Third Step).

[0158] In FIG. 7, the lid 8 of the high-pressure vessel is further lowered to adhere to the body 7. At that time, the volume occupied by the upper mold 40 is slightly reduced. Thus, at the end of FIG. 7, the pressure medium 6 in the upper mold 40 is squeezed out. The squeezed pressure medium 6 overcomes gravity and flows out to the gravity pressure medium adjustment tank 42 above the lid 8. Therefore, the liquid level of the pressure medium in the gravity equation pressure-medium equalizing tank 42 is higher in FIG. 7 than in FIG. 6. By this operation, the pressure medium 6 in the high-pressure vessel is densely filled in the piping path without air voids or the like entering. At this stage, the flexible pipe leading to the vacuum pump 50 may be disconnected from the connection nozzle of the suction pipe-connection box 54. After the lid 8 is brought into close contact with the body 7 of the high-pressure vessel, the press frame 33 is installed by sliding or the like. This is for supporting the axial force applied to the lid 8 from the pressure medium 6. The lid 8 and the high-pressure vessel 7 are fastened by these. Also, the gate valve 59 on the side of the gravity type pressure medium adjusting tank 42 is closed, and the gate valve 58 on the side of the pressurizing mechanism 10 is opened. In dry process, after this, the pressurizing mechanism 10 is operated to pressurize with the same pressure medium 6. That is, the entire inner surface of the upper molding die 40 and the entire outer surface of the lower molding die 39 are simultaneously pressurized by hydrostatic pressure. As a result, the high-pressure cells 9 can be pressurized isotropically with a uniform pressure without gaps and precisely without directionality.

(Fourth step).

[0159] FIG. 6 and FIG. 7 show the configuration in which four High-pressure cells 9 of three types in the body 7 of the horizontally placed high-pressure vessel are simultaneously processed without contact with the pressure medium. The types of the High-pressure cells 9 illustrated here are three, and the number thereof is four. Essentially, if the number of High-pressure cells 9 is two or more, there is no limit to type or quantity. However, in the case of pressure medium non-contact type (dry process), changing the type of high-pressure cells 9 for high-temperature and high-pressure processing in the processing pit 46 requires the following replacement of the devices. First, the upper mold mounting jig 41 for fixing the upper mold 40 and the lower support mechanism 47 must be replaced. In addition, it may be necessary to replace the lower mold 39 in some cases. Therefore, the pressure medium non-contact type (dry process) is not suitable when the type and number of High-pressure cells 9 to be processed vary from day to day. This method is suitable for efficient high-temperature and high-pressure treatment of many products with the composition that does not vary in type and number.

[0160] FIGS. 8A to 8C are an enlarged view of the upper molding die 40 for the heat- and fluid-resistant elastic material used in the dry process apparatus described in FIG. 6 and FIG. 7, and an explanatory view of the effect thereof. This is an enlarged schematic diagram of the upper molding die 40 for the heat- and fluid-resistant elastic material used in the pressure medium contactless apparatus. FIGS. 8A to 8C are described with the following symbols. FIG. 8A shows the state before pressurization by the pressure medium. FIG. 8B to FIG. 8C show the state after pressurization. Note that FIG. 8B indicates the force balance when the upper mold 40 is not present. FIG. 8C shows the force balance when the upper mold 40 is present. It should be noted that these show the structure at the cross-sectional position of the A-A line shown in FIG. 7. An enlarged view of the structure of the upper mold 40 at the cross-sectional position of the B-B line shown in FIGS. 8A to 8C is as follows. (a) is the integrated hollow cylinder. (b) is the vertical split type. (c) is the vertically divided three-part type. (d) is the vertically divided 4-part type.

[0161] In FIGS. 8A and C, and the magnitude and direction of the force exerted by the pressure medium 6 are indicated by arrows. This figure shows the state in which the pressure is balanced by the pressure medium 6 in the high-pressure vessel with the pressurizing mechanism 10 in operation. The pressure medium 6 pressurized by the pressurizing mechanism 10 has the following effects. In b, only the entire outer surface of the lower mold 39 is hydrostatically pressurized. On the other hand, in FIG. 8C, the entire inner surface of the upper molding die 40 and the entire outer surface of the lower molding die 39 are hydrostatically pressurized simultaneously. The pressurization of the pressure medium 6 in the high-pressure vessel creates force balance and imbalance, as shown in FIGS. 8B and C.

[0162] Without the upper molding die 40, the stress from above is insufficient. Therefore, the high-pressure cells 9 are lifted by the action of the pressure medium 6 as shown in b. As a result, the high-pressure cells 9 are pressed against the lid 8 with the non-isotropic force. If there is the upper molding die 40, the force from above is applied evenly. Therefore, the high-pressure cells 9 are isotropically pressurized while maintaining its original position. Any upper mold 40 of (a), (b), (c) and (d) can be isotropically pressed. The upper molding die 40 should be selected to conform to the shape of the upper portion of the high-pressure cells 9.

[0163] FIGS. 9A to 9B are the schematic diagram (a. wet process, b. dry process) of the heat convection circulation of the pressure medium 6 by the thermosiphon in the high-pressure vessel. As described in Example 2 below, under the operating conditions of the present invention, the viscosity of the organic solvent and the like used as the pressure medium 6 is approximately the same as that of water at normal temperature and pressure. Therefore, if the following arrangement is devised, thermal convection (thermosiphon) can be generated in the high-pressure vessel. That is, disposing the heating mechanism 28 installed in the high-pressure vessel and disposing the temperature reducing mechanism 25 by means of the cooling jacket 27 attached to the outer wall of the high-pressure vessel. The present invention is the system that intentionally increases the mass and volume of the pressure medium by housing two or more High-pressure cells in the high-pressure vessel to control the pressure of the pressure medium. Here, by preventing localization of temperature due to retention, the accuracy of temperature measurement and control, that is, the accuracy of pressure control in the present invention can be improved. FIG. 9A is the structure for wet process. FIG. 9B is the structure for dry process. In both cases, the heating sources within the high-pressure vessel are the internal heating source 14 within the high-pressure cells and the pressure medium heater 30 of the heating mechanism 28. The cooling jacket 27 is attached to the outside of the high-pressure vessel. In FIGS. 9A and 9B, both a and b show that the body 7 is a cylindrical high-pressure vessel (hereinafter referred to as high-pressure cylinder). Heating sources are arranged on the central axis in the body 7 of the high-pressure vessel at the central portion (the center position of the cylinder) and the bottom portion (the lower end of the cylinder). They are arranged vertically in the line on the central axis.

[0164] FIG. 9A shows an example of the structure capable of generating the thermosiphon in the pressurized medium contact type (wet process) high-temperature and high-pressure treatment apparatus using liquid medium hydrostatic pressurization in which the high-pressure cylinder is vertically placed. In the vertical installation, the High-pressure cells 9 suspended from the lid 8 are arranged vertically in the line on the central axis of the high-pressure cylinder. FIG. 9A shows an example in which four High-pressure cells 9 are suspended. The internal heat source 14 is housed inside each high-pressure cell 9. Further, the pressure medium heater 30 is arranged at the center of the bottom plate (lower end of the high-pressure cylinder). The cooling jacket 27 of one temperature reducing mechanism 25 is arranged in the upper half range from the approximate center position of the outer wall of the high-pressure cylinder. The cooling jacket 27 is also arranged inside the lid 8. Two partition plates 31 made of ceramic or the like are installed on both sides in parallel with the four High-pressure cells 9. The partition plate 31 is for the purpose of blocking mixing due to flow of fluids on both sides. The copper plate 65 for average temperature measurement, which is thin and elongated like the wire, is installed on this surface over the entire length in the vertical direction. The fluid (the pressure medium with the slightly reduced density) heated by two types of heat sources rises between the two partition plates 31, that is, in the central portion of the high-pressure cylinder. The heated fluid moved to the upper part of the high-pressure cylinder is cooled by the cooling jacket 27 inside the lid 8 and the cooling jacket 27 on the upper half of the outer wall of the high-pressure cylinder. Then, cold fluid (pressure medium with slightly increased density) descends along the outer wall. This system heats the lower end, and center of the central portion of the high-pressure cylinder and cools the upper half of the outer wall. That is, the heated fluid rises in the central portion and the cooled fluid descends in the outer wall portion. This forms the thermosiphon.

