Preparation method of transition metal carbide particle reinforced tantalum-based composite material

Abstract

The invention discloses a preparation method of a transition metal carbide particle reinforced tantalum-based composite material, and belongs to the field of refractory metal-based composite materials. The invention aims to solve the problems that the engineering stress is low, the deformability is weak, secondary recrystallization coarsening is easy to occur to crystal grains when the crystal grains are used at high temperature and the like, and the application of the tantalum material in the fields of high-temperature mechanical bearing and corrosion environment is limited in the traditional powder metallurgy sintering preparation of the tantalum material. The method is simple in process and high in production efficiency. The carbide particle reinforced tantalum-based composite material prepared through the technical route has the advantages of being small in grain, stable in high-temperature grain size, high in engineering stress and high in deformation elongation rate, and the problems that a traditional powder metallurgy sintering state tantalum material is low in engineering stress and difficult to deform, and grain recrystallization coarsening is caused when the traditional powder metallurgy sintering state tantalum material is used for a long time at the high temperature are effectively solved. The relative density gt of the carbide particle reinforced tantalum-based composite material; the tensile strength of the alloy is 300-800MPa, the elongation percentage is 97%, the room-temperature hardness is 1.6-3.5 GPa, the tensile strength is 300-800MPa, and the elongation

Description

Technical Field

[0001] This invention belongs to the field of refractory metal matrix composites, specifically relating to a method for preparing a tantalum matrix composite material reinforced with transition metal carbide particles. Background Technology

[0002] Tantalum is a typical example of a refractory metal, characterized by its high atomic number, high density, good ductility, and excellent corrosion resistance. It has irreplaceable applications in various fields such as aerospace, military, chemical, and nuclear industries. However, tantalum has a high melting point (2996℃), and traditional smelting methods for preparing tantalum-based composite materials are not only energy-intensive and costly, but also prone to forming coarse as-cast structures, failing to meet the requirements of practical applications and high efficiency, environmental friendliness, and energy conservation. Subsequent, energy-intensive, and complex heat treatment processes are necessary to achieve its superior engineering stress resistance, ductility, and mechanical properties. Summary of the Invention

[0003] The purpose of this invention is to solve the problems of low engineering stress, weak deformation ability, and easy secondary recrystallization and coarsening of grains in traditional powder metallurgy sintering preparation of tantalum materials, which limit the application of tantalum materials in high-temperature mechanical load-bearing and corrosive environments. The invention provides a method for preparing tantalum-based composite materials reinforced with transition metal carbide particles.

[0004] This invention addresses the problems of existing technologies by proposing a powder metallurgy sintering process to improve the microstructure, deformation capacity, and overall mechanical properties of sintered pure tantalum through the dispersion strengthening of transition metal carbide particles. Transition metal carbides possess excellent properties such as high melting point, high hardness, and extremely high thermal and mechanical stability. They are also virtually resistant to various acid and alkali chemical corrosions at room temperature. These properties make them widely used in machining, mineral mining, manufacturing wear-resistant and high-temperature components, and nuclear reactors. Common transition metal carbides include titanium carbide (TiC), zirconium carbide (ZrC), hafnium carbide (HfC), tantalum carbide (TaC), and tungsten carbide (WC). Their common characteristics include high melting points (many carbides have melting points above 3000℃), stable physicochemical properties, and good electrical and thermal conductivity. The dispersed distribution of carbide particles in the matrix refines the grains by hindering dislocation and grain boundary movement, thereby improving the overall mechanical properties of the material. Meanwhile, transition metal carbides and tantalum exhibit excellent chemical interfacial bonding strength and synergistic deformation capacity during high-temperature load-bearing processes. The transition metal carbide particle-reinforced tantalum-based composite material prepared using the technical route of this invention possesses advantages such as fine grains, uniform second-phase distribution, high engineering stress, and high elongation. The carbide particle-reinforced tantalum-based composite material has a relative density >97%, a room temperature hardness of 1.6~3.5 GPa, a tensile strength of 300~800 MPa, and an elongation of 2%~25%. Its mechanical properties are comparable to or even superior to those of traditional tantalum alloys, and it features a simple and efficient process, low overall energy consumption, and controllable microstructure and properties.

[0005] A method for preparing a transition metal carbide particle-reinforced tantalum-based composite material includes the following steps:

[0006] I. Weighing materials:

[0007] Tantalum powder and transition metal carbide powder are weighed according to a certain volume ratio to obtain the raw materials;

[0008] II. Powder Mixing:

[0009] After the tantalum powder weighed in step one is initially mixed with the transition metal carbide powder, it is ball-milled in an inert gas or vacuum environment and then sieved in an inert gas environment through an 80-320 mesh sieve to obtain a uniformly mixed composite raw material.

[0010] III. Sintering:

[0011] The uniformly mixed raw materials obtained in step two are placed in a graphite mold and sintered in a vacuum or inert gas environment to obtain tantalum-based composite materials reinforced with transition metal carbide particles of different volume fractions.

[0012] The present invention has the following beneficial effects:

[0013] I. This invention proposes for the first time a method for preparing tantalum-based composite materials reinforced with transition metal carbide particles. A three-dimensional planetary ball milling method is used to thoroughly mix tantalum powder and transition metal carbide powder to form a uniform composite powder, overcoming the challenge of uniform mixing with large density differences and small component contents. A multi-step / rapid sintering method is employed to obtain tantalum-based composite materials reinforced with transition metal carbide particles of different volume fractions. The omnidirectional planetary ball milling ensures thorough and uniform mixing of tantalum powder and transition metal carbide powder, and the control of ball milling process parameters effectively avoids adverse factors such as powder particle agglomeration, cold welding between particles, and caking. This effectively improves the uniformity of the second phase distribution, refines the grains, and promotes dense sintering.

