锆合金表面CrAl基耐高温涂层及氧化行为研究
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摘要
目的了解锆合金和涂层的高温氧化行为,通过表面涂层提升锆合金的耐高温氧化性能。方法采用多弧离子镀技术在锆合金基体上制备了CrAlN、CrTiAlN涂层,模拟反应堆失水(LOCA)事故时的高温氧化行为,在360～1160℃下进行1 h氧化测试,对原始锆合金和带涂层样品的氧化增重行为进行了研究。通过X射线衍射和扫描电子显微镜对氧化前后样品的物相结构和形貌进行系统表征分析。结果锆合金在760℃及以下形成深色的混合型锆氧化膜,在860℃以上呈现龟裂和局部剥落。两种涂层氧化时,通过形成致密的Cr_2O_3和Al_2O_3混合氧化层,显著降低了氧化增重。CrAlN涂层在760℃时具有较好的抗氧化性,1060℃时开裂而失去保护作用。CrTiAlN涂层在860℃时能保护基体不受氧化,1060℃时局部开裂,基体开始出现氧化层。结论利用多弧离子镀技术制备的锆合金表面CrAlN和CrTiAlN涂层,在模拟反应堆LOCA事故下具有良好的耐高温氧化性,显示出这两种涂层有潜力发展成为核用事故容错燃料(ATF)包壳涂层。
The work aims to understand high-temperature oxidation behavior of zircaloy and coatings, and to improve high temperature oxidation resistance of zircaloy. CrAlN and CrTiAlN coatings were deposited on zirconium alloys by adopting multi-arc ion plating technique, high-temperature oxidation behavior in loss of coolant accident(LOCA) in nuclear power plant was simulated, oxidation tests were conducted for 1 h at 360～1160 ℃ to study oxidation weight gain behavior of original zirconium alloy and coated samples. X-ray diffractometer and scanning electron microscope were used to systematically characterize and analyze phase structure and morphology of the samples before and after oxidation. Fuscous mixed zirconium oxide film was formed on the surface of zirconium alloy at the temperature below 760 ℃, and the film presented cracking and local spalling at the temperature over 860 ℃. Both coatings significantly decreased the oxidation weight gain by forming a dense Cr_2O_3 and Al_2O_3 oxide layer. CrAlN coatings showed good oxidization resistance at 760 ℃ and lose protective effect at 1060 ℃; CrTiAlN coatings protected the substrate from oxidization at 860 ℃, oxide layer appeared on partially fractured substrate at 1060 ℃. CrAlN and CrTiAlN coatings can be potentially good candidates for accident tolerant fuel(ATF) cladding coatings since such coatings prepared by virtue of multi-arc ion plating technique exhibit excellent high-temperature oxidation resistance in simulated LOCA in reactors.
The work aims to understand high-temperature oxidation behavior of zircaloy and coatings, and to improve high temperature oxidation resistance of zircaloy. CrAlN and CrTiAlN coatings were deposited on zirconium alloys by adopting multi-arc ion plating technique, high-temperature oxidation behavior in loss of coolant accident(LOCA) in nuclear power plant was simulated, oxidation tests were conducted for 1 h at 360～1160 ℃ to study oxidation weight gain behavior of original zirconium alloy and coated samples. X-ray diffractometer and scanning electron microscope were used to systematically characterize and analyze phase structure and morphology of the samples before and after oxidation. Fuscous mixed zirconium oxide film was formed on the surface of zirconium alloy at the temperature below 760 ℃, and the film presented cracking and local spalling at the temperature over 860 ℃. Both coatings significantly decreased the oxidation weight gain by forming a dense Cr_2O_3 and Al_2O_3 oxide layer. CrAlN coatings showed good oxidization resistance at 760 ℃ and lose protective effect at 1060 ℃; CrTiAlN coatings protected the substrate from oxidization at 860 ℃, oxide layer appeared on partially fractured substrate at 1060 ℃. CrAlN and CrTiAlN coatings can be potentially good candidates for accident tolerant fuel(ATF) cladding coatings since such coatings prepared by virtue of multi-arc ion plating technique exhibit excellent high-temperature oxidation resistance in simulated LOCA in reactors.
引文
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[26]VAZ F,REBOUTA L,ANDRITSCHKY M,et al.Thermal oxidation of Ti1-xAlxN coatings in air[J].Journal of the European ceramic society,1997,17(15-16):1971-1977.
[2]OTT L J,ROBB K R,WANG D.Preliminary assessment of accident-tolerant fuels on LWR performance during normal operation and under DB and BDB accident conditions[J].Journal of nuclear materials,2014,448:520-533.
[3]BRAGG-SITTION S M.Development of advanced accident tolerant fuels for commercial light water reactors[J].Nuclear news,2014,57:83-91.
[4]杨红艳,张瑞谦,彭小明,等.锆合金包壳表面涂层研究进展[J].表面技术,2017,46(1):69-77.YANG Hong-yan,ZHANG Rui-qian,PENG Xiao-ming,et al.Research progress regarding surface coating of zirconium alloy cladding[J].Surface technology,2017,46(1):69-77.
[5]柏广海,陈志林,张晏玮,等.核燃料包壳锆合金表面涂层研究进展[J].稀有金属材料与工程,2017(7):2035-2040.BAI Guang-hai,CHEN Zhi-lin,ZHANG Yan-wei,et al.Research progress of coating on zirconium alloy for nuclear fuel cladding[J].Rare metal materials&engineering,2017(7):2035-2040.
