CN113004051A - SiCfInterface layer structure of/SiC composite material fuel cladding and preparation method - Google Patents
SiCfInterface layer structure of/SiC composite material fuel cladding and preparation method Download PDFInfo
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- CN113004051A CN113004051A CN201911326646.8A CN201911326646A CN113004051A CN 113004051 A CN113004051 A CN 113004051A CN 201911326646 A CN201911326646 A CN 201911326646A CN 113004051 A CN113004051 A CN 113004051A
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- 239000002131 composite material Substances 0.000 title claims abstract description 48
- 238000005253 cladding Methods 0.000 title claims abstract description 22
- 239000000446 fuel Substances 0.000 title claims abstract description 19
- 238000002360 preparation method Methods 0.000 title claims abstract description 13
- XKRFYHLGVUSROY-UHFFFAOYSA-N Argon Chemical compound [Ar] XKRFYHLGVUSROY-UHFFFAOYSA-N 0.000 claims abstract description 100
- 229910010271 silicon carbide Inorganic materials 0.000 claims abstract description 77
- HBMJWWWQQXIZIP-UHFFFAOYSA-N silicon carbide Chemical compound [Si+]#[C-] HBMJWWWQQXIZIP-UHFFFAOYSA-N 0.000 claims abstract description 73
- 229910052786 argon Inorganic materials 0.000 claims abstract description 50
- 238000000151 deposition Methods 0.000 claims abstract description 47
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 claims abstract description 44
- 230000008021 deposition Effects 0.000 claims abstract description 37
- DWAWYEUJUWLESO-UHFFFAOYSA-N trichloromethylsilane Chemical compound [SiH3]C(Cl)(Cl)Cl DWAWYEUJUWLESO-UHFFFAOYSA-N 0.000 claims abstract description 31
- 239000001257 hydrogen Substances 0.000 claims abstract description 21
- 229910052739 hydrogen Inorganic materials 0.000 claims abstract description 21
- 239000000835 fiber Substances 0.000 claims abstract description 18
- 150000002431 hydrogen Chemical class 0.000 claims abstract description 18
- 238000000034 method Methods 0.000 claims abstract description 14
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 claims abstract description 13
- 238000010438 heat treatment Methods 0.000 claims abstract description 12
- 238000001035 drying Methods 0.000 claims abstract description 11
- CSCPPACGZOOCGX-UHFFFAOYSA-N Acetone Chemical compound CC(C)=O CSCPPACGZOOCGX-UHFFFAOYSA-N 0.000 claims abstract description 10
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 claims abstract description 10
- 239000000126 substance Substances 0.000 claims abstract description 10
- 238000001764 infiltration Methods 0.000 claims abstract description 9
- 230000008595 infiltration Effects 0.000 claims abstract description 9
- 238000001816 cooling Methods 0.000 claims abstract description 8
- 239000007789 gas Substances 0.000 claims abstract description 8
- 238000004321 preservation Methods 0.000 claims abstract description 5
- 238000004506 ultrasonic cleaning Methods 0.000 claims abstract description 5
- 239000002296 pyrolytic carbon Substances 0.000 claims description 21
- 239000000463 material Substances 0.000 claims description 11
- 238000000280 densification Methods 0.000 claims description 4
- 238000005086 pumping Methods 0.000 claims description 3
- 238000004140 cleaning Methods 0.000 claims description 2
- 229910052582 BN Inorganic materials 0.000 description 5
- PZNSFCLAULLKQX-UHFFFAOYSA-N Boron nitride Chemical compound N#B PZNSFCLAULLKQX-UHFFFAOYSA-N 0.000 description 5
- 238000007254 oxidation reaction Methods 0.000 description 4
- 239000011159 matrix material Substances 0.000 description 3
- 230000003647 oxidation Effects 0.000 description 3
- 239000000203 mixture Substances 0.000 description 2
- 230000001590 oxidative effect Effects 0.000 description 2
- ZOXJGFHDIHLPTG-UHFFFAOYSA-N Boron Chemical compound [B] ZOXJGFHDIHLPTG-UHFFFAOYSA-N 0.000 description 1
- 239000011184 SiC–SiC matrix composite Substances 0.000 description 1
- BLRPTPMANUNPDV-UHFFFAOYSA-N Silane Chemical compound [SiH4] BLRPTPMANUNPDV-UHFFFAOYSA-N 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 229910052796 boron Inorganic materials 0.000 description 1
- 229910010293 ceramic material Inorganic materials 0.000 description 1
- 239000011248 coating agent Substances 0.000 description 1
- 238000000576 coating method Methods 0.000 description 1
- 238000013329 compounding Methods 0.000 description 1
- 230000007123 defense Effects 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 239000001307 helium Substances 0.000 description 1
