【摘要】 利用密度泛函理论(DFT)的平面波赝势方法计算了不同注入电荷和掺杂Fe原子比例的PdxFey(110)表面原子结构和电子结构特性。结果表明,Fe原子比例对表面褶皱s影响较小,注入电荷数量对表面褶皱s影响很大;Fe原子掺杂使Pd的4d10轨道电子向低能级轨道移动,增加了d空穴。布居分析表明电极的表层电荷分布比金属态表面增多;Fe掺杂的表层电荷分布比不掺杂电极表面增多。电子结构分析表明,电极表面的s、p、d轨道电子和总电子均比金属态表面减少;Fe掺杂后,Pd和Fe的表面原子趋向于杂化构型,Pd表层原子向Fe表层原子发生电子转移,增加表面反应活性,有利于电催化反应。更多还原

【Abstract】 The atomic and electronic structure of Pd( 110) and PdxFey( 110) surfaces were calculated using density functional theory( DFT) based on the plane wave pseudopotential method. The results show that the Fe atomic ratio has little effect on the surface corrugation( s),and the injection charge has a large effect on the surface corrugation. Electrons were transferred between Pd and Fe after Fe atom doping. Furthermore,the d hole in the 4d10sub-shell increased. The surface charge distribution on the electrode surface is greater than that on the metal surface. The s,d,and p electron density of the electrode surface was lower than that of the metal surface. The electrocatalytic reaction activity increased due to the hybridization of Pd and Fe surface electrons.更多还原