[0014] II. The process of this invention is simple, greatly reducing the production cost of transition metal carbide particle-reinforced tantalum-based composite materials. It achieves high deformation capacity, tensile strength, and yield stress improvement in tantalum materials without traditional hot working and heat treatment processes. Simultaneously, it significantly improves the controllability of the production process, ensuring precise component ratios and material purity in the carbide particle-reinforced tantalum-based composite materials. The carbide particle-reinforced tantalum-based composite materials prepared using this invention have a relative density >97%, a room temperature hardness of 1.6~3.5 GPa, a tensile strength of 300~800 MPa, and an elongation of 2%~25%. Specifically, using zirconium carbide as the reinforcing phase, and through control of the zirconium carbide volume content and preparation process, the prepared zirconium carbide particle-reinforced tantalum-based composite material exhibits excellent comprehensive properties, including a density of 97.6%, a room temperature hardness of 1.45 GPa, a tensile strength of 485 MPa, and an elongation of 22.3%. Attached Figure Description

[0015] Figure 1 XRD patterns of zirconium carbide-reinforced tantalum-based composites prepared in Examples 1, 2, and 8 with different volume fractions;

[0016] Figure 2 SEM images of zirconium carbide-reinforced tantalum-based composite materials prepared by adding different volume fractions in Examples 1, 2, and 8. Detailed Implementation

[0017] The following embodiments are intended to further illustrate the content of the present invention, but should not be construed as limiting the present invention. Any modifications and substitutions made to the methods, steps, or conditions of the present invention without departing from the essence of the invention are within the scope of the present invention.

[0018] Specific Implementation Method 1: This implementation method provides a method for preparing a transition metal carbide particle-reinforced tantalum-based composite material, comprising the following steps:

[0019] I. Weighing materials:

[0020] Tantalum powder and transition metal carbide powder are weighed according to a certain volume ratio to obtain the raw materials;

[0021] II. Powder Mixing:

[0022] After the tantalum powder weighed in step one is initially mixed with the transition metal carbide powder, it is ball-milled in an inert gas or vacuum environment and then sieved in an inert gas environment through an 80-320 mesh sieve to obtain a uniformly mixed composite raw material.

[0023] III. Sintering:

[0024] The uniformly mixed raw materials obtained in step two are placed in a graphite mold and sintered in a vacuum or inert gas environment to obtain tantalum-based composite materials reinforced with transition metal carbide particles of different volume fractions.

[0025] Specific Implementation Method Two: This implementation method differs from Specific Implementation Method One in that the transition metal carbides mentioned in step one are titanium carbide, zirconium carbide, hafnium carbide, niobium carbide, tantalum carbide, molybdenum carbide, and tungsten carbide. The other steps are the same as in Specific Implementation Method One.

[0026] Specific Implementation Method Three: This implementation method differs from Specific Implementation Method One or Two in that the volume fraction of transition metal carbide powder in the raw materials mentioned in step one is 0.3% to 30%. The other steps are the same as in Specific Implementation Method One or Two.

[0027] Specific Implementation Method Four: This implementation method differs from Specific Implementation Methods One to Three in that the ball milling mixing process described in step two is as follows: a planetary ball mill is used, with both the mill jar and the grinding balls made of zirconium oxide. The ball-to-material ratio is (5~20):1, the mill speed is 50 r / min~500 r / min, the milling time is 12 h~48 h, and the sieving is performed through an 80 mesh~320 mesh sieve. Other steps are the same as in Specific Implementation Methods One to Three.

[0028] Specific Implementation Method Five: This implementation method differs from Specific Implementation Methods One to Four in that the ball milling mixing process described in step two is as follows: A three-dimensional planetary ball mill is used, with both the mill jar and the grinding balls made of zirconium oxide. The ball-to-material ratio is 10:1, the mill speed is 300 r / min, the milling time is 24 hours, and the sieve is an 80-mesh sieve. Other steps are the same as in Specific Implementation Methods One to Four.

[0029] Specific Implementation Method Six: This implementation method differs from Specific Implementation Methods One to Five in that the ball milling mixing process described in step two is as follows: A three-dimensional planetary ball mill is used, with both the mill jar and the grinding balls made of zirconium oxide. The ball-to-material ratio is 5:1, the mill speed is 200 r / min, the milling time is 48 hours, and the sieve is an 80-mesh sieve. Other steps are the same as in Specific Implementation Methods One to Five.

[0030] Specific Implementation Method Seven: This implementation method differs from Specific Implementation Methods One through Six in that the sintering described in step three can be spark plasma sintering. The other steps are the same as in Specific Implementation Methods One through Six.

[0031] Specific Implementation Method Eight: This implementation method differs from Specific Implementation Methods One to Seven in that the sintering described in step three is hot-pressing sintering; the hot-pressing sintering process is as follows: heating from room temperature to 1600℃~2200℃, holding at 1600℃~2200℃ for 30min~300min, then cooling to room temperature, with a heating rate of 10℃ / min~30℃ / min and a cooling rate of 10℃ / min~30℃ / min, and maintaining a pressure of 10MPa~100MPa during the sintering process. Other steps are the same as in Specific Implementation Methods One to Seven.

[0032] Specific Implementation Method Nine: This implementation method differs from Specific Implementation Methods One to Eight in that the sintering described in step three is spark plasma sintering; the spark plasma sintering process is as follows: heating from room temperature to 1600℃~2200℃, holding at 1600℃~2200℃ for 10min~60min, then cooling to room temperature, with a heating rate of 30℃ / min~150℃ / min and a cooling rate of 30℃ / min~150℃ / min, and maintaining a pressure of 10MPa~100MPa during the sintering process. Other steps are the same as in Specific Implementation Methods One to Eight.