[0165] In addition, in the vertically placed high-pressure cylinder, the maximum temperature (TC1) after reaching a steady state is at the upper part of the uppermost high-pressure cells in the central part. Its lowest temperature (TC2) is at the lower end of the outer wall cooling jacket. The average temperature (TC3) is on the copper plate 65 for average temperature measurement. The average temperature does not differ greatly at any position on the long and narrow copper plate like the wire.

[0166] FIG. 9B shows the structure in which the high-pressure cylinder is placed horizontally. This is the non-contact pressure medium (dry process) high-temperature and high-pressure treatment apparatus that utilizes hydrostatic pressurization of the liquid medium and has the structure capable of generating the thermosiphon. FIG. 9B shows the structure at the cross-sectional position of line A-Ain FIG. 7.

[0167] The basic configuration is the same as that of FIG. 9A, but since the high-pressure cylinder is placed horizontally, a plurality of High-pressure cells 9 is arranged horizontally. Therefore, only one of the high-pressure cells 9 is visible on the A-A line cross section. Due to this structure, if the heat quantity of the internal heating source 14 is different in each high-pressure cells 9, the temperature inside the high-pressure vessel tends to be localized in the horizontal direction. Therefore, in the horizontal installation, the pressure medium heater 30 and the cooling jacket 27 should be controlled for each processing pit 46.

[0168] Heating of the fluid is provided by the internal heat source 14 at the center of the high-pressure cylinder and the pressure medium heater 30 at the lower end. Cooling is provided by the cooling jacket 27 on the upper lid 8 of the high-pressure cylinder and the cooling jacket 27 on the upper half of the body of the high-pressure cylinder. Mixing of fluids is blocked by two partition plates 31 in one high-pressure cell. As a result, the heated fluid rises in the central portion and the cooled fluid descends in the outer wall portion. That is, the thermosiphon is formed.

[0169] The maximum temperature (TC1), minimum temperature (TC2), and average temperature (TC3) are the same concept as the previous section.

EXAMPLES

[0170] Hereinafter, embodiments of the present invention will be described more specifically with the following configurations based on examples. In addition, the scope of the present invention is not limited by the examples. [0171] Example 1: High-pressure vessel, lid, fixing system of high-pressure cells, and pressurizing mechanism [0172] Example 2: Type and physical properties of pressure medium, viscosity, and compressibility under high pressure [0173] Example 3: Fluid-Proof [Heat-Resistant] Elastic Material Used in Molds [0174] Example 4: Heat-resistant penetrating tube and foldable vacuum exhaust port [0175] Example 5: Temperature lowering mechanism for pressure medium, heating mechanism in high-pressure vessel, and thermosiphon structure [0176] Example 6: High-pressure parts such as high-pressure check valves [0177] Example 7: structure of high-pressure cells and the internal anvil [0178] Example 8: Type and Thermal Conductivity of Super hard Materials for the internal anvils in High-pressure cells

Example 1

[0179] In Embodiment 1, the high-pressure vessel, the lid, the method of fixing the processed material, and the pressurizing mechanism will be described. To facilitate pressure control, the high-pressure vessel of the present invention is required to have an internal volume as large as possible within a reasonable range, and to increase the weight and volume of the pressure medium in the piping system. Therefore, two or more High-pressure cells are installed in one high-pressure vessel. The main body of the high-pressure vessel is the cylindrical high-pressure cylinder that can easily ensure performance related to pressure resistance and is easy to manufacture. High-pressure cylinders are generally single-walled cylinders or composite cylinders made by shrink fitting. There is also the wire-wound structure (the structure in which piano wire or the like is wound around the outer circumference of the high-pressure cylinder to strengthen it). High pressure cylinders are typically designed according to the design fatigue curve that has a 99.99% or greater probability of non-failure. The structure and design of the pressure vessel, such as the shape and thickness of the high-pressure cylinder, are based on JIS B8265 (2017) and JIS B8267 (2015). In many cases, high-pressure equipment for mass production is frame-type in which the axial force applied to the lid is supported by the press frame.

[0180] When the high-pressure cylinder is used, the thickness of the vessel wall should increase exponentially as the diameter of the cylinder increases. The reasonable system would be the high-pressure cylinder with as small the diameter as possible. Therefore, only one row of High-pressure cells is provided in the diametrical direction of the high-pressure vessel. A plurality of them is provided in the longitudinal direction of the cylinder. As a result, if the installation orientation is vertical, it will have a vertically long shape. If the installation direction is horizontal, it will have the horizontally long shape. Also, in the case of wet process, both vertical and horizontal placement are possible, but in the case of dry process, only horizontal placement is possible due to restrictions on the mold.

[0181] In the case of the split sphere type with the diameter of 29 cm (corresponding volume is about 10 liters) of Non-Patent Document 2, the weight of one high-pressure cell is estimated to be about 700 Kg. Larger sizes can weigh several tons. In this case, the tensile strength of the lower mold made of elastic material is insufficient. Therefore, the elastic material cannot support the high-pressure cells. For the horizontal dry process equipment, the method of supporting the heavy high-pressure cells inside the high-pressure vessel must be considered.

[0182] The horizontal supporting method of the wet process apparatus can be any of the hanging type, the stationary type, and the sliding type. In the case of horizontal placement of the dry process equipment, the equipment is placed individually on the floor due to mold restrictions. The hanging type is also possible. In the case of the hanging type in the vertical wet process apparatus, the hanging net may be used under the lid. Also, in the case of the stationary type on the horizontal floor, if the flow path of the pressure medium is devised, it may be the stationary type of stacking separated by spacers. Table 1 summarizes the configurations that can be used for wet process and dry process, and the high-pressure cells support methods. Table 1 also describes the installation orientation of the body of the high-pressure vessel and the handling of the lid.

[0183] As the pressure medium pressurizing mechanism, the hydraulic or electric piston pressurizing device, the combination device of the electric high-pressure pump and the pressure amplifier, and the like are commercially available. Any model may be used. Hydraulic or electric piston pressure devices or reciprocating piston type pressure devices are often used when constant pressure control is desired in the high-pressure range. The maximum working pressure of the hydraulic piston pressure device reaches 700 MPa. Some electric high-pressure pumps alone reach about 100 MPa. In addition, when the pressurizing mechanism moves so that one pressurizing mechanism is shared by a plurality of high-pressure vessels as shown in FIG. 4 of the present invention, the compact and lightweight electric high-pressure pump is advantageous. An example of a combined device of the electric high-pressure pump and the pressure amplifier is the two-stage discharge type electric pump MP-75 (55 Kw, maximum operating pressure 70 MPa) manufactured by Riken Company. There is also the ultra-high pressure hydraulic booster IRE-10K-46 (maximum secondary pressure is 1000 MPa).

