Preparation process of ultra-high-temperature modified C / SiC ceramic matrix composite leading edge

Abstract

The invention discloses a preparation process of a superhigh-temperature modified C / SiC ceramic matrix composite leading edge. The preparation process comprises the following steps: step S1, shaping a compiled fine-compiled puncture preform; s2, performing interface deposition on the shaped prefabricated body to obtain a front edge I; s3, performing chemical vapor deposition SiC operation on the front edge I to obtain a front edge II; s4, the front edge II is subjected to slurry dipping, and a front edge III is obtained; s5, introducing the resin L3 into the leading edge III to obtain a leading edge IV; s6, introducing the PCS into the leading edge IV to obtain a leading edge V; s7, introducing a phenolic resin precursor into the front edge V to obtain a front edge VI; and S8, the front edge VI is subjected to reactive melt infiltration, and the front edge of the part is obtained. According to the preparation method, CVI, slurry impregnation, PIP and RMI are combined, an ultra-high-temperature phase is introduced, and the preparation efficiency of the C / SiC ceramic-based composite material is improved.

Description

TECHNICAL FIELD

[0001] The present application relates to the technical field of continuous fiber reinforced ceramic matrix composites, in particular to a preparation process of an ultra-high temperature modified C / SiC ceramic matrix composite leading edge. BACKGROUND

[0002] With the rapid development of aerospace technology, the application demand of aircraft in ultra-high temperature environment is increasing. The leading edge component of the aircraft as a key component to withstand high temperature ablation, high speed airflow scouring and other extreme environments, puts forward high requirements on the high temperature resistance, oxidation resistance, ablation resistance and mechanical properties of the material.

[0003] At present, carbon fiber reinforced ceramic matrix (C / SiC) composite material has become an important candidate material for high temperature thermal structure material in the field of aerospace due to its low density, high specific strength, high specific modulus and other excellent properties. However, C / SiC composite material is easy to oxidize and ablate in high temperature oxygen environment, which limits its application. In order to solve this problem, researchers introduce ultra-high temperature ceramic phase (UHTCs) to modify it. UHTCs has the characteristics of high melting point, low density, high strength and hardness, high thermal conductivity, etc., which can significantly improve the oxidation resistance and ablation resistance of C / SiC composite material, and meet the demand of thermal protection material in high temperature environment.

[0004] However, the existing preparation process has many shortcomings, for example, patent CN117263708A uses chemical liquid phase gasification deposition process to introduce ultra-high temperature phase, which overcomes the problems of long preparation period and high production cost of traditional precursor impregnation and pyrolysis method, but this method causes great damage to the fiber, which is not conducive to its load bearing; patent ZL 201110348234.1 uses chemical vapor deposition / infiltration method to prepare double gradient carbide modified C / C composite material, which improves the ablation resistance of the material, but the chemical vapor deposition efficiency is low, which is not conducive to engineering production. In addition, the existing process still has room for improvement in realizing lightweight, uniform and dense structure and high reliability.

[0005] Therefore, it is necessary to develop an ultra-high temperature modified leading edge preparation process that can balance low cost, high efficiency, uniform density and excellent performance, which is a key technical method to meet the development needs of modern aircraft. SUMMARY

[0006] In view of the above problems in the prior art, the present application provides a preparation process of an ultra-high temperature modified C / SiC ceramic matrix composite leading edge, which solves the problems of high cost and low efficiency in the preparation of existing C / SiC composite materials.

[0007] In order to achieve the above purpose, the technical scheme adopted by the present application is as follows: A preparation process of an ultra-high temperature modified C / SiC ceramic matrix composite leading edge, comprising the following steps: Step S1, shaping the completed fine weaving puncture preform; Step S2, interface deposition is performed on the shaped preform to obtain a leading edge I; Step S3, chemical vapor deposition of SiC is performed on the leading edge I, and after the deposition is completed, the leading edge I is machined to obtain a leading edge II; Step S4, slurry impregnation is performed on the leading edge II to obtain a leading edge III; Step S5, L3 resin is introduced into the leading edge III by vacuum impregnation to obtain a leading edge IV; Step S6, PCS is introduced into the leading edge IV by vacuum impregnation to obtain a leading edge V; Step S7, phenolic resin precursor is introduced into the leading edge V by vacuum impregnation to obtain a leading edge VI; Step S8, reaction melt impregnation is performed on the leading edge VI to obtain a part leading edge.