[0033] Specific Implementation Method Ten: This implementation method differs from Specific Implementation Methods One to Nine in that the sintering described in step three can be a multi-step sintering process. The multi-step sintering process is as follows: The temperature is raised from room temperature to a range of 1000℃ to 1600℃. A holding period is set within this range for 10 to 120 minutes, maintaining a pressure of 10 MPa to 100 MPa. Then, the temperature is raised further to 1600℃ to 2200℃ and held for 30 to 300 minutes, maintaining a pressure of 10 MPa to 100 MPa. The other steps are the same as in Specific Implementation Methods One to Nine.

[0034] The beneficial effects of the present invention are verified using the following embodiments:

[0035] Example 1: A method for preparing a zirconium carbide-reinforced tantalum-based composite material (Ta-3 vol.% ZrC), comprising the following steps:

[0036] I. Weighing materials:

[0037] Tantalum powder and transition metal carbide powder are weighed according to a certain volume ratio to obtain the raw materials;

[0038] The transition metal carbide mentioned in step one is zirconium carbide;

[0039] The volume fraction of transition metal carbide powder in the raw materials mentioned in step one is 3%;

[0040] II. Powder Mixing:

[0041] After the tantalum powder weighed in step one is initially mixed with the transition metal carbide powder, it is ball-milled in a vacuum environment and then sieved in an inert gas environment to obtain a uniformly mixed raw material.

[0042] The ball milling process described in step two is as follows: an all-around planetary ball mill is used, with the grinding jar and grinding balls made of zirconium oxide, a ball-to-material ratio of 20:1, a ball mill speed of 250 r / min, and a grinding time of 24 h; the uniformly mixed composite powder is then sieved in an inert gas environment, using an 80-mesh sieve.

[0043] III. Sintering:

[0044] The uniformly mixed raw materials obtained in step two are placed in a graphite mold and sintered in an inert gas environment to obtain zirconium carbide reinforced tantalum-based composite material (Ta-3vol.%ZrC).

[0045] The sintering described in step three is hot pressing sintering; the hot pressing sintering process is as follows: the temperature is raised from room temperature to 1900℃, held at 1900℃ for 60 minutes, and then cooled to room temperature. The heating rate is 20℃ / min, the cooling rate is 20℃ / min, and the pressure is maintained at 30MPa during the sintering process.

[0046] The inert gas mentioned in steps two and three is argon.

[0047] The zirconium carbide-reinforced tantalum-based composite material prepared in Example 1 exhibits high density, uniform second-phase distribution, and uniform elemental distribution with no significant segregation. The zirconium carbide-reinforced tantalum-based composite material has a density of 97.6%, a room temperature hardness of 1.45 GPa, a tensile strength of 485 MPa, and an elongation of 22.3%, demonstrating excellent overall performance.

[0048] Example 2: A method for preparing a zirconium carbide-reinforced tantalum-based composite material (Ta-5 vol.% ZrC), comprising the following steps:

[0049] I. Weighing materials:

[0050] Tantalum powder and transition metal carbide powder are weighed according to a certain volume ratio to obtain the raw materials;

[0051] The transition metal carbide mentioned in step one is zirconium carbide;

[0052] The volume fraction of transition metal carbide powder in the raw materials mentioned in step one is 5%;

[0053] II. Powder Mixing:

[0054] After the tantalum powder weighed in step one is initially mixed with the transition metal carbide powder, it is ball-milled in a vacuum environment and then sieved in an inert gas environment to obtain a uniformly mixed raw material.

[0055] The ball milling process described in step two is as follows: an all-around planetary ball mill is used, with the grinding jar and grinding balls made of zirconium oxide, a ball-to-material ratio of 20:1, a ball mill speed of 250 r / min, and a grinding time of 24 h; the uniformly mixed composite powder is then sieved in an inert gas environment, using an 80-mesh sieve.

[0056] III. Sintering:

[0057] The uniformly mixed raw materials obtained in step two are placed in a graphite mold and sintered in an inert gas environment to obtain zirconium carbide reinforced tantalum-based composite material (Ta-5vol.%ZrC).

[0058] The sintering described in step three is hot pressing sintering; the hot pressing sintering process is as follows: the temperature is raised from room temperature to 1900℃, held at 1900℃ for 60 minutes, and then cooled to room temperature. The heating rate is 20℃ / min, the cooling rate is 20℃ / min, and the pressure is maintained at 30MPa during the sintering process.

[0059] The inert gas mentioned in steps two and three is argon.

[0060] The zirconium carbide-reinforced tantalum-based composite material prepared in Example 2 exhibits high density, uniform second-phase distribution, and uniform elemental distribution with no significant segregation. The zirconium carbide-reinforced tantalum-based composite material has a density of 97.8%, a room temperature hardness of 1.83 GPa, a tensile strength of 517 MPa, and an elongation of 20.5%, demonstrating excellent overall performance.

[0061] Example 3: A method for preparing a zirconium carbide-reinforced tantalum-based composite material (Ta-3 vol.% ZrC), comprising the following steps:

[0062] I. Weighing materials:

[0063] Tantalum powder and transition metal carbide powder are weighed according to a certain volume ratio to obtain the raw materials;

[0064] The transition metal carbide mentioned in step one is zirconium carbide;

[0065] The volume fraction of transition metal carbide powder in the raw materials mentioned in step one is 3%;

[0066] II. Powder Mixing:

[0067] After the tantalum powder weighed in step one is initially mixed with the transition metal carbide powder, it is ball-milled in a vacuum environment and then sieved in an inert gas environment to obtain a uniformly mixed raw material.

