Estimations of electric field effects on the oxygen reduction reaction based on the density functional theory

被引:252
作者
Karlberg, G. S. [1 ]
Rossmeisl, J. [1 ]
Norskov, J. K. [1 ]
机构
[1] Tech Univ Denmark, Ctr Atom Scale Mat Design, Dept Phys, Nano DTU, DK-2800 Lyngby, Denmark
关键词
D O I
10.1039/b705938h
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
By varying the external electric field in density functional theory (DFT) calculations we have estimated the impact of the local electric field in the electric double layer on the oxygen reduction reaction (ORR). Potentially, including the local electric field could change adsorption energies and barriers substantially, thereby affecting the reaction mechanism predicted for ORR on different metals. To estimate the effect of local electric fields on ORR we combine the DFT results at various external electric field strengths with a previously developed model of electrochemical reactions which fully accounts for the effect of the electrode potential. We find that the local electric field only slightly affects the output of the model. Hence, the general picture obtained without inclusion of the electric field still persists. However, for accurate predictions at oxygen reduction potentials close to the volcano top local electric field effects may be of importance.
引用
收藏
页码:5158 / 5161
页数:4
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