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金属学报  2018, Vol. 54 Issue (8): 1187-1192    DOI: 10.11900/0412.1961.2017.00488
  本期目录 | 过刊浏览 |
La含量对Ce-La合金氢化动力学的影响
王帅鹏, 罗文华(), 李赣, 李海波, 张广丰
表面物理与化学国家重点实验室 绵阳 621907
Effect of La Content on Hydriding Kinetics of Ce-La Alloys
Shuaipeng WANG, Wenhua LUO(), Gan LI, Haibo LI, Guangfeng ZHANG
Science and Technology on Surface Physics and Chemistry Laboratory, Mianyang 621907, China
全文: PDF(1728 KB)   HTML
摘要: 

采用压降法结合原位形貌观察研究了La含量(0~10%,质量分数)对Ce-La合金氢化动力学的影响,并利用XRD和Raman光谱仪对Ce-La合金表面氧化膜的结构进行了表征。结果表明,随La含量的增加,Ce-La合金的氢化反应进程不断加快,表现为孕育期时间变短,成核速率和反应速率增大。随着La含量增加,Ce-La合金表面氧化膜中的氧空位增多,CeO2的晶格常数变大。La掺杂引起的表面氧空位缺陷增强了H原子在氧化膜中的迁移性能,使得具有更高La含量的Ce-La合金的氢化反应进程变快。

关键词 Ce-La合金La含量氧空位氢化动力学    
Abstract

Various metals, such as uranium and plutonium, have the potential to form hydride phases while environment develop so that they are exposed to low standard of hydrogen in a long time storage environment. The generation of hydride phases has safety implications, for instance the potential to cause unintended thermal excursions and to adversely alter mechanical properties. So the reaction of alloys between hydrogen is of signi?cant industrial interest. The hydrogenation kinetics characteristics of Ce-La alloys have the similarity with some actinide materials. Investigating the growth kinetics of Ce-La alloy hydride reaction sites is of fundamental importance to the development of predictive model of hydriding behavior. In this work, the effect of La content (0~10%, mass fraction) on hydriding kinetics of Ce-La alloys was studied by pressure consume curve, and the effects of La content on surface morphology and oxidation film structure of Ce-La alloy were observed by in situ OM, XRD and Raman spectra. The results show that doped La can shorten the induction period and accelerate the nucleation rate, so as to accelerate the hydriding rate. Furthermore, doped La can cause the lattice expansion and promote the formation of oxygen vacancy in the oxidation film. The apparent activation energies of pure Ce and Ce-10La alloy are 51.12 and 41.53 kJ/mol, respectively, suggesting that the diffusion barrier of hydrogen in the oxidation film of Ce-10La alloys is lower. The oxygen vacancy and the lattice expansion caused by doped La may promote the diffusion ability of hydrogen in the oxide film. Hydrogen diffusion through the oxide film decides the hydriding rate. So doped La accelerate the hydrogenation.

Key wordsCe-La alloy    La content    oxygen vacancy    hydriding kinetics
收稿日期: 2017-11-20     
ZTFLH:  O643  
基金资助:国家自然科学基金项目No.11504344
作者简介:

作者简介 王帅鹏,男,1992年生,硕士

引用本文:

王帅鹏, 罗文华, 李赣, 李海波, 张广丰. La含量对Ce-La合金氢化动力学的影响[J]. 金属学报, 2018, 54(8): 1187-1192.
Shuaipeng WANG, Wenhua LUO, Gan LI, Haibo LI, Guangfeng ZHANG. Effect of La Content on Hydriding Kinetics of Ce-La Alloys. Acta Metall Sin, 2018, 54(8): 1187-1192.

链接本文:

https://www.ams.org.cn/CN/10.11900/0412.1961.2017.00488      或      https://www.ams.org.cn/CN/Y2018/V54/I8/1187

图1  不同La含量Ce-La合金预氧化后的XRD谱
图2  不同La含量Ce-La合金表面氧化物Raman谱
图3  不同La含量Ce-La合金氢化反应压力随时间的变化
图4  不同La含量Ce-La合金氢化后的表面形貌
图5  孕育期随La含量的变化
图6  不同La含量Ce-La合金氢化速率随时间的变化曲线
图7  不同温度下Ce和Ce-10La合金氢化反应压力随时间的变化
图8  Ce和Ce-10La合金孕育期随温度变化的Arrhenius曲线
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