- 229910052734 helium Inorganic materials 0.000 description 1
- SWQJXJOGLNCZEY-UHFFFAOYSA-N helium atom Chemical compound [He] SWQJXJOGLNCZEY-UHFFFAOYSA-N 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 125000004430 oxygen atom Chemical group O* 0.000 description 1
- 229910000077 silane Inorganic materials 0.000 description 1
- 125000003866 trichloromethyl group Chemical group ClC(Cl)(Cl)* 0.000 description 1
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- C04B35/571—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on non-oxide ceramics based on carbides or oxycarbides based on silicon carbide obtained from Si-containing polymer precursors or organosilicon monomers
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Abstract
The invention belongs to SiCfThe technical field of interface layers of/SiC composite fuel cladding, in particular to SiCfAn interface layer structure of a/SiC composite fuel cladding and a preparation method thereof. Sequentially PyC, SiC, PyC and SiC boundary layers from inside to outside. Sequentially putting the silicon carbide fiber prefabricated member into acetone and ethanol for ultrasonic cleaning, and drying in a drying box; placing the prefabricated member into a deposition furnace for preparing an interface layer: vacuumizing the deposition furnace, heating, and sequentially introducing argon and methane gas; stopping introducing methane, introducing only argon, and sequentially introducing hydrogen and trichloromethylsilane; stopping introducing trichloromethylsilane and hydrogen in sequence, introducing argon, introducing methane, depositing and pyrolyzingCarbon; depositing a silicon carbide interface layer, after heat preservation is finished, stopping sequentially introducing trichloromethylsilane and hydrogen, continuously introducing argon, and cooling to room temperature along with the furnace; and (3) putting the prefabricated member into a deposition furnace to be densified through a chemical vapor infiltration process. The interface layer prepared by the method is suitable for SiCf/SiC composite material cladding tubes with the wall thickness of 0.5-2 mm.
Description
Technical Field
The invention belongs to SiCfThe technical field of interface layers of/SiC composite fuel cladding, in particular to SiCfAn interface layer structure of a/SiC composite fuel cladding and a preparation method thereof.
Background
SiCfthe/SiC composite material combines the advantages of high-performance SiC fibers and SiC matrixes, has the characteristics of high strength, low density, high temperature resistance, low chemical activity and the like, is a very promising high-temperature structural material, and has very wide application prospects in the fields of national defense, aerospace, energy sources and the like. In SiCfIn the/SiC composite material, both the fiber and the matrix are determined, and the interface between the fiber and the matrix is used for influencing SiCfKey factors of the performance of the/SiC composite ceramic material. The interface itself is closely related to the fiber, matrix, process, etc. SiCfThe interface of the SiC/SiC composite material is a key factor for controlling the toughness of the material, the modification of the interface is one of keys for improving the performance of the material, and the strength and the toughness of the composite material can be improved simultaneously through the fiber coating.
SiCfThe most commonly used materials for the/SiC composite are pyrolytic carbon (PyC) layer and BN (boron nitride) layer, and from the mechanical point of view, the PyC interface layer can make the composite material exhibit nonlinear mechanical behavior, but the critical disadvantage is that it is very easily oxidized in an oxidizing atmosphere above 800 ℃, and the application of the PyC interface layer in a high-temperature oxidizing atmosphere is limited. BN (boron nitride) has a similar layered structure to pyrolytic carbon, but has excellent oxidation resistance, and the BN starts to be oxidized at 850 ℃ to generate B after oxidation2O3The fiber has the capability of self-healing cracks at high temperature, can prevent oxygen atoms from further dispersing into the material, and obviously improves the oxidation resistance of the fiber, thereby prolonging the service life of the composite material under the high-temperature oxidation atmosphere. However, boron element generates helium under irradiation conditions, and cannot be used as a cladding material.