[0068] The ball milling process described in step two is as follows: an all-around planetary ball mill is used, with the grinding jar and grinding balls made of zirconium oxide, a ball-to-material ratio of 20:1, a ball mill speed of 250 r / min, and a grinding time of 24 h; the uniformly mixed composite powder is then sieved in an inert gas environment, using an 80-mesh sieve.

[0069] III. Sintering:

[0070] The uniformly mixed raw materials obtained in step two are placed in a mold and sintered in an inert gas environment to obtain zirconium carbide reinforced tantalum-based composite material (Ta-3vol.%ZrC).

[0071] The sintering described in step three is hot pressing sintering; the hot pressing sintering process is as follows: the temperature is raised from room temperature to 1800℃, held at 1800℃ for 60 minutes, and then cooled to room temperature. The heating rate is 20℃ / min, the cooling rate is 20℃ / min, and the pressure is maintained at 30MPa during the sintering process.

[0072] The inert gas mentioned in steps two and three is argon.

[0073] The zirconium carbide-reinforced tantalum-based composite material prepared in Example 3 has high density, uniform second-phase distribution, uniform element distribution, and no obvious segregation. The zirconium carbide particle-reinforced tantalum-based composite material has a density of 97.6%, a hardness of 1.68 GPa, a flexural strength of 938 MPa, a tensile strength of 465 MPa, and an elongation of 17.7%.

[0074] Example 4: A method for preparing a zirconium carbide-reinforced tantalum-based composite material (Ta-3 vol.% ZrC), comprising the following steps:

[0075] I. Weighing materials:

[0076] Tantalum powder and transition metal carbide powder are weighed according to a certain volume ratio to obtain the raw materials;

[0077] The transition metal carbide mentioned in step one is zirconium carbide;

[0078] The volume fraction of transition metal carbide powder in the raw materials mentioned in step one is 3%;

[0079] II. Powder Mixing:

[0080] After the tantalum powder weighed in step one is initially mixed with the transition metal carbide powder, it is ball-milled in a vacuum environment and then sieved in an inert gas environment to obtain a uniformly mixed raw material.

[0081] The ball milling process described in step two is as follows: an all-around planetary ball mill is used, with the grinding jar and grinding balls made of zirconium oxide, a ball-to-material ratio of 20:1, a ball mill speed of 250 r / min, and a grinding time of 24 h; the uniformly mixed composite powder is then sieved in an inert gas environment, using an 80-mesh sieve.

[0082] III. Sintering:

[0083] The uniformly mixed raw materials obtained in step two are placed in a mold and sintered in an inert gas environment to obtain zirconium carbide reinforced tantalum-based composite material (Ta-3vol.%ZrC).

[0084] The sintering described in step three is hot pressing sintering; the hot pressing sintering process is as follows: the temperature is raised from room temperature to 1700℃, held at 1700℃ for 60 minutes, and then cooled to room temperature. The heating rate is 20℃ / min, the cooling rate is 20℃ / min, and the pressure is maintained at 30MPa during the sintering process.

[0085] The inert gas mentioned in steps two and three is argon.

[0086] The zirconium carbide-reinforced tantalum-based composite material prepared in Example 4 has high density, uniform second-phase distribution, uniform element distribution, and no obvious segregation. The zirconium carbide particle-reinforced tantalum-based composite material has a density of 87.5%, a hardness of 1.34 GPa, a tensile strength of 459 MPa, and an elongation of 15.8%.

[0087] Example 5: A method for preparing a zirconium carbide-reinforced tantalum-based composite material (Ta-3vol.%ZrC), comprising the following steps:

[0088] I. Weighing materials:

[0089] Tantalum powder and transition metal carbide powder are weighed according to a certain volume ratio to obtain the raw materials;

[0090] The transition metal carbide mentioned in step one is zirconium carbide;

[0091] The volume fraction of transition metal carbide powder in the raw materials mentioned in step one is 3%;

[0092] II. Powder Mixing:

[0093] After the tantalum powder weighed in step one is initially mixed with the transition metal carbide powder, it is ball-milled in a vacuum environment and then sieved in an inert gas environment to obtain a uniformly mixed raw material.

[0094] The ball milling process described in step two is as follows: an all-around planetary ball mill is used, with the grinding jar and grinding balls made of zirconium oxide, a ball-to-material ratio of 20:1, a ball mill speed of 250 r / min, and a grinding time of 24 h; the uniformly mixed composite powder is then sieved in an inert gas environment, using an 80-mesh sieve.

[0095] III. Sintering:

[0096] The uniformly mixed raw materials obtained in step two are placed in a mold and sintered in an inert gas environment to obtain zirconium carbide reinforced tantalum-based composite material (Ta-3vol.%ZrC).

[0097] The sintering described in step three is hot pressing sintering; the hot pressing sintering process is as follows: the temperature is raised from room temperature to 1600℃, held at 1600℃ for 60 minutes, and then cooled to room temperature. The heating rate is 20℃ / min, the cooling rate is 20℃ / min, and the pressure is maintained at 30MPa during the sintering process; the uniformly mixed composite powder is sieved in an inert gas environment, and the sieve is an 80-mesh sieve.

[0098] The inert gas mentioned in steps two and three is argon.

[0099] The zirconium carbide-reinforced tantalum-based composite material prepared in Example 5 has high density, uniform distribution of the second phase, uniform distribution of all elements, and no obvious segregation. The zirconium carbide particle-reinforced tantalum-based composite material has a density of 87.5%, a hardness of 1.22 GPa, a tensile strength of 323 MPa, and an elongation of 8.1%.