[0008] The present application combines CVI, slurry impregnation, PIP and RMI processes, fully utilizes the advantages of each process, overcomes the shortcomings of single process, improves the performance and preparation efficiency of the material, and introduces ultra-high temperature phase by slurry impregnation method, which solves the problem of low CVI deposition efficiency and improves the uneven distribution of ultra-high temperature phase in PIP process, effectively improving the preparation efficiency of C / SiC ceramic matrix composite.

[0009] Further, in the interface deposition of step S2, the deposition is performed by propylene flow of 0.1-20L / min and argon flow of 0.5-21L / min, the deposition time is 10-80h, and the temperature is 400-1100℃.

[0010] Further, in the chemical vapor deposition of SiC of step S3, the flow rate of trichloromethylsilane is 1-15L / min, the flow rate of argon is 1-15L / min, the flow rate of hydrogen is 1-15L / min, the temperature is 500-1200℃, and the deposition time is 20-100h.

[0011] Further, the slurry impregnation method of step S4 comprises: Step S41, configuring the ultra-high temperature powder into a slurry with a volume fraction of 2%-30%; Step S42, impregnating the slurry into the inside of the leading edge II; Step S43, placing the leading edge II obtained in step S42 in an oven and baking at 50-300℃ for 24H to obtain a leading edge III containing ultra-high temperature powder.

[0012] Further, the ultra-high temperature powder includes, but is not limited to, ZrB2 powder, HfB2 powder, ZrC powder or HfC powder of various particle sizes.

[0013] Further, the vacuum impregnation method of step S5 includes: Step S51, vacuumizing: the leading edge III is hung above the L3 resin without being immersed, and vacuumizing is performed for 10-45 min; Step S52, vacuum impregnation: the leading edge III obtained in step S51 is completely immersed in the L3 resin, and vacuum impregnation is performed for 10-45 min; Step S53, pressure impregnation: the leading edge III obtained in step S52 is immersed in the L3 resin and transferred into a pressure tank, the pressure is 0.2-1.5 MPa, pressure impregnation is performed for 10-45 min, then it is transferred into an oven for slow curing at 30-200℃ for 2-20 h, finally, pyrolysis is performed at 700-1600℃ for 0.5-5 h, and the leading edge IV containing the L3 resin is obtained.

[0014] Further, the vacuum impregnation method of step S6 includes: Step S61, vacuumizing: the leading edge IV is hung above the PCS without being immersed, and vacuumizing is performed for 10-45 min; Step S62, vacuum impregnation: the leading edge IV obtained in step S61 is completely immersed in the PCS, and vacuum impregnation is performed for 10-45 min; Step S63, pressure impregnation: the leading edge IV obtained in step S62 is immersed in the PCS and transferred into a pressure tank, the pressure is 0.2-1.5 MPa, pressure impregnation is performed for 10-45 min, then it is transferred into an oven for slow curing at 30-100℃ for 2-20 h, finally, pyrolysis is performed at 500-1500℃ for 0.5-5 h, and the leading edge V containing the PCS is obtained.

[0015] Further, the vacuum impregnation method of step S7 includes: Step S71, vacuumizing: the leading edge V is hung above the phenolic resin without being immersed, and vacuumizing is performed for 10-45 min; Step S72, vacuum impregnation: the leading edge V obtained in step S71 is completely immersed in the phenolic resin, and vacuum impregnation is performed for 10-45 min; Step S73, pressure impregnation: the leading edge V obtained in step S72 is immersed in the phenolic resin and transferred into a pressure tank, the pressure is 0.2-1.5 MPa, pressure impregnation is performed for 10-45 min, then it is transferred into an oven for slow curing at 30-200℃ for 2-20 h, finally, pyrolysis is performed at 600-1500℃ for 0.5-5 h, and the leading edge VI containing the phenolic resin is obtained.

[0016] The application discloses a preparation process of an ultra-high temperature modified C / SiC ceramic matrix composite leading edge. The present application combines CVI (chemical vapor deposition), slurry impregnation, PIP (vacuum impregnation), RMI (reactive melt infiltration), fully utilizes the advantages of each process, overcomes the shortcomings of single process, improves the performance and preparation efficiency of the material, introduces ultra-high temperature phase by the method of slurry impregnation, on the one hand solves the problem of low deposition efficiency of CVI, on the other hand improves the problem of uneven distribution of ultra-high temperature phase in PIP process, effectively improves the preparation efficiency of C / SiC ceramic matrix composite material. BRIEF DESCRIPTION OF DRAWINGS

[0017] Figure 1 A process flow chart of a preparation process of an ultra-high temperature modified C / SiC ceramic matrix composite leading edge of the present application. DETAILED DESCRIPTION

[0018] The specific embodiments of the present application are described below to facilitate the understanding of the present application by those skilled in the art, but it should be clear that the present application is not limited to the scope of the specific embodiments, and for those skilled in the art, it is obvious that various changes are within the spirit and scope of the present application defined and determined by the appended claims, and all the inventions utilizing the concept of the present application are within the scope of protection.