Disclosure of Invention
The invention aims to provide SiCfThe interface layer structure of the fuel cladding of the/SiC composite material and the preparation method effectively solve the problem that a single PyC interface layer in the SiCf/SiC composite material is unstable under the irradiation condition, and improve the mechanical property and the interface stability of the material.
In order to achieve the purpose, the technical scheme adopted by the invention is as follows:
SiCfThe interface layer structure of the/SiC composite fuel cladding comprises PyC, SiC, PyC and SiC interface layers from inside to outside in sequence.
The thickness of each interface layer is 50 nm-200 nm.
SiCfThe preparation method of the interface layer structure of the/SiC composite fuel cladding comprises the following steps:
the method comprises the following steps: sequentially putting the silicon carbide fiber prefabricated member into acetone and ethanol for ultrasonic cleaning, and drying in a drying box;
step two: placing the prefabricated member processed in the step one into a deposition furnace for preparing an interface layer: vacuumizing the deposition furnace, heating, sequentially introducing argon and methane gas, and adjusting the flow ratio of argon to methane to be 1: (2-5);
step three: stopping letting in methane, only letting in argon, letting in hydrogen, trichloromethylsilane, argon in proper order again: hydrogen gas: the flow ratio of trichloromethylsilane is (5-10): (5-10): 1;
step four: sequentially stopping introducing trichloromethylsilane and hydrogen, introducing argon, introducing methane, and depositing pyrolytic carbon according to the second step;
step five: repeating the third step, depositing a silicon carbide interface layer, after the heat preservation is finished, stopping sequentially introducing trichloromethylsilane and hydrogen, continuously introducing argon, and cooling to room temperature along with the furnace;
step six: putting the silicon carbide fiber prefabricated part with the composite interface layer prepared in the step five into a deposition furnace for densification through a chemical vapor infiltration process: vacuumizing the deposition furnace, heating, sequentially introducing argon, hydrogen, trichloromethylsilane and argon: hydrogen gas: trichloromethyl groupThe flow ratio of the silane is (5-10): (5-10): 1, introducing argon, and cooling to room temperature along with the furnace to obtain the belt (PyC/SiC)2SiC of composite interface layerfa/SiC composite material.
In the first step, the cleaning time is 30 minutes, and the product is dried in a drying box for 30 minutes at 120 ℃.
And step two, vacuumizing the deposition furnace to less than 1Pa, heating to 1000-1200 ℃ at the speed of 6-10 ℃/min, sequentially introducing argon and methane gas, and adjusting the flow ratio of argon to methane to be 1: (2-5), keeping the pressure in the deposition furnace at 500-2000 Pa, and keeping the temperature for 3-4 h.
And step three, only introducing argon for 0.5-1 h, sequentially introducing hydrogen, trichloromethylsilane and argon: hydrogen gas: the flow ratio of trichloromethylsilane is (5-10): (5-10): 1, the pressure in the deposition furnace is 500-2000 Pa, and the temperature is kept for 3-4 h.
And step four, introducing argon for 0.5-1 hour.
Sixthly, putting the material into a deposition furnace to be densified through a chemical vapor infiltration process: vacuum pumping of deposition furnace<1Pa, heating to 1000-1200 ℃ at the speed of 6-10 ℃/min, and introducing argon, hydrogen, trichloromethylsilane and argon in sequence: hydrogen gas: the flow ratio of trichloromethylsilane is (5-10): (5-10): 1, the pressure in the deposition furnace is 500 Pa-2000 Pa, the deposition is carried out for 250 h-450 h, argon is introduced, the mixture is cooled to room temperature along with the furnace, and the belt (PyC/SiC) is obtained2SiC of composite interface layerfa/SiC composite material.
The beneficial effects obtained by the invention are as follows:
the invention is realized by design (PyC/SiC)2The structure and thickness of the composite interface layer are prepared on the silicon carbide fiber prefabricated part (PyC/SiC) at one time by Chemical Vapor Infiltration (CVI)2The SiCf/SiC composite material is prepared by compounding the interface layer and then by a chemical vapor infiltration process, the invention can effectively solve the problem that a single PyC interface layer in the SiCf/SiC composite material is unstable under the irradiation condition, and the mechanical property and the interface stability of the material are improved. The interface layer is suitable for SiCf/SiC composite material cladding with the wall thickness of 0.5-2 mmA tube.
Detailed Description
The present invention will be described in detail with reference to specific examples.