[0100] Example 6: A method for preparing a zirconium carbide-reinforced tantalum-based composite material (Ta-10 vol.% ZrC), comprising the following steps:

[0101] I. Weighing materials:

[0102] Tantalum powder and transition metal carbide powder are weighed according to a certain volume ratio to obtain the raw materials;

[0103] The transition metal carbide mentioned in step one is zirconium carbide;

[0104] The volume fraction of transition metal carbide powder in the raw materials mentioned in step one is 10%;

[0105] II. Powder Mixing:

[0106] After the tantalum powder weighed in step one is initially mixed with the transition metal carbide powder, it is ball-milled in a vacuum environment and then sieved in an inert gas environment to obtain a uniformly mixed raw material.

[0107] The ball milling process described in step two is as follows: an all-around planetary ball mill is used, with the grinding jar and grinding balls made of zirconium oxide, a ball-to-material ratio of 20:1, a ball mill speed of 250 r / min, and a grinding time of 24 h; the uniformly mixed composite powder is then sieved in an inert gas environment, using an 80-mesh sieve.

[0108] III. Sintering:

[0109] The uniformly mixed raw materials obtained in step two are placed in a mold and sintered in an inert gas environment to obtain zirconium carbide reinforced tantalum-based composite material (Ta-10vol.%ZrC).

[0110] The sintering described in step three is hot pressing sintering; the hot pressing sintering process is as follows: the temperature is raised from room temperature to 1800℃, held at 1800℃ for 60 minutes, and then cooled to room temperature. The heating rate is 20℃ / min, the cooling rate is 20℃ / min, and the pressure is maintained at 30MPa during the sintering process.

[0111] The inert gas mentioned in steps two and three is argon.

[0112] The zirconium carbide-reinforced tantalum-based composite material prepared in Example 6 has high density, uniform second-phase distribution, uniform element distribution, and no obvious segregation. The zirconium carbide particle-reinforced tantalum-based composite material has a density of 98.3%, a hardness of 2.05 GPa, a flexural strength of 1311 MPa, a tensile strength of 488 MPa, and an elongation of 8.6%.

[0113] Example 7: A method for preparing a tantalum carbide-reinforced tantalum-based composite material (Ta-3 vol.% TaC), comprising the following steps:

[0114] I. Weighing materials:

[0115] Tantalum powder and transition metal carbide powder are weighed according to a certain volume ratio to obtain the raw materials;

[0116] The transition metal carbide mentioned in step one is tantalum carbide;

[0117] The volume fraction of transition metal carbide powder in the raw materials mentioned in step one is 3%;

[0118] II. Powder Mixing:

[0119] After the tantalum powder weighed in step one is initially mixed with the transition metal carbide powder, it is ball-milled in a vacuum environment and then sieved in an inert gas environment to obtain a uniformly mixed raw material.

[0120] The ball milling process described in step two is as follows: an all-around planetary ball mill is used, with the grinding jar and grinding balls made of zirconium oxide, a ball-to-material ratio of 20:1, a ball mill speed of 250 r / min, and a grinding time of 24 h; the uniformly mixed composite powder is then sieved in an inert gas environment, using an 80-mesh sieve.

[0121] III. Sintering:

[0122] The uniformly mixed raw materials obtained in step two are placed in a mold and sintered in an inert gas environment to obtain tantalum carbide reinforced tantalum-based composite material (Ta-3vol.%TaC).

[0123] The sintering described in step three is hot pressing sintering; the hot pressing sintering process is as follows: the temperature is raised from room temperature to 1800℃, held at 1800℃ for 60 minutes, and then cooled to room temperature. The heating rate is 20℃ / min, the cooling rate is 20℃ / min, and the pressure is maintained at 30MPa during the sintering process.

[0124] The inert gas mentioned in steps two and three is argon.

[0125] The tantalum carbide-reinforced tantalum-based composite material prepared in Example 7 has high density, uniform distribution of the second phase, uniform distribution of all elements, and no obvious segregation. The tantalum carbide particle-reinforced tantalum-based composite material has a density of 98.5%, a hardness of 2.68 GPa, a flexural strength of 1079 MPa, a tensile strength of 692 MPa, and an elongation of 13%.

[0126] Example 8: A method for preparing a tantalum carbide-reinforced tantalum-based composite material (Ta-10 vol.% TaC), comprising the following steps:

[0127] I. Weighing materials:

[0128] Tantalum powder and transition metal carbide powder are weighed according to a certain volume ratio to obtain the raw materials;

[0129] The transition metal carbide mentioned in step one is tantalum carbide;

[0130] The volume fraction of transition metal carbide powder in the raw materials mentioned in step one is 10%;

[0131] II. Powder Mixing:

[0132] After the tantalum powder weighed in step one is initially mixed with the transition metal carbide powder, it is ball-milled in a vacuum environment and then sieved in an inert gas environment to obtain a uniformly mixed raw material.

[0133] The ball milling process described in step two is as follows: an all-around planetary ball mill is used, with the grinding jar and grinding balls made of zirconium oxide, a ball-to-material ratio of 20:1, a ball mill speed of 250 r / min, and a grinding time of 24 h; the uniformly mixed composite powder is then sieved in an inert gas environment, using an 80-mesh sieve.

[0134] III. Sintering:

[0135] The uniformly mixed raw materials obtained in step two are placed in a mold and sintered in an inert gas environment to obtain tantalum carbide reinforced tantalum matrix composite material (Ta-10vol.%TaC).

[0136] The sintering described in step three is hot pressing sintering; the hot pressing sintering process is as follows: the temperature is raised from room temperature to 1800℃, held at 1800℃ for 60 minutes, and then cooled to room temperature. The heating rate is 20℃ / min, the cooling rate is 20℃ / min, and the pressure is maintained at 30MPa during the sintering process.

[0137] The inert gas mentioned in steps two and three is argon.

