Pt基电极材料硫中毒机理的计算机模拟研究  

A first principles study on the mechanism of sulfur poisoning for Pt-based electrode materials

作　　者：沈凯[1] 张岩星[1] 王金龙[1] 路战胜[1] 杨宗献[1] 

机构地区：[1]河南师范大学物理与信息工程学院,新乡453007

出　　处：《原子与分子物理学报》2011年第1期156-160,共5页Journal of Atomic and Molecular Physics

基　　金：国家自然科学基金(10674042);河南省创新型科技人才队伍建设工程(104200510014);河南师范大学"大学生创新实验计划"(国家级)(081047624)

摘　　要：采用基于密度泛函理论的第一性原理方法和超原胞模型,计算并分析了Pt及Cu掺杂的Pt基合金的表面态密度,以及S在Pt及Pt基合金表面的吸附能和态密度情况.考虑了多种掺杂体系及吸附构型,结果表明:Cu掺杂会降低Pt基体系表面费米能级附近态密度,Pt皮肤的存在可以有效地减小Cu掺杂对体系表面态密度的影响;与S在纯Pt表面吸附相比较,S在掺杂体系表面的吸附能较小,且S的吸附对掺杂体系费米能级附近表面态密度影响较小.以上研究结果有助于为改善Pt基电极材料的催化性能,尤其是其抗S中毒性能提供理论依据.The electronic and energetic properties of the pristine and S adsorbed Pt and Cu-doping Pt surfaces are presented by first principles method. It is found that： the peak of the density of states near to the Fermi level would be lowered by the Cu dopant, while the Pt-skin would reduce the influence of the Cu dopant on the density of states. Comparing with the undoped system, the Cu dopant will reduce the interaction between the S and Pt surface and the peak of the density of states near to the Fermi level is much less influenced by the S adsorption. The results can theoretically help to improve the catalytic properties and explain the mechanism of sulfur poisoning for Pt-based electrode materials.

关 键 词：PT Cu S中毒 掺杂 密度泛函理论 

分 类 号：O469[理学—凝聚态物理]