TABLE-US-00001 TABLE 1 Classification Quantity per Complicated Support method of processing Orientation container handling Hanging stationary sliding Wet Vertical 3-5 pieces complicated x Wet Horizontal 3-10 pieces Somewhat complicated Dry Horizontal 3-10 pieces simple x explanatory notes : preferable, : less favorable, x: not feasible

Example 2

[0184] In Example 2, the type and physical properties, and the viscosity and compressibility under high pressure of the pressure medium will be described. In the high-temperature and high-pressure processing of the present invention, pressure is applied by hydrostatic pressurization, so the pressure medium must have a certain degree of heat resistance. The internal heating source that heats the processed material to 1300-1500 C. is in the high-pressure cells. The present invention is based on the idea of controlling the pressure inside the high-pressure vessel by measuring and controlling the temperature. Therefore, the pressure medium to be used must be the liquid fluid whose compressibility due to pressure and volume change rate or volume expansion rate due to temperature are known.

[0185] The first target for the high-temperature side use temperature (maximum use temperature) of the pressure medium used in the present invention is 250 C. The reason for this is that the elastic material used in the high-pressure vessel has the heat resistance limit. If the stretchable material with high heat resistance such as the composite material is developed, the next target is to raise the temperature to 300 to 400 C. as necessary. As a result, the pressurization performance due to thermal expansion of the pressure medium is further enhanced. In addition, the required pressure cannot be unconditionally determined only on the pressure medium side. This is because the working pressure correlates with the boosting effect which is proportional to the size of the high-pressure cells. Higher pressure limits are required to apply to larger size diamond synthesis. Therefore, the withstand pressure limit of high-pressure equipment such as high-pressure vessels and press frames is set at 1 GPa. As the first target, the performance of the pressurizing mechanism is set to 500 MPa, which is in the prior art. The multi-anvil, such as the segmented sphere type high-pressure cells, has the pressure multiplication factor of 10 to 100 times. Therefore, the high-pressure cells have the multi-anvil structure in order to reliably obtain the working pressure of 5 GPa required for diamond synthesis. With these, the present invention is directed towards the production of larger size synthetic diamonds. After the pressure is increased to 500 MPa by the pressurizing mechanism, the volume is expanded by heating the pressure medium to maintain the high pressure. After that, the pressure is further increased to about 700 MPa. This is the value that is acceptable for high-pressure parts such as valves that are currently available. This allows synthetic diamonds to be produced in larger sizes.

[0186] Candidates for the liquid pressure medium that can be used under the above temperature and pressure conditions are as follows, and their physical properties are shown in Table 2. Candidates are toluene, ethanol, methanol, benzene, and acetone. In addition, water, which is often used as the pressure medium in the prior art, is added to Table 2. These organic solvents may be mixed together or used as the mixed liquid with water.

[0187] On the other hand, if the type of pressure medium is selected, machine oil or synthetic oil may be used as in Non-Patent Document 2. However, these are known to be difficult to use even at room temperature. Rolling oil, base oil (base material for oil and grease), and alkyl naphthalene and alkylbenzene, which are synthetic oils, solidify at about 300 MPa. Gasoline engine oil and gear oil solidify at 500-700 MPa. Since poly--olefin does not solidify up to 1200 MPa, it may be possible to use it if its characteristic values such as compression rate and expansion rate are obtained. However, these oils may pollute the surroundings and make them oily.

Therefore, it should be noted that handling such as decontamination is difficult.

[0188] In addition, since silicone oil generally has the high compressibility due to pressure, attention should be paid to each type when using it for the purpose of the present invention. For example, dimethyl silicone oil has the volumetric shrinkage of about 15% under the pressure of 350 MPa at room temperature. These are commonly used as loose liquid springs. When the device is used in pressure-first mode, and the pressure medium is pressurized prior to heating, the pressure medium compresses significantly. Subsequent heating with the internal heating source may cause the pressure medium to undergo an unexpected volume expansion. The reason is that the pressure medium in the high-pressure vessel has the mass larger than expected. Therefore, dimethyl silicone oil is not highly applicable to the pressure medium of the present invention.

TABLE-US-00002 TABLE 2 Item Physical property value specific melting Thermal volumetric Name of density heat point conductivity expansion substance (g/cm.sup.2) (J/kg C.) ( C.) (W/m/K) (10.sup.3/K) water 0.998 4,182 0.00 0.673 (80) 0.21 toluene 0.878 1,679 94.99 0.119 (80) 1.07 ethanol 0.789 2,416 114.50 0.150 (80) 1.08 methanol 0.793 2,470 97.78 0.186 (60) 1.19 benzene 0.879 1,738 5.50 0.137 (50) 1.22 acetone 0.791 2,160 94.82 0.146 (60) 1.43 Note 1) The physical properties in the table above are measured under normal pressure and at a temperature of 20 to 25 C. Note 2) Values in parentheses indicate measured temperatures ( C.) Note 3) The coefficient of expansion of water is highly dependent on temperature, reaching 0.0018/K at 220 C. Reference) Rika Chronology 2021, p. Physics 27, Physics 53, Physics 54, Physics 62, Physics 65

[0189] It is well known that the viscosity of liquids increases under high pressure. In the pressure vessel under high pressure, the liquid flow is different from that under normal pressure. When the viscosity of the liquid increases, the flow of the pressure medium in the high-pressure vessel becomes stagnant, and there is the tendency for the portion with the high temperature to occur locally. If there is the heating source or cooling mechanism in the high-pressure vessel, this tendency becomes stronger. Therefore, when measuring and controlling temperature, this point must be taken into consideration. The principled solution to this problem is the thermosiphon mechanism. First, the pressure dependence of the viscosity (m Pa.Math.s) of the liquid used as the pressure medium and the temperature dependence of the part thereof are shown. Table 3 shows the viscosities of the candidate liquids for the pressure medium under high pressure registered in the Japanese National Institute of Advanced Industrial Science and Technology (AIST) Distributed Thermophysical Property Database. Table 3 shows the reported viscosities of the liquids under measured pressures from 0.1 to 400 MPa, with the measured temperatures given in parentheses in the table. Reported temperatures range from 10 to 160 C. In addition, information on a plurality of experimental reports is registered in this database. Therefore, due to differences in data acquisition conditions among experiments, numerical values such as measured pressure are slightly different. Therefore, in this specification, Table 3 is used for the purpose of grasping the global pressure/temperature dependence of viscosity.

[0190] At 400 MPa at the same temperature in Table 3, the viscosity of methanol is about twice and that of ethanol is about four times as high as under normal pressure conditions. In the case of toluene, the viscosity at 200 MPa does not change much compared to that under normal pressure. Conversely, the viscosity of benzene at 400 MPa is about half of that under normal pressure. That is, depending on the type of substance, the viscosity at 400 MPa is 0.5 to 4 times higher than that under normal pressure.

[0191] Numerical values including temperature conditions in parentheses should be examined in detail in Table 3. The viscosities of substances other than benzene decrease by half when the temperature rises from room temperature to 75 to 160 C. Conversely, benzene is the only substance whose viscosity increases two to three times when heated.

TABLE-US-00003 TABLE 3 Viscosity at each pressure (mPa .Math. s) and its temperature dependence Substance Pressure name 0.1 MPa about 100 MPa about 200 MPa about 400 MPa water(ref.) 1.00 (25) 1.53 (15) 1.46 (15) 1.67 (15) 1.27 (20) 0.60 (47) 0.45 (67) 0.29 (107) 0.21 (147) toluene 0.58 (25) 1.18 (25) 0.52 (30) 0.42 (50) 0.70 (75) 0.39 (75) ethanol 1.20 (25) 2.00 (30) 2.60 (30) 5.00 (30) methanol 0.61 (25) 1.27 (10) 1.63 (10) 2.42 (10) 0.87 (30) 0.99 (30) 1.54 (30) 0.67 (50) 0.82 (50) 1.08 (50) benzene 0.60 (25) 0.66 (75) 0.44 (75) 0.33 (75) 1.11 (120) 0.70 (120) 0.51 (120) 1.78 (160) 1.50 (160) 1.03 (160) acetone 0.310 (25) Note 1) Values in parentheses indicate measured temperature ( C.) Reference) Japan Institute of Advanced Industrial Science and Technology (AIST) distributed thermophysical property database.