[0019] Example 1 Reference Figure 1 The present embodiment provides a preparation process of an ultra-high temperature modified C / SiC ceramic matrix composite leading edge, which aims to solve the problems of high cost and poor efficiency in the preparation of existing C / SiC composite material, and the specific steps in the present embodiment will be described in detail below.

[0020] A preparation process of an ultra-high temperature modified C / SiC ceramic matrix composite leading edge, comprising the following steps: Step S1, shaping the fine-weave puncture preform completed by weaving; In the present embodiment, a fine-weave puncture preform is used, and the fine-weave puncture preform completed by weaving in advance is clamped and shaped by a preform mold to prevent deformation during deposition.

[0021] Step S2, interfacial deposition of the shaped preform to obtain a leading edge I; Specifically, in the interfacial deposition of step S2, the deposition is carried out with a propylene flow rate of 0.1-20 L / min and an argon flow rate of 0.5-21 L / min, a deposition time of 10-80 h and a temperature of 400-1100℃.

[0022] In this embodiment, the preform formed by clamping and shaping by the preform mold is subjected to interfacial deposition. During interfacial deposition, the deposition is performed at a propylene flow rate of 0.1 L / min, 10 L / min, or 20 L / min, etc., an argon flow rate of 0.5 L / min, 11 L / min, or 21 L / min, etc., a deposition time of 10 h, 20 h, 50 h, or 80 h, etc., and a temperature of 400℃, 600℃, 800℃, or 1100℃, etc. The number of deposition furnace times is determined according to the actual requirements of the interface. In this embodiment, a thick interface is taken as an example, and 2-8 furnace times of deposition are performed to obtain the leading edge I.

[0023] Step S3: performing a chemical vapor deposition SiC operation on the leading edge I, and after the deposition is completed, performing mechanical processing on the leading edge I to obtain a leading edge II. Specifically, in the chemical vapor deposition SiC operation of step S3, the flow rate of trichloromethylsilane is 1-15 L / min, the flow rate of argon is 1-15 L / min, the flow rate of hydrogen is 1-15 L / min, the temperature is 500-1200℃, and the deposition time is 20-100 h.

[0024] In this embodiment, in the chemical vapor deposition SiC operation, the flow rate of trichloromethylsilane is 10 L / min, the flow rate of argon is 10 L / min, the flow rate of hydrogen is 10 L / min, the temperature is 1000℃, and the deposition time is 80 h. After the deposition is completed, the leading edge I is subjected to mechanical processing to form a final size, and the leading edge II is obtained.

[0025] Step S4: performing slurry impregnation on the leading edge II to obtain a leading edge III. Specifically, the slurry impregnation method of step S4 includes: Step S41: configuring ultra-high temperature powder into a slurry at a volume fraction of 2% to 30%. Step S42: impregnating the slurry into the inside of the leading edge II. Step S43: placing the leading edge II obtained in step S42 in an oven for baking at 50-300℃ for 24 H to obtain the leading edge III containing ultra-high temperature powder.

[0026] Specifically, the ultra-high temperature powder includes but is not limited to ZrB2 powder, HfB2 powder, ZrC powder, or HfC powder of various particle sizes.

[0027] In this embodiment, ZrB2 powder is used as the ultra-high temperature powder, the ZrB2 powder is configured into a slurry at a volume fraction of 2% to 30%, and the leading edge II is completely immersed in the configured slurry for impregnation. After the impregnation is completed, the leading edge II is placed in an oven for baking at 200℃ for 24 H to obtain the leading edge III containing ultra-high temperature powder.

[0028] Step S5, introducing L3 resin into the leading edge III by vacuum impregnation to obtain a leading edge IV; Specifically, the vacuum impregnation method of step S5 includes: Step S51, vacuumizing: suspending the leading edge III above the L3 resin without immersion, vacuumizing for 10-45 min; Step S52, vacuum impregnation: completely immersing the leading edge III obtained in step S51 in the L3 resin, vacuum impregnating for 10-45 min; Step S53, pressure impregnation: immersing the leading edge III obtained in step S52 in the L3 resin and transferring into a pressure tank, pressure 0.2-1.5 MPa, pressure impregnating for 10-45 min, then transferring into an oven for slow curing at 30-200℃ for 2-20 h, and finally pyrolyzing at 700-1600℃ for 0.5-5 h to obtain the leading edge IV containing L3 resin.