[0138] The tantalum carbide-reinforced tantalum-based composite material prepared in Example 8 has high density, uniform second-phase distribution, uniform element distribution, and no obvious segregation. The tantalum carbide particle-reinforced tantalum-based composite material has a density of 97.7%, a hardness of 3.27 GPa, a flexural strength of 983 MPa, a tensile strength of 786 MPa, and an elongation of 9.4%.

[0139] Example 9: A method for preparing a titanium carbide-reinforced tantalum-based composite material (Ta-3 vol.% TiC), comprising the following steps:

[0140] I. Weighing materials:

[0141] Tantalum powder and transition metal carbide powder are weighed according to a certain volume ratio to obtain the raw materials;

[0142] The transition metal carbide mentioned in step one is titanium carbide;

[0143] The volume fraction of transition metal carbide powder in the raw materials mentioned in step one is 3%;

[0144] II. Powder Mixing:

[0145] After the tantalum powder weighed in step one is initially mixed with the transition metal carbide powder, it is ball-milled in a vacuum environment and then sieved in an inert gas environment to obtain a uniformly mixed raw material.

[0146] The ball milling process described in step two is as follows: an all-around planetary ball mill is used, with the grinding jar and grinding balls made of zirconium oxide, a ball-to-material ratio of 20:1, a ball mill speed of 250 r / min, and a grinding time of 24 h; the uniformly mixed composite powder is then sieved in an inert gas environment, using an 80-mesh sieve.

[0147] III. Sintering:

[0148] The uniformly mixed raw materials obtained in step two are placed in a mold and sintered in an inert gas environment to obtain titanium carbide reinforced tantalum-based composite material (Ta-3vol.%TiC).

[0149] The sintering described in step three is hot pressing sintering; the hot pressing sintering process is as follows: the temperature is raised from room temperature to 1800℃, held at 1800℃ for 60 minutes, and then cooled to room temperature. The heating rate is 20℃ / min, the cooling rate is 20℃ / min, and the pressure is maintained at 30MPa during the sintering process.

[0150] The inert gas mentioned in steps two and three is argon.

[0151] The titanium carbide-reinforced tantalum-based composite material prepared in Example 9 has high density, uniform second-phase distribution, uniform element distribution, and no obvious segregation. The titanium carbide particle-reinforced tantalum-based composite material has a density of 98.5%, a hardness of 2.18 GPa, a flexural strength of 1080 MPa, a tensile strength of 568 MPa, and an elongation of 16.1%.

[0152] Example 10: A method for preparing a titanium carbide-reinforced tantalum-based composite material (Ta-10 vol.% TiC), comprising the following steps:

[0153] I. Weighing materials:

[0154] Tantalum powder and transition metal carbide powder are weighed according to a certain volume ratio to obtain the raw materials;

[0155] The transition metal carbide mentioned in step one is titanium carbide;

[0156] The volume fraction of transition metal carbide powder in the raw materials mentioned in step one is 10%;

[0157] II. Powder Mixing:

[0158] After the tantalum powder weighed in step one is initially mixed with the transition metal carbide powder, it is ball-milled in a vacuum environment and then sieved in an inert gas environment to obtain a uniformly mixed raw material.

[0159] The ball milling process described in step two is as follows: an all-around planetary ball mill is used, with the grinding jar and grinding balls made of zirconium oxide, a ball-to-material ratio of 20:1, a ball mill speed of 250 r / min, and a grinding time of 24 h; the uniformly mixed composite powder is then sieved in an inert gas environment, using an 80-mesh sieve.

[0160] III. Sintering:

[0161] The uniformly mixed raw materials obtained in step two are placed in a mold and sintered in an inert gas environment to obtain titanium carbide reinforced tantalum-based composite material (Ta-10vol.%TiC).

[0162] The sintering described in step three is hot pressing sintering; the hot pressing sintering process is as follows: the temperature is raised from room temperature to 1800℃, held at 1800℃ for 60 minutes, and then cooled to room temperature. The heating rate is 20℃ / min, the cooling rate is 20℃ / min, and the pressure is maintained at 30MPa during the sintering process.

[0163] The inert gas mentioned in steps two and three is argon.

[0164] The titanium carbide-reinforced tantalum-based composite material prepared in Example 10 has high density, uniform second-phase distribution, uniform element distribution, and no obvious segregation. The titanium carbide particle-reinforced tantalum-based composite material has a density of 98.5%, a hardness of 2.94 GPa, a flexural strength of 862 MPa, a tensile strength of 672 MPa, and an elongation of 7.4%.

[0165] Example 11: A method for preparing a zirconium carbide-reinforced tantalum-based composite material (Ta-3 vol.% ZrC), comprising the following steps:

[0166] I. Weighing materials:

[0167] Tantalum powder and transition metal carbide powder are weighed according to a certain volume ratio to obtain the raw materials;

[0168] The transition metal carbide mentioned in step one is zirconium carbide;

[0169] The volume fraction of transition metal carbide powder in the raw materials mentioned in step one is 3%;

[0170] II. Powder Mixing:

[0171] After the tantalum powder weighed in step one is initially mixed with the transition metal carbide powder, it is ball-milled in a vacuum environment and then sieved in an inert gas environment to obtain a uniformly mixed raw material.

[0172] The ball milling process described in step two is as follows: an all-around planetary ball mill is used, with the grinding jar and grinding balls made of zirconium oxide, a ball-to-material ratio of 15:1, a ball mill speed of 200 r / min, and a grinding time of 24 h; the uniformly mixed composite powder is then sieved in an inert gas environment, using an 80-mesh sieve.

[0173] III. Sintering:

[0174] The uniformly mixed raw materials obtained in step two are placed in a mold and sintered in an inert gas environment to obtain zirconium carbide reinforced tantalum-based composite material (Ta-3vol.%ZrC).

