H、He离子辐照对国产ZIRLO合金氧化膜的影响
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摘要
针对国产ZIRLO合金开展了H、He离子辐照对其腐蚀性能影响的研究。对国产ZIRLO合金样品分别进行高温(300℃)H、He离子辐照试验,辐照峰值剂量为1dpa,之后进行模拟一回路腐蚀试验。通过腐蚀增重方法得到腐蚀动力学曲线。利用慢正电子湮没多普勒展宽谱对未辐照样品和辐照样品进行微观结构表征,用透射电子显微镜对腐蚀125d的样品进行微观结构表征。结果表明,H、He离子辐照并未改变ZIRLO合金的腐蚀机理。He离子辐照产生的空位团可促进腐蚀过程中裂纹形核,增加了氧扩散通道,减少氧扩散激活能,导致腐蚀初期有明显的加速效应。H离子辐照对腐蚀的加速现象不如He离子辐照明显,原因是H离子辐照产生H-空位复合缺陷对氧扩散激活能减少作用较小。
The corrosion behavior of domestic ZIRLO was investigated in 300℃ PWRsimulating loop after irradiation.Hydrogen and helium ions irradiation experiments were carried out at the temperature of 300℃,with the damage peak dose of 1 dpa using the injection energy of 100 keV and 150 keV respectively.The corrosion kinetics curvewas obtained by measuring weight gain of the alloy.Irradiation defects of Zr matrix and microstructure of oxide film were determined by Doppler broadening spectra based on slow positron beam and transmission electron microscope.The results illustrate that irradiation does not change the corrosion mechanism of the zirconium alloy.Vacancy clusters produced by helium ions promote the nucleation of the cracks in the corrosion process,and generate extra channels for oxygen ions and the reduction of activation energy for oxygen diffusion,leading to the obvious acceleration effect in corrosion at the initial stage.While hydrogen ions irradiation has less acceleration effect on the corrosion compared with helium ions irradiation,because complex-defect pairs composed of vacancies and hydrogen ions have little effect on the reduction of activation energy for oxygen diffusion in corrosion process.
The corrosion behavior of domestic ZIRLO was investigated in 300℃ PWRsimulating loop after irradiation.Hydrogen and helium ions irradiation experiments were carried out at the temperature of 300℃,with the damage peak dose of 1 dpa using the injection energy of 100 keV and 150 keV respectively.The corrosion kinetics curvewas obtained by measuring weight gain of the alloy.Irradiation defects of Zr matrix and microstructure of oxide film were determined by Doppler broadening spectra based on slow positron beam and transmission electron microscope.The results illustrate that irradiation does not change the corrosion mechanism of the zirconium alloy.Vacancy clusters produced by helium ions promote the nucleation of the cracks in the corrosion process,and generate extra channels for oxygen ions and the reduction of activation energy for oxygen diffusion,leading to the obvious acceleration effect in corrosion at the initial stage.While hydrogen ions irradiation has less acceleration effect on the corrosion compared with helium ions irradiation,because complex-defect pairs composed of vacancies and hydrogen ions have little effect on the reduction of activation energy for oxygen diffusion in corrosion process.
引文
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[31]PECHEUR D,LEFEBVRE F,MOTTA A T,et al.Precipitate evolution in the Zircaloy-4oxide layer[J].Journal of Nuclear Materials,1992,189(3):318-332.
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[33]PROFF C,ABOLHASSANI S,LEMAIGNAN C.Oxidation behaviour of zirconium alloys and their precipitates—A mechanistic study[J].Journal of Nuclear Materials,2013,432(1-3):222-238.
[2]刘建章.核材料科学与工程:核结构材料[M].北京:化学工业出版社,2007.
[3]袁改焕,卫新民.锆合金研究进展及我国核电站用锆材国产化的思考[J].钛工业进展,2011,28(6):18-22.YUAN Gaihuan,WEI Xinming.Progress in zirconium alloys and thinking about localization of zirconium material for domestic nuclear power plants[J].Titanium Industry Progress,2012,28(6):18-22(in Chinese).
[4] MARDON J P,CHARQUET D,SENEVAT J.Influence of composition and fabrication process on out-of-pile and in-pile properties of M5alloy[J].Optical Materials,2000,18(3):331-336.
[5] SABOL G P.ZIRLOTM—An alloy development success[J].Journal of Astm International,2005,2(2):1-22.
[6] COX B.Some thoughts on the mechanisms of inreactor corrosion of zirconium alloys[J].Journal of Nuclear Materials,2005,336(2-3):331-368.
[7] FONTANA M G,STAEHLE R W.Advances in corrosion science and technology:Volume 7[M].US:Plenum Press,1970.
[8] YILMAZBAYHAN A,BREVAL E,MOTTA A T,et al.Transmission electron microscopy examination of oxide layers formed on Zr alloys[J].Journal of Nuclear Materials,2006,349(3):265-281.
