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金属学报  2018, Vol. 54 Issue (2): 325-338    DOI: 10.11900/0412.1961.2017.00459
  本期目录 | 过刊浏览 |
ODS钢中氧化物/铁素体界面捕氢行为的第一原理研究
冯宇超1,2, 邢炜伟3, 王寿龙1,2, 陈星秋1(), 李殿中1, 李依依1
1 中国科学院金属研究所沈阳材料科学国家研究中心 沈阳 110016
2 中国科学技术大学材料科学与工程学院 沈阳 110016
3 中国科学院金属研究所 沈阳 110016
First-Principles Study of Hydrogen Behaviors at Oxide/Ferrite Interface in ODS Steels
Yuchao FENG1,2, Weiwei XING3, Shoulong WANG1,2, Xingqiu CHEN1(), Dianzhong LI1, Yiyi LI1
1 Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences, Shenyang 110016, China
2 School of Materials Science and Engineering, University of Science and Technology of China, Shenyang 110016, China
3 Institute of Metal Research, Chinese Academy of Sciences, Shenyang 110016, China
引用本文:

冯宇超, 邢炜伟, 王寿龙, 陈星秋, 李殿中, 李依依. ODS钢中氧化物/铁素体界面捕氢行为的第一原理研究[J]. 金属学报, 2018, 54(2): 325-338.
Yuchao FENG, Weiwei XING, Shoulong WANG, Xingqiu CHEN, Dianzhong LI, Yiyi LI. First-Principles Study of Hydrogen Behaviors at Oxide/Ferrite Interface in ODS Steels[J]. Acta Metall Sin, 2018, 54(2): 325-338.

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摘要: 

通过第一原理计算系统研究了氧化物弥散强化钢(ODS钢)中H原子在氧化物析出相Y2TiO5和Y2Ti2O7间隙的占位能;计算了H在Y2Ti2O7/bcc-Fe界面的占位能,分析发现这些H原子占位均容易固溶在电荷密度较高的间隙位置。计算也进一步揭示,在界面处Fe空位更容易形成;H原子倾向于占据Y2Ti2O7/bcc-Fe界面中Fe相一侧,而He原子则容易占据氧化物一侧,这表明在ODS钢中H原子会优先被氧化物沉淀相与基体间界面所吸收。ODS钢中大量弥散析出的纳米氧化物与基体间的界面结构,客观上实现了H原子的有效分散,并能够将H团簇稳定在更细小的尺度;而且在界面H团簇长大过程中会吸收大量的H原子和空位,可能以此作为辐照离位损伤缺陷的自愈合点,从而解释了ODS钢优越的耐辐照损伤性能。同时,计算也尝试解释了H-He双粒子辐照对ODS钢辐照空洞的产生存在协同效应的实验结果。

关键词 ODS钢Y2Ti2O7/bcc-Fe界面H第一原理计算    
Abstract

Ferritic oxide dispersion strengthened (ODS) steels, which usually contain a very high density of nano-sized Y-Ti-O particles and oxide precipitates (Y2Ti2O7 or/and Y2TiO5), have been demonstrated to be a leading candidate for promising structural materials in advanced fission and fusion energy applications. By means of first-principles calculations, the defect formation energies and preference sites of hydrogen (H) and helium (He) atoms trapped in Y2Ti2O7, Y2TiO5 and Y2Ti2O7/bcc-Fe interface, were investigated. The calculations uncover that (1) H atoms prefer to occupy the interstitial sites with high pre-exsiting charge densities of Y2Ti2O7 and Y2TiO5, (2) the Y2Ti2O7/bcc-Fe interface trends to attract vacancies in bcc-Fe matrix because of its lower vacancy formation energies, (3) at the Y2Ti2O7/bcc-Fe interface, H at om prefers to occupy the interstitial sites around the bcc-Fe side while He atom prefers to occupy the interstitial sites around Y2Ti2O7 side. All these results demonstrate that both H and He atoms produced by nuclear transmutation reactions would be trapped by oxides precipitates and Y2Ti2O7/bcc-Fe interface in case of the formation of large bubbles. This implies that high density of nanometer-sized oxide precipitates and Y2Ti2O7/bcc-Fe interfaces in ODS steels effectively disperse H atoms and inhibit H clusters in finer size. Besides that, during the growth process of the finer H clusters at interfaces they trap a large number of both H atoms and vacancies, acting as self-healing sites for irradiation damage. These facts potentially corresponds to the excellent capability of ODS steels to resist irradiation damage. Moreover, the calculation results may also interpret the synergistic effect of irradiation damage produced by both H and He to ODS steels.

Key wordsODS steel    Y2Ti2O7/bcc-Fe interface    hydrogen    first-principles calculation
收稿日期: 2017-11-01     
基金资助:国家自然科学基金项目No.51474202
作者简介: 作者简介 冯宇超,男,1994年生,硕士生
图1  Y2Ti2O7和Y2TiO5晶体结构
Method a / nm B / GPa
PAW-PBE 0.283 188
Calculated 0.276~0.287[48,49,50,51,52,53,54,55,56,57] 169~182[53~55,58~60]
Experimental 0.287[61] 168[62]
表1  bcc-Fe晶格常数和体模量
Method a / nm B / GPa
PAW-PBE 1.019 182
Calculated 1.000, 1.017, 209, 183,
1.020[63], 1.011[64] 181[63], 193[64]
Experimental 1.009~1.010[65,66,67] 170, 190, 192[68]
表2  Y2Ti2O7晶格常数和体模量
Method Lattice constant / nm B / GPa
a b c
PAW-PBE 1.045 0.372 1.135 149
Calculated[63] 1.046 0.373 1.137 128
Experimental[69] 1.035 0.370 1.125 -
表3  Y2TiO5晶格常数和体模量
图2  Y2Ti2O7中八面体和四面体间隙、Y2TiO5中多面体间隙位置A和B和通道间隙位置C
图3  H团簇在Y2TiO5和Y2Ti2O7的缺陷形成能
图4  Y2TiO5中H在间隙中的晶面电子定域函数图
图5  Y2Ti2O7中H在间隙中的晶面电子定域函数图
图6  计算中采用的界面匹配关系
图7  bcc-Fe(100)/Y2Ti2O7(100)界面配位方式以及体系总能随界面距离变化曲线
图8  计算中采用的界面模型和对应的Y/Ti-bridge界面结构
图9  富Y/Ti界面上各种H原子间隙占位和对应的界面俯视图
图10  单个H原子在Y2TiO5、Y2Ti2O7、bcc-Fe、bcc-Fe/Y2Ti2O7 界面中的H缺陷形成能
图11  含有H缺陷的代表性晶面的局域电荷密度等高线图和相应的三维电荷密度等值图(等值面值为0.6)
图12  富Y/Ti界面结构中不同位置H原子与其近邻原子态密度图
图13  富Y/Ti界面结构中H和He团簇的间隙占位
图14  单个He原子、H-He团簇、单个H原子在bcc-Fe/Y2Ti2O7 界面中的缺陷形成能
图15  Y2Ti2O7/bcc-Fe界面捕获H、He的机制图
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