SiCfThe interface layer structure of the/SiC composite fuel cladding comprises an inner layer which is a PyC interface layer, and sequentially comprises SiC, PyC and SiC interface layers from inside to outside, wherein the thickness of each interface layer is 50 nm-200 nm.
SiCfThe preparation method of the interface layer structure of the/SiC composite fuel cladding comprises the following steps:
the method comprises the following steps: and (3) putting the silicon carbide fiber prefabricated part into acetone and ethanol in sequence, carrying out ultrasonic cleaning for 30 minutes, and drying for 30 minutes in a drying box at 120 ℃.
Step two: placing the prefabricated member processed in the step one into a deposition furnace for preparing an interface layer: vacuumizing the deposition furnace to less than 1Pa, heating to 1000-1200 ℃ at the speed of 6-10 ℃/min, introducing argon and methane gas in sequence, and adjusting the flow ratio of argon to methane to be 1: (2-5), keeping the pressure in the deposition furnace at 500-2000 Pa, and keeping the temperature for 3-4 h.
Step three: stopping introducing methane, introducing argon only, continuing for 0.5-1 h, sequentially introducing hydrogen, trichloromethylsilane and argon: hydrogen gas: the flow ratio of trichloromethylsilane is (5-10): (5-10): 1, the pressure in the deposition furnace is 500-2000 Pa, and the temperature is kept for 3-4 h.
Step four: and sequentially stopping introducing the trichloromethylsilane and the hydrogen, introducing the argon, continuing for 0.5-1 h, introducing the methane, and depositing the pyrolytic carbon according to the step two.
Step five: and repeating the third step, depositing a silicon carbide interface layer, after the heat preservation is finished, stopping sequentially introducing the trichloromethylsilane and the hydrogen, continuously introducing the argon, and cooling to the room temperature along with the furnace.
Step six: putting the silicon carbide fiber prefabricated part with the composite interface layer prepared in the step five into a deposition furnace for densification through a chemical vapor infiltration process: vacuum pumping of deposition furnace<1Pa, heating to 1000-1200 ℃ at the speed of 6-10 ℃/min, and introducing argon, hydrogen, trichloromethylsilane and argon in sequence: hydrogenGas: the flow ratio of trichloromethylsilane is (5-10): (5-10): 1, the pressure in the deposition furnace is 500 Pa-2000 Pa, the deposition is carried out for 250 h-450 h, argon is introduced, the mixture is cooled to room temperature along with the furnace, and the belt (PyC/SiC) is obtained2SiC of composite interface layerfa/SiC composite material.
Examples
1) The wall thickness of the tube of the silicon carbide fiber prefabricated part is 1mm, the silicon carbide fiber prefabricated part is sequentially placed into acetone and ethanol for ultrasonic cleaning for 30 minutes, and is dried for 30 minutes in a drying box at 120 ℃.
2) Placing the prefabricated member treated in the step 1) into a deposition furnace for interface layer deposition: equipment evacuation 10-1Pa, heating to 1100 ℃ at the speed of 10 ℃/min, sequentially introducing argon and methane gas, and adjusting the gas flow ratio to be 1: and 4, keeping the pressure in the deposition furnace at 1000Pa, and keeping the temperature for 4 hours.
3) Stopping introducing methane, introducing argon, continuing for 0.5h, and sequentially introducing hydrogen and trichloromethylsilane (CH)3SiCl3)，Ar：H2：CH3SiCl3The ratio of (A) to (B) is 5: 6: 1, keeping the pressure in the furnace at 1000Pa, and keeping the temperature for 3 h.
4) Stopping the introduction of CH in sequence3SiCl3And H2Ar is introduced for 0.5h, methane is introduced and the pyrolytic carbon is again deposited according to step 2).
5) Repeating the step 3), depositing a silicon carbide interface layer, and stopping sequentially introducing CH after heat preservation is finished3SiCl3And H2And continuously introducing Ar, and cooling to room temperature along with the furnace.
6) Putting the silicon carbide fiber preform with the composite interface layer prepared in the step 5) into a deposition furnace for densification through a CVI (chemical vapor infiltration) process: equipment evacuation 10-1Pa, heating to 1100 ℃ at the speed of 10 ℃/min, and introducing argon, hydrogen, trichloromethylsilane, Ar: h2：CH3SiCl3The ratio of (A) to (B) is 5: 5: 1, depositing for 300h under the pressure of 1000Pa in the furnace, introducing Ar, and cooling to room temperature along with the furnace to obtain the SiCf/SiC composite material with the (PyC/SiC)2 composite interface layer.