[0029] In this embodiment, first, the leading edge III is suspended above the L3 resin without immersion, vacuumizing for 30 min, then the leading edge III is completely immersed in the L3 resin, vacuum impregnating for 30 min, then the leading edge III is immersed in the L3 resin and transferred into a pressure tank, pressure impregnating for 30 min at a pressure of 1.0 MPa, then transferred into an oven for slow curing at 180℃ for 10 h, and finally pyrolyzing at 700-1600℃ for 3 h, so as to introduce L3 resin into the leading edge III by vacuum impregnation process to obtain the leading edge IV containing L3 resin.

[0030] Step S6, introducing PCS into the leading edge IV by vacuum impregnation to obtain a leading edge V; Specifically, the vacuum impregnation method of step S6 includes: Step S61, vacuumizing: suspending the leading edge IV above the PCS without immersion, vacuumizing for 10-45 min; Step S62, vacuum impregnation: completely immersing the leading edge IV obtained in step S61 in the PCS, vacuum impregnating for 10-45 min; Step S63, pressure impregnation: immersing the leading edge IV obtained in step S62 in the PCS and transferring into a pressure tank, pressure 0.2-1.5 MPa, pressure impregnating for 10-45 min, then transferring into an oven for slow curing at 30-100℃ for 2-20 h, and finally pyrolyzing at 500-1500℃ for 0.5-5 h to obtain the leading edge V containing PCS.

[0031] In this embodiment, first, the leading edge IV is hung above the PCS without being immersed, vacuumed for 30 min, then the leading edge IV is completely immersed in the PCS, vacuum impregnated for 30 min, then the leading edge IV is immersed in the PCS and transferred into a pressure tank, after pressure impregnation for 30 min at a pressure of 1.0 MPa, it is transferred into an oven for slow curing at 80℃ for 18 h, and finally pyrolysis at 1200℃ for 3 h, so as to introduce the PCS into the leading edge III by vacuum impregnation process to obtain the leading edge V containing PCS.

[0032] Step S7, introducing the phenolic resin precursor into the leading edge V by vacuum impregnation to obtain the leading edge VI; Specifically, the vacuum impregnation method of step S7 comprises: Step S71, vacuuming: the leading edge V is hung above the phenolic resin without being immersed, vacuumed for 10-45 min; Step S72, vacuum impregnation: the leading edge V obtained in step S71 is completely immersed in the phenolic resin, vacuum impregnated for 10-45 min; Step S73, pressure impregnation: the leading edge V obtained in step S72 is immersed in the phenolic resin and transferred into a pressure tank, pressure impregnation for 10-45 min at a pressure of 0.2-1.5 MPa, then transferred into an oven for slow curing at 30-200℃ for 2-20 h, and finally pyrolysis at 600-1500℃ for 0.5-5 h to obtain the leading edge VI containing phenolic resin.

[0033] In this embodiment, first, the leading edge V is hung above the phenolic resin without being immersed, vacuumed for 35 min, then the leading edge V is completely immersed in the phenolic resin, vacuum impregnated for 35 min, then the leading edge V is immersed in the phenolic resin and transferred into a pressure tank, pressure impregnation for 35 min at a pressure of 1.0 MPa, then transferred into an oven for slow curing at 150℃ for 15 h, and finally pyrolysis at 1000℃ for 3.5 h, so as to introduce the phenolic resin into the leading edge V by vacuum impregnation process to obtain the leading edge VI containing phenolic resin.

[0034] Step S8, reacting melt impregnation is performed on the leading edge VI to obtain a part leading edge.

[0035] In this embodiment, an appropriate amount of prepared mixed material is placed in a crucible lined with graphite paper and scraped flat, first rough pressing, then compaction with a press, then scraped flat with a scraper, and then compaction with a press, and the thickness of the powder is 15 mm.

[0036] The leading edge VI is placed in the crucible filled with mixed material, and then mixed material is added above the leading edge VI, and the press is compacted, and RMI (reactive melt impregnation) is performed, and the part leading edge is obtained after RMI.

[0037] Although the specific embodiments of the application have been described in some detail to provide a thorough understanding thereof, it will be apparent to one skilled in the art that variations in form, detail, and implementation can be made without departing from the spirit of the application as described above. The described embodiments are to be considered in all respects only as illustrative and not restrictive.