[0192] In Table 3 the viscosity of the liquid under high pressure should be considered further. Assuming the pressure (500 MPa) and temperature (250 C.) conditions of the pressure medium of the first target of the present invention, the pressure/temperature dependence is as follows. These are slightly different for each substance. However, the amount of increase is within about 0.5 to 2 times the viscosity at normal temperature and normal pressure. Its viscosity is expected to be about 1 m Pa s. That is, the viscosity of the pressure medium temporarily increases under high pressure but decreases with heating. This means that under the operating conditions of the present invention, the viscosity is approximately the same as that of water at normal temperature and normal pressure. Temperature measurement and control are relatively easy if the viscosity is about the same as that of water at normal temperature and normal pressure. However, the operation mode at startup does not have to be the complete boost-first type. The operation mode at the time of start-up should also simultaneously raise the temperature constantly. These measures are necessary for implementation. Even so, the decrease in viscosity due to the high pressure does not hinder the measurement and control of the temperature of the pressure medium. In other words, driving and control will not be lost.

[0193] Under high pressure, the liquid is compressed to some extent. In the present invention, the pressure medium should have the volume expansion ratio at the temperature (250 C.) used as the processing condition that is greater than the compression ratio at the applicable pressure (500 MPa). Therefore, the volume expansion coefficient of the liquid depending on the temperature is as shown in Table 2, and the compressibility (1E-9/Pa) of the liquid due to pressure is shown in Table 4. Note that(blank) in Table 4 indicates that no compression rate was found in the data published in Rika Chronicles 2021. No figures were found for organic solvents. However, in the case of organic solvents, among compounds having the same number of carbon atoms, compounds with a greater degree of freedom in intramolecular rotation have a greater compressibility. According to this, the order of compressibility is linear compound>side chain compound>monocyclic compound>fused ring compound. In addition, among monohydric alcohols, the shorter the chain length, the more easily compressible. That is, according to this principle, the compressibility of ethanol, benzene, etc., for which data on compressibility of 500 MPa was not found, is theoretically equivalent to or lower than that of methanol. These viscosities are not much larger than the 2E-10/Pa of methanol.

TABLE-US-00004 TABLE 4 pressure Compressibility for each pressure (1E9/Pa) substance 0.1 500 1000 name MPa MPa MPa water 0.36 0.18 0.12 toluene 0.9 0.22 ethanol 1.11 methanol 1.23 0.21 benzene 0.95 acetone 1.26 0.21 Note 1) All measurement temperatures are 20 C., Reference) Rika Chronicles 2021, p. Physics 35

[0194] Table 5 shows the results of comparing the compression rate (%) and the expansion rate (%) of the pressure medium in the liquid state under high pressure. The compression rate (%) was calculated from the compression rate of each pressure (0.1, 100, 200, 500 MPa) reported in Table 4 and the like. The expansion ratio was calculated by multiplying the expansion coefficient of the physical property by the temperature (100 and 250 C.). In the present invention, the expansion rate at least at 250 C. should be greater than the compression rate at 500 MPa. The Compression column in Table 5 indicates the compression rate (%). Those at 0.1 MPa and 500 MPa were calculated from the liquid compressibility (1E-9/Pa) by the pressure in Table 4. For 100 MPa and 200 MPa, the values read from the figure of the reference in the lower column of the table were quoted. The quoted values are shown in brackets. Also, the compressibility of ethanol, benzene, etc. is considered to be about the same as that of methanol. Also, the compressibility does not exceed 15% at 500 MPa. Furthermore, its compression rate is generally about 11% or less. Therefore, the values <11% are also shown in the table here. The expansion column in Table 5 shows the calculated value of the expansion rate (%) calculated from the volume expansion coefficient of the liquid depending on the temperature in Table 2.

TABLE-US-00005 TABLE 5 expansion Physical compression property Calculated evaluation Calculated value (Literature value) value value Applicability pressure Expansion Expansion as single Compression rate (%) rate rate pressure substance 0.1 MPa 100 MPa 200 MPa 500 MPa (10.sup.3/K) at 200 C. medium Water(ref.) 0.4% (4%) (8%) 9.0% 0.21 3.8% low toluene 0.9% 11.0% 1.07 19.3% high ethanol 1.1% (7%) (11%) <11% 1.08 19.4% high methanol 1.2% (8%) 10.5% 1.19 21.4% high benzene 1.0% <11% 1.22 22.0% high acetone 1.3% 10.5% 1.43 26.7% high Note 1) Refer to Table 4 for the compression rate (1E9/Pa) of the calculated value of the compression rate. Note 2) The coefficient of expansion is shown in Table 2, and the starting temperature is assumed to be 20 C. Note 3) The numbers in parentheses in the table above are the numbers read in FIG. 2 of Citation 1. Citation 1) Kaoru Makita, Pressure effect on thermophysical properties of organic liquids, Thermophysical Properties, Vol. 1, No. 1 (1987).

[0195] According to Table 5, the expansion rate of organic solvents such as toluene, ethanol, methanol, benzene, and acetone at 250 C. is about 20% or more. Usually, the compression rate does not exceed 15% at 500 MPa. The compression ratio will generally be about 11% or less. Therefore, they alone satisfy the requirements of the pressure medium of the present invention. However, at 150 C., the expansion rate approaches approximately 15%. Therefore, more precise data are required for use at lower temperatures.

[0196] Certainly, water, which is the pressure medium frequently used in the prior art, has an expansion rate of 3.8% when used alone. Water has a compression ratio of 9.0%. For this reason, water does not meet the pressure medium requirements of the present invention. However, organic solvents such as ethanol, methanol and acetone are soluble in water. If the mixed liquid of these organic solvents and water is used as the pressure solvent, the compressibility can be freely selected according to the mixing ratio, as is widely known. FIG. 10 compares the compressibility at 100 MPa of pure alcohol substances such as ethanol and methanol (FIG. 2 in FIG. 101 and alcohol solutions with low alcohol concentration (FIGS. 8A to 8C in FIG. 10). There are no peculiarities except for the presence of a concave portion where the compressibility is minimal in the region of the low alcohol concentration around mole fraction of 0.1 (mol/mol). The compressibility of the mixture increases almost proportionally as the alcohol concentration increases and approaches the compressibility of the pure substance of alcohol. Therefore, the compressibility can be freely set by the liquid mixture of the water-soluble organic solvent and water.

[0197] In conclusion, the flow of the invention is as follows. First, the temperature of the pressure medium is measured. Heating and cooling functions then control the temperature of the pressurized solvent. Based on this, pressure control is realized by volumetric expansion with pressure multiplication due to heat. This pressure solvent can be selected from toluene, ethanol, methanol, benzene, acetone, etc., and mixtures of these organic solvents. For water-soluble substances such as ethanol, methanol, and acetone, mixed liquids of these organic solvents and water can be selected.

