添加SnAl元素与中温烧结对Cr/Zr膜基界面结合强度的影响
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摘要
目的通过在Cr膜中添加Sn Al元素及中温液相烧结,提高锆合金膜基界面结合强度。方法在Cr靶中添加SnAl元素,制备一种均匀分布的Cr Sn Al合金靶材(原子比Cr:Sn:Al=95:4:1),并利用直流磁控溅射(DCMS)技术在锆合金表面制备约5μm厚的Cr SnAl膜层,再将CrSnAl膜层试样放入Ar保护气氛炉中进行中温烧结(温度为600℃,时间为30 min),随炉冷却至室温。利用XRD、SEM、EDS及体式显微镜分析中温烧结对Cr Sn Al膜层形貌、组织结构及元素扩散的影响;根据涂层弯曲断裂形貌、切削划痕力和切屑形貌综合评价膜基界面结合强度。结果添加SnAl后,Cr膜层表面孔隙等缺陷明显减少,膜基界面结合强度得到较大提升,从41.7 MPa提升到了45.8 MPa。600℃烧结后,Cr SnAl膜层韧性增强,并出现韧窝形貌,剪切唇仅为烧结前CrSnAl膜层的1/2,Cr Sn Al/Zr界面结合强度进一步提升到52.1 MPa。结论 Cr膜中添加SnAl有利于膜基界面元素扩散,对膜基界面结合强度提高有较大影响;中温烧结Cr Sn Al膜层韧性及膜基界面结合强度均有较大提升,进而改善了膜基界面结合性能。
The work aims to increase the bonding strength of zirconium alloy film-based interface by SnAl elements in Cr film and intermediate-temperature liquid phase sintering. SnAl element was added to Cr target to prepare a CrSnAl alloy target with an evenly distributed atomic ratio of Cr∶Sn∶Al=95∶4∶1. DC magnetron sputtering(DCMS) technology was used to prepare approximately 5 μm thick CrSnAl film on the surface of zirconium alloy and then the CrSnAl film sample was placed in an Ar atmosphere furnace for sintering at an intermediate temperature of 600 ℃ for 30 minutes and the coated sample was cooled down to room temperature with the furnace. Effect of intermediate-temperature sintering on morphology, structure and element diffusion of Cr Sn Al films was investigated by XRD, SEM, EDS and stereoscopic microscope, respectively and the film-based interface bonding strength was evaluated by coating bending fracture morphology, cutting scratch force and chip morphology. The defects such as pores on the surface of Cr film with SnAl addition were significantly reduced, and the bond strength at the interface of the film was greatly improved. The average bonding strength at the interface was increased from 41.7 MPa to 45.8 MPa. The toughness of the Cr Sn Al film after sintered at 600 ℃ was enhanced, and the dimple appearance was observed. The shear lip was only 1/2 of the pre-sintered CrSnAl film, and the CrSnAl/Zr interface bond strength was further increased to 52.1 MPa. Therefore, the addition of SnAl to the Cr film is beneficial to the diffusion of element at the interface of the film, and has a great influence on the bonding strength of the film-based interface. CrSnAl film sintered at medium temperature increases the toughness of the film and the bonding strength of the film-based interface, thus improving the interface properties of the film-based interface.
The work aims to increase the bonding strength of zirconium alloy film-based interface by SnAl elements in Cr film and intermediate-temperature liquid phase sintering. SnAl element was added to Cr target to prepare a CrSnAl alloy target with an evenly distributed atomic ratio of Cr∶Sn∶Al=95∶4∶1. DC magnetron sputtering(DCMS) technology was used to prepare approximately 5 μm thick CrSnAl film on the surface of zirconium alloy and then the CrSnAl film sample was placed in an Ar atmosphere furnace for sintering at an intermediate temperature of 600 ℃ for 30 minutes and the coated sample was cooled down to room temperature with the furnace. Effect of intermediate-temperature sintering on morphology, structure and element diffusion of Cr Sn Al films was investigated by XRD, SEM, EDS and stereoscopic microscope, respectively and the film-based interface bonding strength was evaluated by coating bending fracture morphology, cutting scratch force and chip morphology. The defects such as pores on the surface of Cr film with SnAl addition were significantly reduced, and the bond strength at the interface of the film was greatly improved. The average bonding strength at the interface was increased from 41.7 MPa to 45.8 MPa. The toughness of the Cr Sn Al film after sintered at 600 ℃ was enhanced, and the dimple appearance was observed. The shear lip was only 1/2 of the pre-sintered CrSnAl film, and the CrSnAl/Zr interface bond strength was further increased to 52.1 MPa. Therefore, the addition of SnAl to the Cr film is beneficial to the diffusion of element at the interface of the film, and has a great influence on the bonding strength of the film-based interface. CrSnAl film sintered at medium temperature increases the toughness of the film and the bonding strength of the film-based interface, thus improving the interface properties of the film-based interface.
引文
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[2]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.
[3]TANG C,STUEBER M,SEIFERT H J,et al.Protective coatings on zirconium-based alloys as accident-tolerant fuel(ATF)claddings[J].Corrosion reviews,2017,35(3):141-165.
[4]王浩然,邱长军,曾小安,等.温度对纯Cr涂层表面形貌和抗腐蚀性能的影响[J].表面技术,2017,46(6):192-196.WANG H R,QIU C J,ZENG X A,et al.Effect of temperature on morphology and corrosion resistance of pure Cr coating[J].Surface&coatings,2017,46(6):192-196.
