摘要
杂质气体在ZrCo合金表面的吸附行为对其储氢性能具有重要的影响.采用基于赝势平面波法的第一性原理对空气中的O_(2)在ZrCo(110)表面的吸附行为进行了研究.对O_(2)在合金表面所有稳定吸附构型进行吸附能分析以及电荷分析的结果表明:O_(2)吸附的最稳定构型为B3(Zr—Co桥位),在该位点的吸附能为−8.124 eV.该构型的态密度和差分电荷密度的结果表明:O_(2)在ZrCo(110)表面该位点的吸附属于强化学吸附,O—O键发生断裂.O原子与ZrCo(110)表面原子的成键本质为O原子的电子和周围表面原子的电子发生电子轨道重叠,即O原子的2s、2p轨道电子与表面的Zr原子的4p、4d轨道电子和Co原子的3d轨道电子发生了电子轨道重叠,出现了轨道杂化现象.研究结果对后续揭示ZrCo合金储氢材料在杂质气体中的毒化机制具有积极作用.
The adsorption behavior of impurity gases on the surface of alloy ZrCo has an important influence on its hydrogen storage performance.The adsorption behavior of O_(2)on the ZrCo(110)surface was investigated with the first principles based on the pseudopotential plane wave method.The results of adsorption energy and charge analysis show that,the most stable geometry configuration was B3(the Zr—Co bridge site)where the adsorption energy was–8.124 eV.The analysis of the density of states and the differential charge density show that,the adsorption behavior of O_(2)on the ZrCo(110)surface is a strong chemical adsorption,where the oxygen-oxygen bond breaks.The essence of bonding between atom O and the ZrCo(110)surface atom is that the electron orbit of atom O overlaps with the electron orbit of the surface atom,i.e.the 2s and 2p orbital electrons of atom O overlapped with the 4p and 4d orbital electrons of atom Zr and the 3d orbital electrons of atom Co on the surface.The research results make senses in revealing the poisoning mechanism of alloy ZrCo in impurity gases.
作者
赵世祥
曾祥国
王云天
严义刚
ZHAO Shixiang;ZENG Xiangguo;WANG Yuntian;YAN Yigang(Key Laboratory of Deep Earth Science and Engineering,Ministry of Education,College of Architecture&Environment,Sichuan University,Chengdu 610065,P.R.China;School of Urban Construction,Chengdu Polytechnic,Chengdu 610041,P.R.China;Institute of New Energy and Low-Carbon Technology,Sichuan University,Chengdu 610065,P.R.China)
出处
《应用数学和力学》
CSCD
北大核心
2023年第2期152-159,共8页
Applied Mathematics and Mechanics
基金
国家自然科学基金委员会-中国工程物理研究院联合重点基金(U2130208)。
