C/C复合材料表面反应熔渗法制备SiC-ZrC涂层的组织与结构
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摘要
采用反应熔渗法(RMI)在密度为1.6 g/cm3的C/C复合材料上制备厚度为20~50μm的SiC-ZrC涂层。研究SiC-ZrC涂层结构以及涂层与C/C复合材料的界面相组成。结果表明:4种不同比例混合后的Zr,Si,C和ZrO_2粉末反应熔渗得到的样品涂层表面质量较好,由于反应过程先达到Si的熔点生成SiC,随着温度升高,当Zr和Si都熔融后,生成ZrC的吉布斯自由能低于SiC,故涂层由内到外呈现SiC-ZrC-SiC的三层结构,所有样品内部都熔渗了不同深度的ZrC和SiC。在偏光显微镜下SiC呈现黄绿色块状和粒状,ZrC呈现灰白色块状;粉末熔体通过共晶反应生成的Si,ZrSi_2,Zr和Zr_2Si与原料中的C以及热解炭反应最终生成SiC和ZrC,反应最终残留物中并没有发现ZrO_2。
SiC-ZrC coatings with thickness of 20-50 μm were deposited by the reactive metal infiltration(RMI) technology on C/C composites with density of 1.6 g/cm~3. The microstructure of SiC-ZrC coating and phase composition of interface between SiC-ZrC coatings and C/C composites were investigated. The results show that, good performance of SiC-ZrC coatings can be obtained by reactive infiltration method on C/C composites with 4 kinds of blending powders(Zr, Si, C and ZrO_2). The temperature first reaches the melting point of Si, which reacts with C. With the temperature increassing, both Siand Zrmelt, and the generating Gibbs free energy of ZrC is lower than SiC, so the coating is a three-layer structure of SiC-ZrC-SiC from inside to outside, and all samples are infiltrated with ZrC and SiC at different depths. SiC is the green granular and bulk phase, and ZrC is the white block phase under observing by polarizing microscope. SiC and ZrC are produced by the reactions of ZrSi_2, Zrand Zr_2 Siwhich synthesized by melting powders eutectic reaction with C and pyrolytic carbon in the raw materials. ZrO_2 is not found in the final products.
SiC-ZrC coatings with thickness of 20-50 μm were deposited by the reactive metal infiltration(RMI) technology on C/C composites with density of 1.6 g/cm~3. The microstructure of SiC-ZrC coating and phase composition of interface between SiC-ZrC coatings and C/C composites were investigated. The results show that, good performance of SiC-ZrC coatings can be obtained by reactive infiltration method on C/C composites with 4 kinds of blending powders(Zr, Si, C and ZrO_2). The temperature first reaches the melting point of Si, which reacts with C. With the temperature increassing, both Siand Zrmelt, and the generating Gibbs free energy of ZrC is lower than SiC, so the coating is a three-layer structure of SiC-ZrC-SiC from inside to outside, and all samples are infiltrated with ZrC and SiC at different depths. SiC is the green granular and bulk phase, and ZrC is the white block phase under observing by polarizing microscope. SiC and ZrC are produced by the reactions of ZrSi_2, Zrand Zr_2 Siwhich synthesized by melting powders eutectic reaction with C and pyrolytic carbon in the raw materials. ZrO_2 is not found in the final products.
引文
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[3]YIN J,XIONG X,ZHANG H B,et al.Microstructure and ablation performances of dual-matrix carbon/carbon composites[J].Carbon,2006,44(9):1690-1694.
[4]JACOBSON N S,CURRY D M.Oxidation microstructure studies of reinforced carbon/carbon[J].Carbon,2006,44(7):1142-1150.
[5]MA J,XU Y D,ZHANG L T,et al.Microstructure characterization and tensile behavior of 2.5D C/Si C composites fabricated by chemical vapor infiltration[J].Scripta Materialia,2006,54(11):1967-1971.
[6]ZHAO D,ZHANG CH R,HU H F,et al.Ablation behavior and mechanism of 3D C/Zr C composite in oxyacetylene torch environment[J].Composites Science and Technology,2011,71(11):1392-1396.
[7]WANG D,ZENG Y,XIONG X,et al.Ablation behavior of Zr B2-Si C protective coating for carbon/carbon composites[J].Ceramics International,2015,41(6):7677-7686.
[8]ZHOU W,YI M Z,PENG K,et al.Preparation of a C/C-Cu composite with Mo2C coatings as a modification interlayer[J].Materials Letters,2015,145:264-268.
[9]ZHOU W Y,RAN L P,PENG K,et al.Effect of carbon/carbon preform density on the microstructure and properties of mo2c interlayer-modified carbon/carbon-copper composites for sliding contact materials[J].Advanced Engineering Materials,2016,18(2):277-283.
[10]YANG X,SU ZH A,HUANG Q ZH,et al.Preparation and oxidation resistance of mullite/Si C coating for carbon materials at 1 150℃[J].Transactions of Nonferrous Metals Society of China,2012,22(12):2997-3002.
[11]CHEN Z,WU W,CHENG H,et al.Microstructure and evolution of iridium coating on the C/C composites ablated by oxyacetylene torch[J].Acta Astronautica,2010,66(5/6):682-687.
[12]MUMTAZ K,J ECHIGOYA,T HIRAI,et al.Iridium coatings on carbon-carbon composites produced by two different sputtering methods:A comparative study[J].Journal of Materials Science Letters,1993,12(12):1411-1412.
[13]舒武炳,郭海明,乔生儒,等.化学气相沉积法制备Ti C涂层的相组成和表面形貌[J].西北工业大学学报,2000(2):229-232.SHU Wubing,GUO Haiming,QIAO Shengru,et al.Phase composition and surface morphology of Ti C coating by chemical vapor deposition[J].Journal of Northwestern Polytechnical University,2000(2):229-232.
[14]王坤杰,郭全贵,史景利,等.在位反应制备Ti C涂层的动力学研究[J].材料工程,2007(z1):169-171.WANG Kunjie,GUO Quangui,SHI Jingli,et al.Study on Kinetic Properties of Ti C Coatings prepared by in-situ Reaction[J].Materials Engineering,2007(z1):169-171.
[15]SUN W,XIONG X,HUANG B Y,et al.Zr C ablation protective coating for carbon/carbon composites[J].Carbon,2009,47(14):3368-3371.
[16]LIU Q,ZHANG L,CHENG L,et al.Chemical vapour deposition of zirconium carbide and silicon carbide hybrid whiskers[J].Materials Letters,2010,64(4):552-554.
[17]LIU Q,ZHANG L,JIANG F,et al.Laser ablation behaviors of Si C-Zr C coated carbon/carbon composites[J].Surface and Coatings Technology,2011,205(17/18):4299-4303.
[18]WANG Y J,CHEN Z,YU S J,et al.Ablation behaviour of a Ta C coating on Si C coated C/C composites at different temperatures[J].Ceramics International,2013,39(1):359-365.
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[23]CHENA H M,XIANG Y,WANG S,et al.Thermodynamic assessment of the C-Si-Zr system[J].Journal of Alloys and Compounds,2009,474:76-80.