[6]PARK J H,KIM H G,PARK J Y,et al.High temperature steam-oxidation behavior of arc ion plated Cr coatings foraccident tolerant fuel claddings[J].Surface&coatings technology,2015,280:256-259.
[7]ZHONG W,MOUCHE P A,HAN X,et al.Performance of iron-chromium-aluminum alloy surface coatings on zircaloy 2 under high-temperature steam and normal BWR operating conditions[J].Journal of nuclear materials,2016,470(12):327-338.
[8]FENG Z,KE P,HUANG Q,et al.The scaling behavior and mechanism of Ti2Al C MAX phase coatings in air and pure water vapor[J].Surface&coatings technology,2015,272:380-386.
[9]KUPRIN A S,BELOUS VА,VOYEVODIN V N,et al.Vacuum-arc chromium-based coatings for protection of zirconium alloys from the high-temperature oxidation in air[J].Journal of nuclear materials,2015,465:400-406.
[10]ALAT E,MOTTA A T,COMSTOCK R J,et al.Multilayer(TiN,TiAlN)ceramic coatings for nuclear fuel cladding[J].Journal of nuclear materials,2016,478:236-244.
[11]HOFMANN S,JEHN H A.Oxidation behavior of Cr Nand(Cr,Al)N hard coatings[J].Werkstoffe korros,1990,41(12):756.
[12]KAWATE M,HASHIMOTO A K,SUZUKI T.Oxidation resistance of Cr1-xAlxN and Ti1-xAlxN films[J].Surface&coatings technology,2003,165(2):163-167.
[13]CHIM Y C,DING X Z,ZENG X T,et al.Oxidation resistance of TiN,CrN,TiAlN and CrAlN coatings deposited by lateral rotating cathode arc[J].Thin solid films,2009,517(17):4845-4849.
[14]余春燕,王社斌,尹小定,等.Cr AlN薄膜高温抗氧化性的研究[J].稀有金属材料与工程,2009,38(6):1015-1018.YU Chun-yan,WANG Shen-bin,YIN Xiao-ding,et al.Study on high-temperature oxidation resistance of Cr AlNcoatings[J].Rare metal materials&engineering,2009,38(6):1015-1018.
[15]FENG Y,ZHANG L,KE R,et al.Thermal stability and oxidation behavior of AlTiN,AlCrN and AlCrSi WNcoatings[J].International journal of refractory metals&hard materials,2014,43(12):241-249.
[16]XU Y X,RIEDL H,HOLEC D,et al.Thermal stability and oxidation resistance of sputtered Ti,Al,Cr,N hard coatings[J].Surface&coatings technology,2017,324:48-56.
[17]DANEK M,FERNANDES F,CAVALEIRO A,et al.Influence of Cr additions on the structure and oxidation resistance of multilayered TiAlCrN films[J].Surface&coatings technology,2017,313:158-167.
[18]FORSEN R,JOHANSSON M P,ODEN M,et al.Effects of Ti alloying of AlCrN coatings on thermal stability and oxidation resistance[J].Thin solid films,2013,534(5):394-402.
[19]魏永强,文振华,蒋志强,等.大颗粒缺陷在电弧离子镀所制备薄膜中的分布状态研究[J].真空,2013,50(6):7-10.WEI Yong-qiang,WEN Zhen-hua,JIANG Zhi-qiang,et al.Research of macroparticles distribution in the films prepared by arc ion plating[J].Vacuum,2013,50(6):7-10.
[20]HARRIS S G,DOYLE E D,WONG Y C,et al.Reducing the macroparticle content of cathodic arc evaporated TiNcoatings[J].Surface&coatings technology,2004,183(2):283-294.
[21]LEMBKE M I,LEWIS D B,MUNZ W D.Localised oxidation defects in Ti AlN/Cr N superlattice structured hard coatings grown by cathodic arc/unbalanced magnetron deposition on various substrate materials[J].Surface&coatings technology,2000,125(1):263-268.
[22]冯长杰,辛丽,李明升,等.电弧离子镀梯度(Ti,Al)N薄膜的结构与抗氧化性能[J].中国腐蚀与防护学报,2008,28(1):1-6.FENG Chang-jie,XIN Li,LI Ming-sheng,et al.Structure and oxidation behavior of gradient(Ti,Al)N film prepared by arc ion plating[J].Journal of Chinese society for corrosion&protection,2008,28(1):1-6.
[23]LIN J,MISHRA B,MOORE J J,et al.A study of the oxidation behavior of CrN and CrAlN thin films in air using DSC and TGA analyses[J].Surface&coatings technology,2008,202(14):3272-3283.
[24]周邦新,蒋有荣.锆-2合金在500~800℃空气中氧化过程的研究[J].核动力工程,1990(3):41-47.ZHOU Bang-xin,JIANG You-rong.Oxidation of zircaloy-2 in air from 500 to 800℃[J].Nuclear power engineering,1990(3):41-47.
[25]刘文庆,周邦新,李强,等.不同介质对Zr-4合金氧化膜结构的影响[J].稀有金属材料与工程,2005,34(4):562-564.LIU Wen-qing,ZHOU Bang-xin,LI Qiang,et al.Effect of different kinds of media on oxide of zircaloy-4[J].Rare metal materials&engineering,2005,34(4):562-564.
[26]VAZ F,REBOUTA L,ANDRITSCHKY M,et al.Thermal oxidation of Ti1-xAlxN coatings in air[J].Journal of the European ceramic society,1997,17(15-16):1971-1977.