锆-硅有机前驱体裂解机理及PIP法制备C/C-ZrC-SiC复合材料的烧蚀行为
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摘要
使用有机锆前驱体(POZ)和聚碳硅烷(PCS)作为前驱体,通过前驱体浸渍-裂解工艺(PIP)制备了C/C-ZrC-SiC复合材料。采用热重分析仪、X射线衍射、扫描电子显微镜等手段研究了Zr-Si混合前驱体的裂解过程中的热失重行为、物相转化过程及显微组织,并详细分析了复合材料的微观结构和烧蚀行为。结果表明:将Zr-Si混合前驱体从室温加热至1 200℃时,ZrC首先转化为无机态的ZrO_2,当裂解温度升高至1 600℃时,ZrO_2通过碳热还原反应生成ZrC陶瓷;SiC晶体的转变温度为1 200～2 000℃。对C/C-ZrC-SiC复合材料烧蚀后的显微组织观察表明,所制备的复合材料具有良好的耐烧蚀性能。
C/C-ZrC-SiC composites were prepared by precursor infiltration and pyrolysis using poly-meric organic zirconium precursor(POZ) and polycarbosilane(PCS) as precursor.Thermogravimetric behavior,phase conversion and microstructure of Zr-Si mixed precursors during pyrolysis were studied by thermal gravimetric analyzer,X-ray diffraction and scanning electron microscope,and the microstructure and ablation behavior of the composites were analyzed in detail.The results indicate that when Zr-Si mixed precursors is heated from room temperature to 1 200 ℃,ZrC precursor transforms to inorganic ZrO_2.When the pyrolysis temperature rises to 1 600 ℃,ZrO_2 can be reduced to ZrC ceramics by carbothermal reduction reaction.The transition temperature of the SiC crystal is 1 200～2 000 ℃.The microstructure of the C/C-ZrC-SiC composites after ablation shows that the prepared composites exhibit good ablation resistance.
C/C-ZrC-SiC composites were prepared by precursor infiltration and pyrolysis using poly-meric organic zirconium precursor(POZ) and polycarbosilane(PCS) as precursor.Thermogravimetric behavior,phase conversion and microstructure of Zr-Si mixed precursors during pyrolysis were studied by thermal gravimetric analyzer,X-ray diffraction and scanning electron microscope,and the microstructure and ablation behavior of the composites were analyzed in detail.The results indicate that when Zr-Si mixed precursors is heated from room temperature to 1 200 ℃,ZrC precursor transforms to inorganic ZrO_2.When the pyrolysis temperature rises to 1 600 ℃,ZrO_2 can be reduced to ZrC ceramics by carbothermal reduction reaction.The transition temperature of the SiC crystal is 1 200～2 000 ℃.The microstructure of the C/C-ZrC-SiC composites after ablation shows that the prepared composites exhibit good ablation resistance.
引文
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[5] HAN J C,HE X D,DU S Y.Oxidation and ablation of 3D carbon-carbon composite at up to 3 000 ℃[J].Carbon,1995,33(4):473-478.
[6] ZHOU W,XIAO P,LUO W,et al.Microstructural evolution of SiC coating on C/C composites exposed to 1 500 ℃ in ambient air[J].Ceramics International,2018.
[7] CUI Y,LI A,LI B,et al.Microstructure and ablation mechanism of C/C-SiC composites[J].Journal of the European Ceramic Society,2014,34(2):171-177.
[8] WEN J,ZHOU S,YI L,et al.Oxidation behavior and high-temperature flexural property of CVD-SiC-coated PIP-C/SiC composites[J].Ceramics International,2018,44(14):16 583-16 588.
[9] HUANG D,ZHANG M,HUANG Q,et al.Preparation of a double layer SiC coating and its oxidation resistance at 1 773 K[J].Corrosion Science,2014,87:134-140.