[0175] The sintering described in step three is hot pressing sintering; the hot pressing sintering process is as follows: the temperature is raised from room temperature to 1800℃, held at 1800℃ for 60 minutes, and then cooled to room temperature. The heating rate is 20℃ / min, the cooling rate is 20℃ / min, and the pressure is maintained at 30MPa during the sintering process.

[0176] The inert gas mentioned in steps two and three is argon.

[0177] The zirconium carbide-reinforced tantalum-based composite material prepared in Example 11 has high density, uniform distribution of the second phase, uniform distribution of all elements, and no obvious segregation. The zirconium carbide particle-reinforced tantalum-based composite material has a density of 97.9%, a hardness of 1.82 GPa, a tensile strength of 458 MPa, and an elongation of 18.2%.

[0178] Example 12: A method for preparing a zirconium carbide-reinforced tantalum-based composite material (Ta-1 vol.% ZrC), comprising the following steps:

[0179] I. Weighing materials:

[0180] Tantalum powder and transition metal carbide powder are weighed according to a certain volume ratio to obtain the raw materials;

[0181] The transition metal carbide mentioned in step one is zirconium carbide;

[0182] The volume fraction of transition metal carbide powder in the raw materials mentioned in step one is 1%;

[0183] II. Powder Mixing:

[0184] After the tantalum powder weighed in step one is initially mixed with the transition metal carbide powder, it is ball-milled in a vacuum environment and then sieved in an inert gas environment to obtain a uniformly mixed raw material.

[0185] The ball milling process described in step two is as follows: an all-around planetary ball mill is used, with the ball mill jar and grinding balls made of zirconium oxide, a ball-to-material ratio of 10:1, a ball mill speed of 200 r / min, and a ball milling time of 24 h; the uniformly mixed composite powder is then sieved in an inert gas environment, using an 80-mesh sieve.

[0186] III. Sintering:

[0187] The uniformly mixed raw materials obtained in step two are placed in a mold and sintered by discharge plasma under vacuum to obtain zirconium carbide reinforced tantalum-based composite material (Ta-1vol.%ZrC).

[0188] The sintering process described in step three is as follows: the temperature is raised from room temperature to 1800℃, held at 1800℃ for 60 minutes, and then cooled to room temperature. The heating rate is 20℃ / min, the cooling rate is 20℃ / min, and the pressure is maintained at 30MPa during the sintering process.

[0189] The inert gas mentioned in step two is argon.

[0190] The zirconium carbide-reinforced tantalum-based composite material prepared in Example 12 has high density, uniform second-phase distribution, uniform element distribution, and no obvious segregation. The zirconium carbide particle-reinforced tantalum-based composite material has a density of 99.1%, a hardness of 1.63 GPa, a tensile strength of 496 MPa, and an elongation of 22.5%.

[0191] Example 13: A method for preparing a zirconium carbide-reinforced tantalum-based composite material (Ta-15 vol.% ZrC), comprising the following steps:

[0192] I. Weighing materials:

[0193] Tantalum powder and transition metal carbide powder are weighed according to a certain volume ratio to obtain the raw materials;

[0194] The transition metal carbide mentioned in step one is zirconium carbide;

[0195] The volume fraction of transition metal carbide powder in the raw materials mentioned in step one is 15%;

[0196] II. Powder Mixing:

[0197] After the tantalum powder weighed in step one is initially mixed with the transition metal carbide powder, it is ball-milled in a vacuum environment and then sieved in an inert gas environment to obtain a uniformly mixed raw material.

[0198] The ball milling process described in step two is as follows: an all-around planetary ball mill is used, with the grinding jar and grinding balls made of zirconium oxide, a ball-to-material ratio of 10:1, a ball mill speed of 150 r / min, and a grinding time of 24 h; the uniformly mixed composite powder is then sieved in an inert gas environment, using an 80-mesh sieve.

[0199] III. Sintering:

[0200] The uniformly mixed raw materials obtained in step two are placed in a mold and subjected to spark plasma sintering in a vacuum environment to obtain zirconium carbide reinforced tantalum-based composite material (Ta-15vol.%ZrC).

[0201] The sintering process described in step three is as follows: the temperature is raised from room temperature to 1800℃, held at 1800℃ for 60 minutes, and then cooled to room temperature. The heating rate is 20℃ / min, the cooling rate is 20℃ / min, and the pressure is maintained at 30MPa during the sintering process.

[0202] The inert gas mentioned in step two is argon.

[0203] The zirconium carbide-reinforced tantalum-based composite material prepared in Example 13 has high density, uniform second-phase distribution, uniform element distribution, and no obvious segregation. The zirconium carbide particle-reinforced tantalum-based composite material has a density of 98.7%, a hardness of 2.93 GPa, a tensile strength of 672 MPa, and an elongation of 5.2%.

[0204] Comparative Example 1: The preparation of pure tantalum material was carried out according to the following steps:

[0205] 1. Weigh the required powder:

[0206] Weigh out pure tantalum powder;

[0207] The purity of tantalum powder mentioned in step one > 99.0 wt.%%

[0208] II. Ball milling:

[0209] The tantalum powder weighed in step one was subjected to all-around planetary ball milling in a vacuum environment and then sieved in argon gas to obtain a uniformly mixed raw material:

[0210] The ball milling process parameters described in step two are: ball-to-material ratio of 20:1, ball mill speed of 200 r / min, and ball milling time of 24 h; the ball-milled powder is sieved in an inert gas environment, and the sieve is an 80-mesh sieve.

[0211] III. Sintering:

[0212] The powder obtained in step two is placed in a mold and hot-pressed and sintered under argon protection to obtain the corresponding pure tantalum material.

[0213] The sintering process described in step three is as follows: the temperature is raised from room temperature to 2100℃, and held at 2100℃ for 10 minutes. The temperature was lowered to room temperature at a rate of 20℃ / min and a rate of 20℃ / min, while maintaining a pressure of 30MPa during sintering.

