CAJ | 학술논문

采用基于密度泛函理论的第一性原理方法,计算并分析了 S原子在 Pt皮肤Pt3 Ni(111)面不同位置的吸附特性.结果表明：S原子在Pt皮肤Pt3 Ni的 fcc位吸附最强,吸附能为5.49 eV；与 S原子在纯净的Pt(111)表面吸附相比较,S原子在Pt皮肤Pt3 Ni(111)面相应吸附位置的吸附能变小,与近邻 Pt原子形成的 S-Pt键变长,表明掺杂的 Ni 会减小相应位点 S 原子的吸附能,降低体系对 S 原子的吸附能力,进而减弱S吸附对体系催化能力的影响；态密度分析发现,S原子的吸附使得Pt基催化剂的催化活性降低,主要是 S的2 p电子引起的；这些结果将为后续研究 Pt基合金电极抗 S中毒效果以及探究 S原子吸附后Pt3 Ni的活性位提供依据.
채용기우밀도범함이론적제일성원리방법,계산병분석료 S원자재 Pt피부Pt3 Ni(111)면불동위치적흡부특성.결과표명：S원자재Pt피부Pt3 Ni적 fcc위흡부최강,흡부능위5.49 eV；여 S원자재순정적Pt(111)표면흡부상비교,S원자재Pt피부Pt3 Ni(111)면상응흡부위치적흡부능변소,여근린 Pt원자형성적 S-Pt건변장,표명참잡적 Ni 회감소상응위점 S 원자적흡부능,강저체계대 S 원자적흡부능력,진이감약S흡부대체계최화능력적영향；태밀도분석발현,S원자적흡부사득Pt기최화제적최화활성강저,주요시 S적2 p전자인기적；저사결과장위후속연구 Pt기합금전겁항 S중독효과이급탐구 S원자흡부후Pt3 Ni적활성위제공의거.
The adsorption properties of S on the Pt skin Pt3Ni(111)surface are studied by first-principles calculations.It is found that S prefer to occupy the fcc site of Pt3Ni(111)surface with a very big adsorp-tion energy (5.49 eV).More importantly,the interaction of the sulfur with Pt surface would reduce up-on the alloy of the Pt and Ni,comparing with that of the pure Pt surface.The electronic structure analy-sis showed that the catalytic effect of Pt-based catalysts reduced is caused by 2p electron of S,and it would be shrinked from the Ni doping.The current results provide a basis for further study the active sites of Pt3Ni(111)surface with adsorbed sulfur.