Example 3

[0198] In Example 3, the Fluid-Proof [Heat-Resistant] Elastic Material used in the mold will be described. Table 6 shows the names of candidate materials for the following parts of the present invention, their properties such as tensile strength, elongation, heat resistance temperature and melting point, and their applicability. Target parts are the following stretchable parts. One is the heat- and fluid-resistant elastic seal in the pressure medium contact type (wet process). Another one is the mold such as the upper mold and the lower mold of the pressure medium non-contact type (dry process) processing apparatus. Even in the case of general elastic materials, the following materials can be applied to the present invention. These are silicone rubber with the maximum heat resistance of 280 C. and fluor rubber with the maximum heat resistance of 300 C. The maximum heat resistant temperature is hereinafter referred to as heat resistant temperature. Here, the heat resistance temperature means the deflection temperature under load. Ethylene-vinyl acetate rubber has the heat resistant temperature of 200 C., which is slightly inferior in performance. In addition, the following materials have high heat resistance and high elongation, so they have high applicability. These are tetra-fluor-ethylene/hexa-fluor-propylene copolymer (FEP), tetra-fluor-ethylene/per-fluor-alkoxy-ethylene copolymer (PFA), and poly-tetra-fluor-ethylene (PTFE), which are heat-resistant fluorine resins. The shape of the molding die is the hollow cylinder or the 2- to 4-part split mold using the heat-resistant elastic material. Refer to Patent Document 6 for its specific shape and structure. However, among general elastic materials (values of heat resistance temperature ( C.) is given in parentheses), the following materials are difficult to use in the present invention. These are natural rubber (120), isoprene rubber (120), nitrile rubber (130), ethylene-propylene rubber (150), neoprene (130), urethane rubber (80). These are difficult to use in the present invention because the heat resistance temperature does not exceed 250 C., which is the intended operating temperature for the pressure medium.

[0199] Furthermore, thermosetting resins are difficult to use. However, among heat-resistant engineering plastics called super engineering plastics, there are also thermoplastic resins that can be applied to the present invention. When the thermoplastic resin is used, there is no problem with plastic deformation as long as it exceeds the heat resistance temperature by about 30% as long as the temperature is below the melting point. The reason for this is that the shape of the processed material is rather well-fitted, and wrinkles do not occur during evacuation. In the rightmost column of Table 6, applicability to the present invention when the elastic material is used alone is evaluated. Those having a heat resistance of less than 200 C. or having an elongation of less than 100% were judged to have low applicability. If the heat resistance is less than 250 C. or the elongation is less than 150%, the applicability is evaluated as moderate. Those having the heat resistance of 250 C. or more and the elongation of 150% or more were judged to have high applicability. When used alone, the higher the tensile strength, the better. However, the tensile strength was not evaluated independently because the insufficient amount can be replenished by reinforcing materials made of dissimilar materials as the composite material.

[0200] As a result, the present heat-resistant engineering plastic alone was evaluated to have medium to low applicability to the present invention from the viewpoint of elongation. However, poly-ether-ketone (PEK), polyimide (PI), poly-benzo-imidazole (PBI) and the like have high tensile strength and high heat resistance. Therefore, the composite material in which two or more types of resin are combined is used. That is, the composite material is formed in which these are used as reinforcing materials for the molding die and another thermoplastic resin having a large elongation is used as the sheet material for the molding die. This increases the applicability of heat-resistant engineering plastics to the present invention. For the upper molded body, the hollow cylinder with the central hollow portion or the 2- to 4-part mold is used, but the manufacturing method is preferably injection molding into the mold.

TABLE-US-00006 TABLE 6 Heatproof Unit applicability Material Type of elastic Tensile strength stretch temperature melting point of elastic name material (MPa) (%) ( C.) ( C.) materials NR natural rubber 3-30 100-1000 120 low NBR synthetic rubber 5-25 100-800 130 low Si synthetic rubber 4-10 50-500 280 high EVA synthetic rubber 7-20 100-600 200 medium FKM synthetic rubber 7-20 100-500 300 high FEP Thermoplastic, C. 20-30 300-350 200 246-280 high PFA Thermoplastic, C. 25-35 200-450 260 280-310 high PTFE Thermoplastic, C. 20-35 200-400 260 327 high PPS Thermoplastic, C. 80 50 230 290 low PEK Thermoplastic, C. 100 60~150 260 373 medium PEEK Thermoplastic, C. 100 60 250 343 low PI Thermoplastic, (Note 2) 115 100 400 medium PAI Thermoplastic, Am 186 15 230 low PES Thermoplastic, Am 84 80 230 low PBI Thermoplastic, Am 130 30 427 low Abbreviations Note) NR: Natural rubber, NBR: Nitrile rubber, Si: Silicone rubber, EVA: Ethylene/vinyl acetate rubber, FKM: Fluor rubber, FEP: Tetra-fluor-ethylene/propylene hexafluoride copolymer, PFA: Tetra-fluor-ethylene Fluorinated ethylene/per-fluor-alkoxy-ethylene copolymer, PTFE: poly-tetra-fluor-ethylene, PPS: poly-phenylene sulfide, PEK: poly-ether-ketone, PEEK: poly-ether-ether-ketone, PL: polyimide, PAI: poly-amide-imide, PES: poly-ether-sulfone, PBI; Poly-benzo-imidazole, C: crystalline, Am: amorphous Note 1) The heat resistance temperature in the above table basically indicates the deflection temperature under load as the maximum heat resistance temperature, but various values have been reported. (Note 2) Polyimide (PI) is basically crystalline, but it is sometimes classified as amorphous due to its slow crystallization rate. Note 3) But here, Ketones are generally hard and have low elongation, but the elongation value of poly-ether-ketone (PEK) is an estimated value.

Example 4

[0201] In Example 4, the heat-resistant penetrating tube and the foldable vacuum exhaust port will be described. These are placed in the central cylindrical portion of the upper mold of the dry process equipment.

[0202] The heat-resistant penetration tube of the present invention penetrates the upper mold and has a heat resistance that matches the working temperature of the pressure medium (eg, 250 C.). This heat resistant penetration tube houses the power and measurement leads. In addition, the cooling water piping (inlet and outlet) of the high-pressure cells is accommodated as necessary. This heat-resistant penetrating tube can maintain its shape even under working pressure (for example, 1 GPa). This is due to the inherent strength of materials and structures that maintain their shape.

[0203] On the other hand, the vacuum exhaust port is not expected to maintain its shape at the working pressure, and a foldable vacuum exhaust port with the following roles is installed. It has the larger diameter than the heat-resistant feed-through tube that passes through the upper mold during vacuum suction prior to high-temperature and high-pressure processing. This diameter ensures the flow path for the atmosphere (gas). The conditions of use are normal temperature and pressure from vacuum to near normal pressure. Furthermore, this vent does not affect the ability of the upper mold to provide isotropic pressure under hydrostatic pressurization.

[0204] At first glance, it may seem that the heat-resistant penetrating tube and the folded-type vacuum exhaust port require contradictory performance. However, these can satisfy the requirements of the present invention by forming coaxial composite structures having different functions inside and outside.

[0205] The heat-resistant penetrating tube allows pressure-resistant power supply and instrumentation lead wires to pass through the hollow part. Also, the cooling water pipe having the large wall thickness is passed through the hollow portion. Therefore, the thick metal pipe with high strength is preferable. The extra space between the lead wire and the thick-walled pipe is densely filled with metal powder such as stainless-steel powder to form the solid pipe to ensure greater strength. If there is no dimensional leeway in arranging the heat-resistant penetration tube in the lid or upper mold of the high-pressure vessel, the heat-resistant penetration tube is made of pure titanium or the titanium alloy with high strength. For thicker pipes, the solid titanium round bar is drilled. Piping materials made of titanium comply with JIS H4635 or JIS H4650 TB340.