[5]陈科培,陈志勇,刘丹,等.锆合金表面激光熔覆TiN/ZrN复合陶瓷涂层的研究[J].应用激光,2015,35(2):166-169.CHEN Ke-pei,CHEN Zhi-yong,LIU Dan,et al.Studying on laser cladding TiN/ZrN composite ceramic layer on zirconium alloy[J].Applide laser,2015,35(2):166-169.
[6]吴亚文,贺秀杰,张继龙,等.锆合金表面Cr Al基耐高温涂层及氧化行为研究[J].表面技术,2018,47(9):34-41.WU Ya-wen,HE Xiu-jie,ZHANG Ji-long,et al.Cr Albased high-temperature coatings on zirconium alloy and oxidation behavior[J].Surface technology,2018,47(9):34-41.
[7]严艳芹,邱长军,黄鹤,等.热处理温度对Cr/Al涂层组织结构及性能的影响[J].表面技术,2017,46(12):78-83.YAN Y Y,QIU C J,HUANG H.et al.Effect of heat treatment temperature on microstructure and properties of Cr/Al coatings[J].Surface technology,2017,46(12):78-83.
[8]GARNER A,HU J,HARTE A,et al.The effect of Sn concentration on oxide texture and microstructure formation in zirconium alloys[J].Acta materialia,2015,99(2-3):259-272.
[9]LUKASZKOWICZ K,SONDOR J,KRIZ A,et al.Structure,mechanical properties and corrosion resistance of nanocomposite coatings deposited by PVD technology onto the X6CrNiMoTi17-12-2 and X40CrMoV5-1 steel substrates[J].Journal of materials science,2010,45(6):1629-1637.
[10]WU Y P,ZHU S F,ZHANG Y P,et al.The adhesion strength and deuterium permeation property of SiC films synthesized by magnetron sputtering[J].International journal of hydrogen energy,2016,41(25):10827-10832.
[11]WU Y Y,JIANG L J,DI H,et al.Effect of Cr2O3 layer on the deuterium permeation properties of Y2O3/Cr2O3 composite coating prepared by MOCVD[J].International journal of hydrogen energy,2016,41(36):16101-16107.
[12]CARR J,VASDUEVAMURTHY G,SNEAD L,et al.Investigations of aluminum-doped self-healing zircaloy surfaces in context of accident-tolerant fuel cladding research[J].Materials engineering and performance,2016,25(6):2347-2355.
[13]唐伟忠.薄膜材料制备原理、技术及应用[M].北京:冶金工业出版社,2003.TANG W Z.Principle,technology and application of thin film materials[M].Beijing:Metallurgical Industry Press,2003.
[14]江炳尧,任琮欣,郑志宏,等.离子束辅助沉积铪薄膜晶粒的择优取向[J].中国有色金属学报,2003(6):1414-1419.JIANG B R,REN Z X,ZHENG Z H,et al.Preferred crystal orientation of Hf films prepared by ion beam assisted depostion[J].The Chinese journal of nonferrous metals,2003(6):1414-1419.
[15]KIM H G,KIM I H,JUNG Y I,et al.Adhesion property and high-temperature oxidation behavior of Cr-coated zircaloy-4 cladding tube prepared by 3D laser coating[J].Journal of nuclear materials,2015,465:531-539.
[16]VINCENT P G,BOURGEOIS S,MONERIE Y.Overall elastoplastic behavior of anisotropic metal-atrix composites reinforced by aligned inclusions.Application to hydrided and irradiated zircaloy-4 cladding tubes[J].Mechanics of materials,2010,42(2):175-188.
[17]钟群鹏,赵子华.断口学[M].北京:高等教育出版社,2006.ZHONG Q P,ZHAO Z H.Fracture theory[M].Beijing:Higher Education Press,2006.
[18]王雪萌,张思倩,袁子尧,等.时效处理对Ti-3Al-8V-6Cr-4Mo-4Zr合金力学性能的影响[J].材料研究学报,2017(6):409-414.WANG X M,ZHANG S Q,YUAN Z Y,et al.Effect of heat treatment on mechanical properties of Ti-3Al-8V-6Cr-4Mo-4Zr alloy[J].Chinese journal of materials research,2017(6):409-414.
[19]陈程,尹海清,曲选辉.高纯钼板断口形貌和组织分析[J].稀有金属,2007,31(1):10-13.CHEN C,YIN H Q,QU X H.Fracture and structure analysis of pure molybdenum plate[J].Chinese journal of rare metals,2007,31(1):10-13.
[20]AUDIGIE P,PUT A V,MURAKAMI H,et al.Chromium and iridium effects on the short-term interdiffusion behaviour between Pt rich?-??bond-coatings and a Ni-Al-Cr alloy[J].Surface and coatings technology,2017,309(15):258-265.
[21]张元其,王玲,杜学铭,等.泡沫Ni/Sn复合钎料超声波钎焊Al2O3陶瓷接头组织及力学性能研究[J].焊接技术,2017,46(5):43-46.ZAHNF Y Q,WANG L,DU X M,et al.Study on microstructure and mechanical properties of Al2O3 ceramic joints by ultrasonic brazing of foam Ni/Sn composites[J].Welding technology,2017,46(5):43-46.
[22]马奔驰.Sn/Al界面Al2O3过渡层形成机理及对界面结合强度的影响[D].哈尔滨:哈尔滨工业大学,2015.MA B C.Forming mechanism of Al2O3 intermediate layer at Sn/Al interface and its effect on interfacial bonding stength[D].Harbin:Harbin Institute of Technology,2015.
[23]罗广南,李文治.离子能量对薄膜附着力及界面原子混合的影响[J].薄膜科学与技术,1994(1):41-46.LUO G N,LI W Z.Influence of ion energy on adhesion of thin films and interface atomic mixing[J].Membrane science and technology,1994(1):41-46.