[0214] The pure tantalum material prepared in Comparative Example 1 had a density of 99.82%, a hardness of 2.34 GPa, a tensile strength of 108 MPa, a yield strength of 108 MPa, and an elongation of 0.5%.

[0215] Figure 1 XRD patterns of zirconium carbide-reinforced tantalum-based composites prepared in Examples 1, 2, and 8 with different volume fractions;

[0216] from Figure 1 It can be seen that in tantalum matrix composites reinforced with zirconium carbide particles of different volume fractions, Ta2C phase is generated in situ at the interface between carbide and tantalum, which effectively improves the bonding force between zirconium carbide particles and tantalum matrix. At the same time, Ta2C has excellent synergistic deformation ability, which effectively maintains the plastic deformation ability and elongation of tantalum matrix composites while improving the engineering stress of tantalum matrix composites.

[0217] Figure 2 SEM images of zirconium carbide-reinforced tantalum matrix composites prepared by adding different volume fractions in Examples 1, 2, and 8;

[0218] from Figure 2 The microstructure diagram shows that zirconium carbide particles of different volume fractions are uniformly distributed in the tantalum matrix, with no obvious pores, resulting in a dense tantalum matrix composite reinforced with zirconium carbide particles. This invention can simply and effectively improve the dispersion uniformity of zirconium carbide particles in the tantalum matrix, laying the foundation for improving the mechanical properties of tantalum matrix composites.

Claims

1. A method for preparing a transition metal carbide particle-reinforced tantalum-based composite material, characterized in that... Includes the following steps: I. Weighing materials: Tantalum powder and transition metal carbide powder are weighed according to a certain volume ratio to obtain the raw materials; II. Powder Mixing: After the tantalum powder weighed in step one is initially mixed with the transition metal carbide powder, it is ball-milled in an inert gas or vacuum environment and then sieved in an inert gas environment through an 80-320 mesh sieve to obtain a uniformly mixed composite raw material. III. Sintering: The uniformly mixed raw materials obtained in step two are placed in a graphite mold and sintered in a vacuum or inert gas environment to obtain tantalum-based composite materials reinforced with transition metal carbide particles of different volume fractions.

2. The method for preparing a transition metal carbide particle-reinforced tantalum-based composite material according to claim 1, characterized in that... The transition metal carbides mentioned in step one are titanium carbide, zirconium carbide, hafnium carbide, niobium carbide, tantalum carbide, molybdenum carbide, and tungsten carbide.

3. The method for preparing a transition metal carbide particle-reinforced tantalum-based composite material according to claim 1, characterized in that... The volume fraction of transition metal carbide powder in the raw materials mentioned in step one is 0.3% to 30%.

4. The method for preparing a transition metal carbide particle-reinforced tantalum-based composite material according to claim 1, characterized in that... The ball milling process described in step two is as follows: a planetary ball mill is used, the ball mill jar and the grinding balls are both made of zirconium oxide, the ball-to-material ratio is (5~20):1, the speed of the ball mill is 50r / min~500r / min, the ball milling time is 12h~48h, and the sieving is 80 mesh~320 mesh.

5. The method for preparing a transition metal carbide particle-reinforced tantalum-based composite material according to claim 4, characterized in that... The ball milling process described in step two is as follows: an all-round three-dimensional planetary ball mill is used, the ball mill jar and the grinding balls are both made of zirconium oxide, the ball-to-material ratio is 10:1, the speed of the ball mill is 300 r / min, the ball milling time is 24 h, and the sieve is 80 mesh.

6. The method for preparing a transition metal carbide particle-reinforced tantalum-based composite material according to claim 4, characterized in that... The ball milling process described in step two is as follows: an all-round three-dimensional planetary ball mill is used, the ball mill jar and the grinding balls are both made of zirconium oxide, the ball-to-material ratio is 5:1, the speed of the ball mill is 200 r / min, the ball milling time is 48 h, and the sieve is 80 mesh.

7. The method for preparing a transition metal carbide particle-reinforced tantalum-based composite material according to claim 1, characterized in that... The sintering described in step three can be electrical discharge plasma sintering.

8. The method for preparing a transition metal carbide particle-reinforced tantalum-based composite material according to claim 1, characterized in that... The sintering described in step three is hot pressing sintering; the hot pressing sintering process is as follows: the temperature is raised from room temperature to 1600℃~2200℃, held at 1600℃~2200℃ for 30min~300min, and then cooled to room temperature. The heating rate is 10℃ / min~30℃ / min, the cooling rate is 10℃ / min~30℃ / min, and the pressure is maintained at 10MPa~100MPa during the sintering process.

9. The method for preparing a transition metal carbide particle-reinforced tantalum-based composite material according to claim 1, characterized in that... The sintering described in step three is spark plasma sintering; the spark plasma sintering process is as follows: heating from room temperature to 1600℃~2200℃, holding at 1600℃~2200℃ for 10min~60min, and then cooling to room temperature, with a heating rate of 30℃ / min~150℃ / min and a cooling rate of 30℃ / min~150℃ / min, and maintaining a pressure of 10MPa~100MPa during the sintering process.

10. The method for preparing a transition metal carbide particle-reinforced tantalum-based composite material according to claim 1, characterized in that... The sintering described in step three can be a multi-step sintering process; the multi-step sintering process is as follows: the temperature is raised from room temperature to a temperature range of 1000℃~1600℃, a holding stage is set in the temperature range of 1000℃~1600℃, the holding time is 10min~120min, the holding pressure is 10MPa~100MPa, and then the temperature is raised to 1600℃~2200℃ and held for 30min~300min, the holding pressure is 10MPa~100MPa.

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