[0206] The strength of the folded-type vacuum exhaust port is supported by the constant value slightly stronger than the vacuum pressure resistance. This secures the space of the hollow portion outside the heat-resistant penetrating tube in the center of the upper mold. For example, the folded-type vacuum exhaust port has the structure comprising the metal mesh tube made of the wire material such as the titanium alloy woven into the mesh to form the spring and the outer cylinder made of the thin heat-resistant elastic material. This secures the space in the central hollow portion of the upper mold. The supporting material in the central hollow part of the upper mold is called the metallic net spring pipe. This metallic net spring pipe has the shape like the stent that is widely used for medical purposes. However, the folded-type vacuum exhaust port is slightly different in that it uses the slightly thicker wire to increase the spring force a little, so that it can maintain its shape to some extent during vacuum suction.

[0207] Medical stents are made of stainless steel or titanium alloy and are several centimeters long. Stents have been widely used for medical purposes such as coronary artery, biliary, esophageal, large intestine, and intracranial artery dilatation operations, and currently exist in various diameters. The shapes of coronary stents are classified into tube type, coil type and mesh type. In addition to stainless steel, tantalum or nickel-titanium alloys are used for the frame material. Shape-memory nickel-titanium alloy stents are expanded by body temperature when placed in the deflated state. This shape memory alloy stent has a certain level of spring force and is therefore relatively close to that of the present invention.

[0208] The stent made of the shape memory alloy was invented more than 30 years before the present invention, but at present there is no specification or standard for its material or manufacturing method. In addition, even today, medical stents themselves are subject to difficult requirements such as installation position accuracy, deployment performance at the target position, adhesion to walls, and the like. Medical stents are manufactured by repeating numerical analysis and prototyping for each of the numerous combinations of design conditions. On the other hand, the required performance of the metallic net spring pipe for the folded-type vacuum exhaust port of the present invention is clear. In addition, it can be installed visually.

[0209] Compared to medical stents, the shape and structure are similar, but metallic net spring pipes are technically quite easy to design and manufacture. Therefore, as an example of the method of manufacturing the metallic net spring pipe for the folded-type vacuum exhaust port, refer to the past patent document 7, which applied for materials and the manufacturing method of the stent made of the shape memory alloy. The folded-type vacuum exhaust port conforms to the medical stent but is actually manufactured in the considerably simplified manner.

Example 5

[0210] In Example 5, the following items are explained. They are 1) the cooling jacket attached to the outer wall of the high-pressure vessel and the cooling mechanism attached, 2) the heating mechanism installed inside the high-pressure vessel, and 3) the thermosiphon structure.

[0211] The pressure regulation function receives the signal from the temperature detecting function that controls the temperature of the pressure medium within the high-pressure vessel. The temperature decrease mechanism operates when the pressure regulation function determines that the pressure should be reduced. The temperature decrease mechanism operates the refrigerant cooler to send the refrigerant to the cooling jacket outside the body of the high-pressure vessel. The returned refrigerant is cooled by the refrigerant cooler. The position where the cooling jacket is attached is determined by the thermosiphon structure, which will be described later. The refrigerant cooler is common commercial chiller equipment. The cooling capacity required by the refrigerant cooler is determined by the amount of heat generated within the high-pressure cells. This is the amount of heat of the internal heating source and the amount of heat of the heating mechanism installed in the high-pressure vessel. Since the working temperature of the pressure medium to be cooled is about several hundred degrees Celsius, the chiller device may be either water-cooled or air-cooled. Alternatively, the refrigerant may be gaseous. This gas is Freon or Freon substitute gas or the like. Furthermore, the refrigerant may be liquid.

[0212] The heating mechanism operates when the pressure regulator determines that pressure should be increased. The heating mechanism operates the pressure medium heating heater power supply to heat the pressure medium with the pressure medium heating heater installed in the high-pressure vessel. The position where the pressure medium heating heater is attached is determined by the thermosiphon structure. The pressure medium heater is the sheath heater or the resistance heater that is high pressure and liquid resistant. The required heating capacity is determined mainly by the temperature to be raised and the weight of the pressure medium in the high-pressure vessel. It should be noted that the heating of the pressure medium need not be rapid. Considering the time (for example, several days) required to produce synthetic diamond, it suffices to reach the predetermined temperature within, for example, one day. The pressure medium heating heater power supply may be of the direct current type or the alternating current type. The pressure medium heater may be the plate type, cartridge type, flexible type, or micro type heater. The heater may have the built-in thermocouple. The resistance heating element may be the metal rod (wire), graphite, SiC, or the like.

[0213] The thermosiphon phenomenon is the convection phenomenon based on the principle that heated fluid becomes lighter and rises, and cold fluid becomes heavier and descends. In general, the density of the liquid has the negative correlation with temperature, that is, the density decreases as the temperature rises. There are few reports of density data showing temperature dependence under high pressure. However, as shown in Table 5, for liquids such as toluene, ethanol, methanol, and benzene, the volume expansion effect is superior to the volume compression effect due to pressure. Even under the high pressure of 500 MPa, their densities decrease as the temperature rises. Further, as described above in Example 2, under the pressure conditions (e.g., 500 MPa) and temperature conditions (e.g., 250 C.) of the pressure medium of the present invention, the viscosity of the pressure medium of the candidate organic solvents is about 1 mPa/s. This is expected to be like the viscosity of water at normal temperature and pressure. Therefore, in principle, the pressure medium under the temperature and pressure conditions of the present invention can generate the thermosiphon due to the density difference caused by the temperature difference between heating and cooling of the pressure medium.

[0214] To generate the thermosiphon inside the high-pressure cylinder, which is the main body of the high-pressure vessel, the heating mechanism and the cooling mechanism must be arranged appropriately. Also, vertical partitions should be installed to prevent hot and cold fluid streams from intermingling. The suitable material for the partition plate is ceramic and the like, which has poor thermal conductivity. On the surface of the partition plate (support plate), the thin, elongated metal plate made of the material with high thermal conductivity such as copper or aluminum is installed over the entire length in the vertical direction. The thermocouple (TC3) for measuring the average temperature is brought into contact here to measure the average temperature of the pressure medium. The heating sources in the high-pressure vessel are the internal heater in the high-pressure cells and the pressure medium heater of the heating mechanism. These are arranged vertically in the line at the central portion (the center position of the cylinder) and the bottom portion (the lower end of the cylinder) on the central axis. The cooling jacket of one of the cooling mechanisms is arranged in the range from the center to the upper half of the outer wall of the high-pressure cylinder. This system heats the lower end and center of the central portion of the high-pressure cylinder and cools the upper half of the outer wall. As a result, a thermosiphon is formed in which the heated fluid rises in the central portion and the cooled fluid descends in the outer wall portion.

[0215] The thermosiphon of the high-pressure cylinder described above determines the maximum temperature at the position where the temperature in the high-pressure vessel should be the highest and the minimum temperature at the position where it should be the lowest. The average temperature of the pressure medium is obtained by measuring the copper plate attached vertically on the partition plate (support plate) for average temperature measurement. This copper plate is the elongated high thermal conductive metal plate like the wire. This copper plate may be installed by rotating the partition plate once in the vertical direction.

[0216] However, if the initial heating degree after starting the apparatus is small, the measured temperature tends to indicate various erroneous values (variation). The reason for this is that heat transfer depends only on heat conduction in the pressure medium, so there is no fluid movement due to thermal convection. Also, it should be noted that if there is abrupt heating or cooling in the middle, the measured temperature will fluctuate for the while. When the certain degree of heating is exceeded after the passage of time from the start of heating, the fluid begins to circulate due to heat convection. After that, the rotation direction of the fluid is maintained, so the measured temperature is stabilized. The flow rate depends on the degree of heating, and if the degree of heating is constant, the flow is steady. This stabilizes the measured temperature.