[10] JIN X,FAN X,LU C,et al.Advances in oxidation and ablation resistance of high and ultra-high temperature ceramics modified or coated carbon/carbon composites[J].Journal of the European Ceramic Society,2018,38(1):1-28.
[11] TANG S,HU C .Design,preparation and properties of carbon fiber reinforced ultra-high temperature ceramic composites for aerospace applications:A review[J].Journal of Materials Science & Technology,2017(2):3-16.
[12] YAN C,LIU R,ZHANG C,et al.Effects of SiC/HfC ratios on the ablation and mechanical properties of 3D Cf/HfC-SiC composites[J].Journal of the European Ceramic Society,2017,37(6):2 343-2 351.
[13] XUE L,SU Z A,YANG X,et al.Microstructure and ablation behavior of C/C-HfC composites prepared by precursor infiltration and pyrolysis[J].Corrosion Science,2015,94:165-170.
[14] JIANG J,WANG S,LI W,et al.Preparation and properties of C/TaC composites via PIP process[J].Ceramics International,2017,43(2):2 379-2 383.
[15] HE Q,LI H,WANG C,et al.Influence of CLVD thermal gradient on the deposition behavior,microstructure and properties of C/C-ZrC composites[J].Ceramics International,2018,44(13):15 631-15 645.
[16] WU H,YI M,GE Y,et al.Microstructural development of a C/C-ZrC-Cu composite prepared by reactive melt infiltration with Zr/Cu powder mixture[J].Materials Characterization,2018,138:238-244.
[17] LI C,LI G,OUYANG H,et al.Microstructure and properties of C/C-ZrC composites prepared by hydrothermal deposition combined with carbothermal reduction[J].Journal of Alloys & Compounds,2018,741:323-330.
[18] ZHOU H,NI D,HE P,et al.Ablation behavior of C/C-ZrC and C/SiC-ZrC composites fabricated by a joint process of slurry impregnation and chemical vapor infiltration[J].Ceramics International,2017.44(5):4 777-4 782.
[19] ZHAO Z,LI W,LI K,et al.Ablation behavior of C/C-ZrC-SiC composites prepared by reactive melt infiltration under oxyacetylene torch at two heat fluxes[J].Ceramics International,2018,44(14):17 345-17 358.
[20] CHANG Y,SUN W,XIONG X,et al.Microstructure and ablation behaviors of a novel gradient C/C-ZrC-SiC composite fabricated by an improved reactive melt infiltration[J].Ceramics International,2016,42(15):16 906-16 915.
[21] HE Q.Microstructure and ablation property of C/C-ZrC-SiC composites fabricated by chemical liquid-vapor deposition combined with precursor infiltration and pyrolysis[J].Ceramics International,2019.45(3):3 767-3 781.
[22] ZHAO Z,LI K,LI W,et al.Preparation,ablation behavior and mechanism of C/C-ZrC-SiC and C/C-SiC composites[J].Ceramics International,2018,44(7):7 481-7 490.
[23] 曹柳絮.PIP及RMI法制备C/C-SiC复合材料过程及其性能研究[D].长沙:中南大学,2014.
[24] LIU Q,ZHANG L,LIU J,et al.The oxidation behavior of SiC-ZrC-SiC-Coated C/SiC minicomposites at ultrahigh temperatures[J].Journal of the American Ceramic Society,2010,93(12):3 990-3 992.
[25] CHEN S,ZHANG Y,ZHANG C,et al.Effects of SiC interphase by chemical vapor deposition on the properties of C/ZrC composite prepared via precursor infiltration and pyrolysis route[J].Materials & Design,2013,46(4):497-502.
[26] LI K Z,JING X,FU Q,et al.Effects of porous C/C density on the densification behavior and ablation property of C/C-ZrC-SiC composites[J].Carbon,2013,57(3):161-168.
[27] ZHAO D,HU H,ZHANG C,et al.A simple way to prepare precursors for zirconium carbide[J].Journal of Materials Science,2010,45(23):6 401-6 405.