Claims (8)
1. SiCfThe interface layer structure of the/SiC composite fuel cladding is characterized in that: sequentially PyC, SiC, PyC and SiC boundary layers from inside to outside.
2. SiC according to claim 1fThe interface layer structure of the/SiC composite fuel cladding is characterized in that: the thickness of each interface layer is 50 nm-200 nm.
3. SiCfThe preparation method of the interface layer structure of the/SiC composite fuel cladding is characterized by comprising the following steps of: the method comprises the following steps:
the method comprises the following steps: sequentially putting the silicon carbide fiber prefabricated member into acetone and ethanol for ultrasonic cleaning, and drying in a drying box;
step two: placing the prefabricated member processed in the step one into a deposition furnace for preparing an interface layer: vacuumizing the deposition furnace, heating, sequentially introducing argon and methane gas, and adjusting the flow ratio of argon to methane to be 1: (2-5);
step three: stopping letting in methane, only letting in argon, letting in hydrogen, trichloromethylsilane, argon in proper order again: hydrogen gas: the flow ratio of trichloromethylsilane is (5-10): (5-10): 1;
step four: sequentially stopping introducing trichloromethylsilane and hydrogen, introducing argon, introducing methane, and depositing pyrolytic carbon according to the second step;
step five: repeating the third step, depositing a silicon carbide interface layer, after the heat preservation is finished, stopping sequentially introducing trichloromethylsilane and hydrogen, continuously introducing argon, and cooling to room temperature along with the furnace;
step six: putting the silicon carbide fiber prefabricated part with the composite interface layer prepared in the step five into a deposition furnace for densification through a chemical vapor infiltration process: vacuumizing the deposition furnace, heating, sequentially introducing argon, hydrogen, trichloromethylsilane and argon: hydrogen gas: the flow ratio of trichloromethylsilane is (5-10): (5-10): 1, introducing argon, and cooling to room temperature along with the furnace to obtain the belt (PyC/SiC)2SiC of composite interface layerfa/SiC composite material.
4. SiC according to claim 3fThe preparation method of the interface layer structure of the/SiC composite fuel cladding is characterized by comprising the following steps of: in the first step, the cleaning time is 30 minutes, and the product is dried in a drying box for 30 minutes at 120 ℃.
5. SiC according to claim 3fThe preparation method of the interface layer structure of the/SiC composite fuel cladding is characterized by comprising the following steps of: step two, vacuumizing the deposition furnace<1Pa, raising the temperature to 1000-1200 ℃ at the speed of 6-10 ℃/min, introducing argon and methane gas in sequence, and adjusting the flow ratio of argon to methane to be 1: (2-5), keeping the pressure in the deposition furnace at 500-2000 Pa, and keeping the temperature for 3-4 h.
6. SiC according to claim 3fThe preparation method of the interface layer structure of the/SiC composite fuel cladding is characterized by comprising the following steps of: and step three, only introducing argon for 0.5-1 h, sequentially introducing hydrogen, trichloromethylsilane and argon: hydrogen gas: the flow ratio of trichloromethylsilane is (5-10): (5-10): 1, the pressure in the deposition furnace is 500-2000 Pa, and the temperature is kept for 3-4 h.
7. SiC according to claim 3fThe preparation method of the interface layer structure of the/SiC composite fuel cladding is characterized by comprising the following steps of: and step four, introducing argon for 0.5-1 hour.
8. SiC according to claim 3fThe preparation method of the interface layer structure of the/SiC composite fuel cladding is characterized by comprising the following steps of: sixthly, putting the material into a deposition furnace to be densified through a chemical vapor infiltration process: vacuum pumping of deposition furnace<1Pa, heating to 1000-1200 ℃ at the speed of 6-10 ℃/min, and introducing argon, hydrogen, trichloromethylsilane and argon in sequence: hydrogen gas: the flow ratio of trichloromethylsilane is (5-10): (5-10): 1, the pressure in the deposition furnace is 500-2000 Pa, the deposition is carried out for 250-450 h, argon is introduced, and the chamber is cooled along with the furnaceWen, to obtain a belt (PyC/SiC)2SiC of composite interface layerfa/SiC composite material.
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