Claims

1. A preparation process for the leading edge of an ultra-high temperature modified C / SiC ceramic matrix composite material, characterized in that, Includes the following steps: Step S1: Shape the completed finely woven piercing prefabricated body; Step S2: Perform interface deposition on the preform after shaping to obtain leading edge I; Step S3: Perform chemical vapor deposition (CVD) on leading edge I. After deposition, perform machining on leading edge I to obtain leading edge II. Step S4: Impregnate leading edge II with slurry to obtain leading edge III; Step S5: Vacuum impregnation is used to introduce L3 resin into leading edge III to obtain leading edge IV; Step S6: Vacuum impregnation is used to introduce PCS into the leading edge IV to obtain the leading edge V; Step S7: Vacuum impregnation is used to introduce the phenolic resin precursor into the leading edge V to obtain the leading edge VI; Step S8: Perform reactive melt infiltration on the leading edge VI to obtain the leading edge of the part.

2. The preparation process of the ultra-high temperature modified C / SiC ceramic matrix composite material front according to claim 1, characterized in that, In the interface deposition of step S2, the propylene flow rate is 0.1~20L / min, the argon flow rate is 0.5~21L / min, the deposition time is 10-80h, and the temperature is 400-1100℃.

3. The preparation process of the ultra-high temperature modified C / SiC ceramic matrix composite material front according to claim 1, characterized in that: In the chemical vapor deposition (CVD) SiC operation in step S3, the flow rate of trichloromethylsilane is 1-15 L / min, the flow rate of argon is 1-15 L / min, the flow rate of hydrogen is 1-15 L / min, the temperature is 500-1200℃, and the deposition time is 20-100 h.

4. The preparation process of the ultra-high temperature modified C / SiC ceramic matrix composite material front according to claim 2, characterized in that, The slurry impregnation method in step S4 includes: Step S41: Prepare a slurry by mixing ultra-high temperature powder at a volume fraction of 2% to 30%; Step S42: Impregnate the slurry into the interior of the leading edge II; Step S43: Place the leading edge II obtained in step S42 in an oven and bake at 50~300℃ for 24 hours to obtain the leading edge III containing ultra-high temperature powder.

5. The preparation process of the ultra-high temperature modified C / SiC ceramic matrix composite material front according to claim 4, characterized in that: The ultra-high temperature powder includes, but is not limited to, ZrB2 powder, HfB2 powder, ZrC powder, or HfC powder of various particle sizes.

6. The preparation process of the ultra-high temperature modified C / SiC ceramic matrix composite material front according to claim 1, characterized in that: The vacuum impregnation method in step S5 includes: Step S51, Vacuuming: Suspend the leading edge III above the L3 resin without immersing it, and vacuum for 10~45 minutes; Step S52, Vacuum Impregnation: Completely immerse the leading edge III obtained in step S51 in L3 resin and vacuum impregnate for 10~45 min; Step S53, Pressure Impregnation: Immerse the leading edge III obtained in step S52 into L3 resin and transfer it into a pressure vessel. After impregnation at a pressure of 0.2~1.5 MPa for 10~45 min, transfer it into an oven and slowly cure it at 30~200℃ for 2~20 h. Finally, pyrolyze it at 700~1600℃ for 0.5~5 h to obtain the leading edge IV containing L3 resin.

7. The preparation process of the ultra-high temperature modified C / SiC ceramic matrix composite material front according to claim 1, characterized in that, The vacuum impregnation method in step S6 includes: Step S61, Vacuuming: Suspend the leading edge IV above the PCS without immersing it, and vacuum for 10~45 minutes; Step S62, Vacuum Impregnation: Completely immerse the leading edge IV obtained in step S61 in the PCS and vacuum impregnate for 10~45 min; Step S63, Pressure Impregnation: Immerse the leading edge IV obtained in step S62 into PCS and transfer it to a pressure vessel. Impregnate at a pressure of 0.2~1.5 MPa for 10~45 min, then transfer it to an oven and slowly cure it at 30~100℃ for 2~20 h. Finally, pyrolyze it at 500~1500℃ for 0.5~5 h to obtain the leading edge V containing PCS.

8. The preparation process of the ultra-high temperature modified C / SiC ceramic matrix composite material front according to claim 7, characterized in that, The vacuum impregnation method in step S7 includes: Step S71, Vacuuming: Suspend the leading edge V above the phenolic resin without immersing it, and vacuum for 10~45 minutes; Step S72, Vacuum Impregnation: The leading edge V obtained in step S71 is completely immersed in phenolic resin and vacuum impregnated for 10~45 min; Step S73, Pressure Impregnation: Immerse the leading edge V obtained in step S72 into phenolic resin and transfer it to a pressure vessel. After impregnation at a pressure of 0.2~1.5 MPa for 10~45 min, transfer it to an oven and slowly cure it at 30~200℃ for 2~20 h. Finally, pyrolyze it at 600~1500℃ for 0.5~5 h to obtain the leading edge VI containing phenolic resin.

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