热处理气氛对Sol-Gel法在ZrH_(1.8)表面制备氧化锆膜层的影响
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摘要
采用溶胶凝胶技术,以正丙醇锆为前驱体,在氢化锆表面制备氧化锆防氢渗透层。研究了当热处理温度为600℃时,不同热处理气氛对溶胶凝胶法制备的氧化锆膜层的截面形貌、表面形貌、物相组成以及阻氢性能的影响。利用扫描电子显微镜(SEM)、激光共聚焦显微镜(CLSM)、X射线衍射仪(XRD)和涡流测厚仪分别测试了氧化锆膜层的截面形貌、表面形貌、相结构及厚度。利用真空脱氢实验对膜层的阻氢性能进行评估。研究结果表明,当热处理气氛中有氧存在时,可在氢化锆表面制得连续、致密的氧化锆膜层;而当热处理气氛中无氧存在时,所制备的氧化锆膜层不连续、均匀性差。热处理气氛中有氧时制备的氧化锆膜层的阻氢效果较无氧时要好,膜层厚度为10.1μm,渗透降低因子(PRF)值为8.4。而不同热处理气氛对氧化锆膜层的物相组成没有显著影响,膜层主要由单斜相氧化锆M-ZrO_2和四方相氧化锆TZrO_2组成,并以单斜相氧化锆M-ZrO_2为主。
Hydrogen permeation barrier on the surface of zirconium hydride was prepared by sol-gel method.Zirconium n-propoxide was precursor in reaction system.The effects of different heat treatment atmospheres on cross-sectional morphologies,surface morphologies,phase composition and hydrogen resistance performance of the films by sol-gel method were explored with heat treatment temperature of 600 ℃.The cross-sectional morphologies,surface morphologies,phase composition and thickness were characterized by scanning election microscopy(SEM),confocal laser scanning microscope(CLSM),X-ray diffractometer(XRD) and thickness gauge,respectively.Hydrogen resistance performance was evaluated by the experiment of vacuum dehydrogenation testing.The results showed that continuous and dense zirconium oxide coatings were prepared on the surface of zirconium hydride when oxygen existed in the heat treatment atmosphere.Discontinuous and heterogeneous zirconium oxide films were prepared under the heat treatment atmosphere without oxygen.And the effects of hydrogen resistance under this condition were better than that in heat treatment atmosphere without oxygen.The thickness of zirconia was 10.1 μm and the permeation reduction factor(PRF) value was 8.4.The different heat treatment atmospheres had no remarkable effect on the phase composition of zirconia films.The phase structure of zirconia films derived from monoclinic phase M-ZrO_2 and tetragonal phase T-ZrO_2,and the films was mainly composed of monoclinic phase M-ZrO_2.
Hydrogen permeation barrier on the surface of zirconium hydride was prepared by sol-gel method.Zirconium n-propoxide was precursor in reaction system.The effects of different heat treatment atmospheres on cross-sectional morphologies,surface morphologies,phase composition and hydrogen resistance performance of the films by sol-gel method were explored with heat treatment temperature of 600 ℃.The cross-sectional morphologies,surface morphologies,phase composition and thickness were characterized by scanning election microscopy(SEM),confocal laser scanning microscope(CLSM),X-ray diffractometer(XRD) and thickness gauge,respectively.Hydrogen resistance performance was evaluated by the experiment of vacuum dehydrogenation testing.The results showed that continuous and dense zirconium oxide coatings were prepared on the surface of zirconium hydride when oxygen existed in the heat treatment atmosphere.Discontinuous and heterogeneous zirconium oxide films were prepared under the heat treatment atmosphere without oxygen.And the effects of hydrogen resistance under this condition were better than that in heat treatment atmosphere without oxygen.The thickness of zirconia was 10.1 μm and the permeation reduction factor(PRF) value was 8.4.The different heat treatment atmospheres had no remarkable effect on the phase composition of zirconia films.The phase structure of zirconia films derived from monoclinic phase M-ZrO_2 and tetragonal phase T-ZrO_2,and the films was mainly composed of monoclinic phase M-ZrO_2.
引文
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[15]Wakako A,Yoshio A.Oxygen diffusion in yttria-stabilized zirconia subjected to uniaxial stress[J].Solid State Ionics,2010,181(8-10):441.
[16]Liang J J,Wei H,Hou G C,Guan H R,Hu Z L.Progress in mechanical and physical properties of hightemperature coating materials[J].Rare Metal Materials and Engineering,2008,37(7):1134.(梁静静,韦华,侯桂臣,管恒荣,胡壮麟.高温涂层材料物理、力学性能研究进展[J].稀有金属材料与工程,2008,37(7):1134.)