[9] ASHER R C,DAVIES D,KIRSTEIN T,et al.The effects of radiation on the corrosion of some Zr alloys[J].Corrosion Science,1970,10(10):695-707.
[10]MOTTA A T,COUET A,COMSTOCK R J.Corrosion of zirconium alloys used for nuclear fuel cladding[J].Annual Review of Materials Research,2015,45:311-343.
[11]朱升云,袁大庆.先进核能系统结构材料辐照性能研究[J].原子核物理评论,2017,34(3):302-309.ZHU Shengyun,YUAN Daqing.Study of radiation properties of structural materials for advanced nuclear energy systems[J]. Nuclear Physics Review,2017,34(3):302-309(in Chinese).
[12]ZIEGLER J F,BIERSACK J P.The stopping and range of ions in matter[J].Nuclear Instruments&Methods in Physics Research,2010,268(11-12):1 818-1 823.
[13]LEMAIGNAN C.2.07-zirconium alloys:Properties and characteristics[J].Comprehensive Nuclear Materials,2012,2(7):217-232.
[14]LEE H P,SCHERER A,BEEBE E D,et al.1.57μm InGaAsP/InP surface emitting lasers by angled focus ion beam etching[J].Electronics Letters,1992,28(6):580-582.
[15]MULLER D A.Structure and bonding at the atomic scale by scanning transmission electron microscopy[J].Nature Materials,2009,8(4):263-270.
[16]WEI J,FRANKEL P,POLATIDIS E,et al.The effect of Sn on autoclave corrosion performance and corrosion mechanisms in Zr-Sn-Nb alloys[J]. Acta Materialia, 2013, 61(11):4 200-4 214.
[17]COUET A,MOTTA A T,AMBARD A.The coupled current charge compensation model for zirconium alloy fuel cladding oxidation,Ⅰ:Parabolic oxidation of zirconium alloys[J].Corrosion Science,2015,100:73-84.
[18]MOTTA A T,SILVA M J G D,YILMAZBAYHAN A,et al.Microstructural characterization of oxides formed on model Zr alloys using synchrotron radiation[J].Journal of ASTM International,2008,5(5):101 257-101 276.
[19]KASS S.Aqueous corrosion of the zircaloys at low temperatures[J].Journal of Nuclear Materials,1969,29(3):315-321.
[20]HUANG J,YAO M Y,GAO C Y,et al.The influence of second phase particles on the crack formation in oxide films formed on zirconium alloys[J].Corrosion Science,2015,99(6):172-177.
[21]郁伟中.正电子物理及其应用[M].北京:科学出版社,2003.
[22]CHEN Z Q,KAWASUSO A,XU Y,et al.Production and recovery of defects in phosphorus-implanted ZnO[J].Journal of Applied Physics,2005,97(1):0135281-6
[23]BORDULEV Y S,LEE K,LAPTEV R S,et al.Positron spectroscopy of defects in hydrogensaturated zirconium[J].Defect&Diffusion Forum,2017,373:138-141.
[24]WAGNER C.Theroetical analysis of the diffusion processes determining the oxidation rate of the alloys[J].J Electrochem Soc,1952,99(10):369-380.
[25]陈鹤鸣,马春来,白新德,主编.核反应堆材料腐蚀及其防护[M].北京:原子能出版社,1984.
[26]TEJLAND P,THUVANDER M,HANS-OLOF A,et al.Detailed analysis of the microstructure of the metal/oxide interface region in Zircaloy-2after autoclave corrosion testing[J].Journal of ASTM International,2011,8(6):1-16.
[27]MOTT N F.The theory of the formation of protective oxide films on metals:Ⅲ[J].Transactions of the Faraday Society,1947,43:429-434.
[28]COUET A,MOTTA A T,AMBARD A.The coupled current charge compensation model for zirconium alloy fuel cladding oxidation,Ⅰ:Parabolic oxidation of zirconium alloys[J].Corrosion Science,2015,100:73-84.
[29]PROFF C,ABOLHASSANI S,DADRAS M M,et al.In situ oxidation of zirconium binary alloys by environmental SEM and analysis by AFM,FIB,and TEM[J].Journal of Nuclear Materials,2010,404(2):97-108.
[30]PROFF C,ABOLHASSANI S,LEMAIGNAN C.Oxidation behaviour of binary zirconium alloys containing intermetallic precipitates[J].Journal of Nuclear Materials,2011,416(1):125-134.
[31]PECHEUR D,LEFEBVRE F,MOTTA A T,et al.Precipitate evolution in the Zircaloy-4oxide layer[J].Journal of Nuclear Materials,1992,189(3):318-332.
[32]COX B,SHEIKH H I.Redistribution of the alloying elements during Zircaloy-2oxidation[J].Journal of Nuclear Materials,1997,249(1):17-32.
[33]PROFF C,ABOLHASSANI S,LEMAIGNAN C.Oxidation behaviour of zirconium alloys and their precipitates—A mechanistic study[J].Journal of Nuclear Materials,2013,432(1-3):222-238.