[0217] On the other hand, since the present invention uses hydrostatic pressurization in principle, the pressure of the pressure medium is not localized. Therefore, the pressure is the same at any position in the high-pressure vessel. Considering the purpose of pressurizing the pressure medium by thermal volume expansion of the pressure medium according to the present invention, the information on the numerical value of the temperature unevenly distributed locally in the pressure medium is not so important. That is, it suffices to know the average representative temperature.

[0218] Therefore, in the case of the configuration of the present invention, the average temperature (TC3) is used as the representative temperature during steady operation. However, the average temperature fluctuates at the start of operation or during sudden heating or cooling. Therefore, when obtaining the representative temperature, logical determination is made by taking into consideration the information of the maximum temperature (TC1) and the minimum temperature (TC2), which have the small range of variation. The representative temperature at the time of start-up, rapid heating or cooling is information that can be easily clarified empirically. This information can be input to the condition judgment function of the control device that reflects the empirical rule.

[0219] Vertical arrangement is possible for the wet process. However, the distance between the rise of the hot fluid and the descent of the cold fluid of the thermosiphon described above is increased. As a result, the sensitivity of temperature measurement and control of the pressure medium becomes dull even in the steady state. Therefore, in addition to the above-described three temperature measurement points, the number of measurement points may be increased in the vertical direction. However, in that case, the monitoring and management will take time and effort.

[0220] In the horizontal arrangement, both the ascending and descending distances are short. This is the same for dry process and wet process. Therefore, there is no problem that monitoring and managing the temperature of the pressure medium requires time and effort. However, when many High-pressure cells are installed in one high pressure vessel, the ambient environment conditions are different. For example, one is the mutual influence of the difference in the amount of heat generated by the internal heat sources of the High-pressure cells installed in the periphery and the center of the horizontal arrangement. Another is the difference in the outer surface area where the high-pressure cylinder is allowed to cool. Therefore, to obtain a more stable steady state, each high-pressure cells should have three temperature measurement points. Therefore, the heating mechanism and cooling mechanism should be controlled separately.

Example 6

[0221] As described in Example 2, the first target for the design pressure limit of the high-pressure equipment such as the high-pressure vessel and the press frame was set to 1 GPa. To utilize this, physical property data such as the compressibility of the pressure medium in the pressure range of 400 MPa or higher should be obtained. These physical property data can be obtained with the DAC device, or the like attached to the side of the device. On the other hand, the maximum working pressure of the available pressure medium is influenced by the pressure limit of high-pressure components such as high-pressure valves attached to the high-pressure piping. DAC is manufactured and sold by Shimizu Seisakusho in Japan.

[0222] In the case of the configuration of the present invention, the displacement of the pressure medium is reduced under high pressure. Therefore, the high-pressure pipes are thin, and the size of the high-pressure parts to be used is also small. According to catalog products of domestic manufacturers, the pressure resistance limit of high-pressure parts is limited to 20 to 70 MPa. These are used in power plants. However, in the ultra-high-pressure area, the European company BUTECH (the Japanese distributor is Sunny Trading Co., Ltd.) supplies various high-pressure specification products. The partition valves (two-way valves and three-way valves) with a withstand pressure limit of about 1 GPa are already on the market as catalog products. Its material is SUS316. The model number is 150V51-316WP for the 2-way valve and 150V53-316WP for the 3-way valve.

[0223] On the other hand, as the check valve, the ball type check valve with the spring is sold. Its model number is 60BC9-316WP-316S. However, this pressure resistance limit is several hundred MPa, which is insufficient for use in the present invention. The manufacturer states that it can be changed if the material can be machined. Alternates are Hastelloy, Inconel, Titanium, ALLOY 400, and the like. As an option, products with pressure resistance limits up to 1,034 MPa are available. Additionally, it can be changed to a titanium alloy whose tension is about three times that of pure titanium. The titanium alloy is, for example, Ti-6A1-4V corresponding to ASTM Grade 5 or Ti-10V-2Fe-3Al corresponding to AMS4983.

[0224] Check valves are often of the ball type. In addition, there are types such as disk type, swing type, wafer type, and lift type. Also, the disk type and the ball type are spring equipped. Those with springs are the same size as piping parts such as nipples and reducers. On the other hand, other valves are of the large size having the water chamber with the valve body in the flow path, like globe valves, gate valves, relief valves (safety valves), and the like. Also, due to the high working pressure, the water chamber (casing) and the valve support must have great strength. These types result in large, forged valves. There are no technical problems in designing and manufacturing these. Depending on the situation, it may be necessary to install the custom-designed giant forged valve. However, check valves that are reinforced by wrapping piano wire around the outer periphery of existing catalog products can also be used. Alternatively, the spring-loaded ball type check valve described above, which is made of the different material, can also be used.

Example 7

[0225] Example 7 describes the high-pressure cells. Each high-pressure cell has the anvil, the processed material, the internal heating source, and the internal thermocouple for temperature measurement. The internal heating source may have the built-in thermocouple. Current and instrumentation leads for the internal heating source and internal thermocouple are exposed from the high-pressure cells. These wires connect to external connectors. Cooling water piping (inlet/outlet) is exposed from the high-pressure cells as required. These pipes connect to external industrial water or tap water. In wet process, each high-pressure cell is wrapped with the heat- and fluid-resistant elastic seal. In dry process, the high-pressure cells are directly placed in the mold. The present invention relates to the pressurizing device for manufacturing synthetic diamond. Therefore, the type and structure of the high-pressure cells are not requirements, except the material of the internal Anvil made of ultra-hard material. Any shape may be used if the high-pressure cells have the symmetrical shape. Examples of such shapes are spherical, hexahedral (cubic), and octahedral. Note that the belt-type high-pressure cell is out of the scope of this description because it does not have the symmetrical shape.

[0226] For example, the segmented sphere type high-pressure cells of the conventional hydrostatic pressurization device (BARS device) for academic research shown in FIG. 1 may be used as it is. The range to be used is the portion of the structure inside the oil layer of the drive oil. In addition, the cube type (cubic type anvil) used in the CCP apparatus described in the above Background of the invention may be used as it is. Furthermore, the regular octahedral shape such as the internal Anvil described in the above Background of the invention may be used as it is.

[0227] However, the temperature of the pressure medium rises due to heat transfer from the internal heat source of the high-pressure cells. For application in the present invention, it is necessary to consider the temperature rise of the pressure medium and to control the temperature by heat transfer.

[0228] In the production of synthetic diamond, the processed material must be heated to 1300-1500 C. As such, the internal heating source is in the internal anvil of the high-pressure cells. The BARS device of FIG. 1, described in the Background of the invention section, uses tungsten carbide (WC) for its internal anvil, which has good thermal conductivity. After a few days of operation, the BARS device experienced an increase in the temperature of the oil acting as the pressure medium until the working pressure of the hydraulic pump and the processed material became uncontrollable. Ultimately, the device solved the problem by running cooling water across and across the high-pressure cells to remove heat from the internal heating source. That is, the cause of the uncontrollable pressure rise in the BARS device is considered as follows. 1) the internal anvil has good thermal conductivity, 2) the volume and mass of the oil layer, which is the pressure medium, was small, and 3) there was no mechanism to control the pressure in the first place. In the present invention, solutions for the above 2) and 3) have already been presented. The first explanation is 1) setting the thermal conductivity of the inner anvil and the temperature control method using it.