[17]Hartmann P,Brezesinski T,Sann J.Defect chemistry of oxide nano-materials with high surface area:ordered mesoporous thin films of the oxygen storage catalyst Ce O2-Zr O2[J].ACS Nano,2013,7(4):2999.
[2]Barrow A T W,Toffolon-Masclet C,Almer J,Daymond M R.The role of chemical free energy and elastic strain in the nucleation of zirconium hydride[J].Journal of Nuclear Materials,2013,441(1-3):395.
[3]Olsson P A T,Massih A R,Blomqvist J,Holston A M A,Bjerkén C.Ab initio thermodynamics of zirconium hydrides and deuterides[J].Computational Materials Science,2014,86:211.
[4]Chen W D,Wang L J,Wang J W,Yan S F.Oxidation behaviors of zirconium hydride in O2and CO2[J].Rare Metal Materials and Engineering,2008,37(11):1970.(陈伟东,王力军,王建伟,闫淑芳.氢化锆在O2和CO2中的氧化行为[J].稀有金属材料与工程,2008,37(11):1970.)
[5]Zhang H F,Yang Q F,Wang Z D,Liu X Z.Study on hydrogen permeation barrier of zirconium hydride[J].Atomic Energy Science and Technology,2005,39:83.(张华峰,杨启法,王振东,刘小舟.氢化锆高温抗氢渗透涂层研究[J].原子能科学技术,2005,39:83.)
[6]Pisarev A,Tsvetkov I,Yarko S.Hydrogen permeation through membranes with cracks in protection layer[J].Fusion Engineering and Design,2007,82(15-24):2120.
[7]Popov B N.Corrosion Engineering[M].Atlanta:Elsevier,2015.327.
[8]Liu Q S,Qin L J,Chang Y,Zhao P.Study on the hydrogen permeation barrier on the surface of the zirconium hydride by the method of CO2reaction[J].Surface Technology,2005,34(2):32.(刘庆生,秦丽娟,常英,赵平.CO2反应法制备氢化锆表面氢渗透阻挡层的研究[J].表面技术,2005,34(2):32.)
[9]Chen W D,Wang L J,Han L,Chen S.Properties of hydrogen permeation barrier on the surface of zirconium hydride[J].Rare Metals,2008,27(5):473.
[10]Xiang N,Song R G,Xiang B,Li H,Wang Z X,Wang C.A study on photocatalytic activity of micro-arc oxidation Ti O2films and Ag+/MAO-Ti O2composite films[J].Applied Surface Science,2015,347:454.
[11]Zhao P,Kong X G,Zou C P.Study on hydrogen barrier of Cr-C alloy fabricated by electroplating upon zirconium hydride[J].Nuclear Power Engineering,2005,26(6):576.(赵平,孔祥巩,邹从沛.氢化锆表面电镀Cr-C氢渗透阻挡层分析[J].核动力工程,2005,26(6):576.)
[12]Xia C R,Cao H Q,Wang H,Yang P H,Meng G Y,Peng D K.Sol-gel synthesis of yttria stabilized zirconia membranes through controlled hydrolysis of zirconium alkoxide[J].Journal of Membrane Science,1999,162(1-2):181.
[13]Yan S F,Liu X D,Chen W D,Wang Z G,Xu Z G.Micro-arc oxidation film on surface of zirconium hydride in silicate system with different cathode voltages[J].Chinese Journal of Rare Metals,2015,39(10):902.(闫淑芳,刘向东,陈伟东,王志刚,徐志高.硅酸盐体系负向电压对氢化锆表面微弧氧化膜的影响[J].稀有金属,2015,39(10):902.)
[14]Yu Q H,Hao L,Li S,He D,Liu X P,Jiang L J,Wang S M.Microstructure and deuterium permeation resistance of the oxide scale prepared by initial oxidation method on vacuum solar receiver[J].Solid State Ionics,2013,231:5.
[15]Wakako A,Yoshio A.Oxygen diffusion in yttria-stabilized zirconia subjected to uniaxial stress[J].Solid State Ionics,2010,181(8-10):441.
[16]Liang J J,Wei H,Hou G C,Guan H R,Hu Z L.Progress in mechanical and physical properties of hightemperature coating materials[J].Rare Metal Materials and Engineering,2008,37(7):1134.(梁静静,韦华,侯桂臣,管恒荣,胡壮麟.高温涂层材料物理、力学性能研究进展[J].稀有金属材料与工程,2008,37(7):1134.)
[17]Hartmann P,Brezesinski T,Sann J.Defect chemistry of oxide nano-materials with high surface area:ordered mesoporous thin films of the oxygen storage catalyst Ce O2-Zr O2[J].ACS Nano,2013,7(4):2999.
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