Example 8

[0229] The super hard materials used for the internal Anvil of the high-pressure cells include those made of metal and those made of ceramic. Metal ones include cemented carbide (WC+Co), tungsten (W), and the like. Those made of ceramics include zirconia (ZrO2), silicon nitride (Si3N4), cermet, boron carbide (B4C), silicon carbide (SiC), and the like. Table 7 shows the thermal conductivity of cemented carbide materials whose Vickers hardness (Hv) is comparable to that of cemented carbide. As shown in Table 7, metal ones have high thermal conductivity, and ceramic ones other than silicon carbide (SiC) have low thermal conductivity.

TABLE-US-00007 TABLE 7 Vickers Coefficient melting hardness of thermal Thermal Material point Hv expansion conductivity abbreviation ( C.) (N/mm.sup.2) (10.sup.6/K) (W/mK) metal ceramics ZrO.sub.2 2715 1400 9.5 3 Si.sub.3N.sub.4 2173 1800 3.4 20 SM 1700 1800 8.3 27 B.sub.4C 2400 3000 4.7 30 WC + Co 2800 1700 6.0 85 SiC 2173 2300 4.7 90 W 3380 1900 4.5 177 Abbreviated note) ZrO.sub.2: zirconia, Si.sub.3N.sub.4: silicon nitride, SM: cermet, B.sub.4C: boron carbide, WC + Co: cemented carbide, SiC: silicon carbide, W: tungsten note) Characteristic values are normal temperature values.

[0230] In the present invention, heating of the processed material by the internal heating source is started at the same time as the pressure is increased by the pressurizing mechanism. To increase the pressure beyond the maximum pressure determined by the performance of the pressurizing mechanism, the pressure medium is thermally expanded by increasing the temperature to obtain the higher pressure.

[0231] In order to increase the temperature rise rate of the pressure medium, that is, the pressure increase rate, the super hard material of the anvil in the high-pressure cells should be the material with high thermal conductivity. Those shown in Table 7 are cemented carbide, silicon carbide, tungsten, or materials based on these.

[0232] On the other hand, to slow down the rate of pressurization of the pressure medium, the super hard material of the anvil in the high-pressure cells should be the material with low thermal conductivity. Shown in Table 7 are low zirconia, silicon nitride, cermet, boron carbide, or materials based on these. As a result, the influence of the internal heating source can be eliminated as much as possible.

[0233] In the present description of the present invention, pressure medium contact type (wet process) and pressure medium non-contact type (dry process) are described mixed in the same document. So, each entry should indicate which one it belongs to. Table 8 shows the function and configuration of the high-temperature and high-pressure processing equipment containing two or more High-pressure cells described above, and the correspondence relationship between wet process and dry process.

TABLE-US-00008 TABLE 8 Functions and configuration of high- Pressure pressure temperature and high-pressure medium medium processing equipment using liquid contact non-contact medium hydrostatic pressurization type type containing two or more high- (Wet (Dry No pressure cells processing) process) 1) High-pressure vessel, press frame, pressure mechanism 2) Liquid pressure medium with known compression and expansion coefficients 3) Pressure medium heater, cooling jacket 4) Arrangement of Vertical/suspension 5) high-pressure Horizontal/stationary 6) vessel and support Horizontal/Sliding system of high- pressure cell 7) Heat and fluid resistant elastic seal 8) A pair of molds (upper and lower) and guide mechanism 9) Heat-resistant penetrating tube, metal mesh spring tube 10) Gravity type pressure medium adjustment tank 11) Types of high-pressure cells (Sphere, hexahedron, octahedron) 12) Thermal convection of pressure medium by thermosiphon 13) Partition plate (support plate), average temperature measurement copper plate 14) Temperature measurement (maximum, minimum, average) and control 15) Check valve with detachable pressure mechanism 16) Shared pressurization mechanism by multiple high-pressure vessels explanatory notes : correlated, : slightly correlated, : no correlation

[0234] In the above description, the high-temperature and high-pressure processing apparatus of the liquid medium pressurization type was explained as the apparatus for producing large-sized synthetic diamonds. However, the material produced by the apparatus need not be limited to large size synthetic diamonds. In addition to synthetic diamonds, the following substances can be produced: cubic boron nitride (cBN) and its analogues, and ceramic materials, hard materials, intermetallic materials, and compacts thereof, including sintered products, produced using high pressure. The method of the present invention can be applied to products manufactured by this high temperature high-pressure (HPHT) manufacturing equipment.

EXPLANATION OF LETTERS OR NUMERALS

[0235] 1. Split-Type High-Pressure Vessel. [0236] 2. Split Frame. [0237] 3. External Anvil (Eight Division). [0238] 4. Internal Anvil (Six Division). [0239] 5. Current and Instrumentation Lead. [0240] 6. Pressure Medium. [0241] 7. Main Part of High-Pressure Vessel (Body). [0242] 8. Lid of High-Pressure Vessel (Lid). [0243] 9. High-Pressure Cells. [0244] 10. Pressurizing Mechanism. [0245] 11. Check Valve. [0246] 12. Slice Valve. [0247] 13. Processed Material. [0248] 14. Internal Heating Source. [0249] 15. Anvil. [0250] 16. Internal Thermocouple. [0251] 17. Connection Cable. [0252] 18. Waterproof Pressure Connector. [0253] 19. Seal of Fluid-Proof [Heat-Resistant] Elastic Material. (Heat- and Fluid-Resistant Elastic Material) [0254] 20. Binding Mechanism. [0255] 21. Source Power Supply of Internal Heating. [0256] 22. High Pressure Vessel Thermocouple. [0257] 23. Temperature Detecting Function. [0258] 24. Pressure Regulation Function. [0259] 25. Temperature Decrease Mechanism. [0260] 26. Refrigerant Cooler. [0261] 27. Cooling Jacket. [0262] 28. Heating Mechanism. [0263] 29. Hydraulic-Medium Heating Heater Power Supply. (Pressure medium heater power supply) [0264] 30. Hydraulic-Medium Heating Heater. (Pressure medium heater) [0265] 31. Partition Plate. (Support Plate) [0266] 32. Piezoelectric Sensor. [0267] 33. Press Frame. [0268] 34. Rail. [0269] 35. Movable Cart. [0270] 36. Pressurization Pump. [0271] 37. High-pressure Hose. [0272] 38. Pressure Medium Tank. [0273] 39. Lower Molding Die. [0274] 40. Upper Molding Die. [0275] 41. Upper Molding Die Mounting Jig. [0276] 42. Gravity Equation Pressure-Medium Equalizing Tank. [0277] 43. Heat-Resistant Penetrating Tube. [0278] 44. High-pressure cell Cooling Water Piping. [0279] 45. Atmospheric Escape Pipe. [0280] 46. Processing Pit. [0281] 47. Lower Support Mechanism. [0282] 48. Pressure-Medium Circulation Layer. [0283] 49. Folded-Type Vacuum Exhaust Port. [0284] 50. Vacuum Pump. [0285] 51. Lower External Anvil. [0286] 52. Upper External Anvil. [0287] 53. Notching. [0288] 54. Suction Pipe-Connection Box. [0289] 55. Decompressing Mechanism. [0290] 56. High-pressure cell of All the Edge Portion Excision Articles (All tip portions cut-off high-pressure cells). [0291] 57. Metallic Net Spring Pipe. [0292] 58. Upper Hydraulic-Medium Slice Valve. [0293] 59. Hydraulic-medium Equalizing Tank Slice Valve. [0294] 60. Atmospheric Release Valve. [0295] 61. Vacuum Pump Valve. [0296] 62. Hydraulic-Medium Atmosphere Release Valve. [0297] 63. Pressure Transmitter. [0298] 64. Press Fit Mouth of Oil Medium. [0299] 65. Copper Plate for Mean-Temperature Measurement.