Role of Local Carbon Structure Surrounding FeN4 Sites in Boosting the Catalytic Activity for Oxygen Reduction

被引:156
|
作者
Liu, Kexi [1 ]
Wu, Gang [2 ]
Wang, Guofeng [1 ]
机构
[1] Univ Pittsburgh, Dept Mech Engn & Mat Sci, Pittsburgh, PA 15261 USA
[2] Univ Buffalo State Univ New York, Dept Chem & Biol Engn, Buffalo, NY 14260 USA
来源
JOURNAL OF PHYSICAL CHEMISTRY C | 2017年 / 121卷 / 21期
基金
美国国家科学基金会;
关键词
DENSITY-FUNCTIONAL THEORY; METAL-ORGANIC FRAMEWORKS; AUGMENTED-WAVE METHOD; IRON-BASED CATALYSTS; N-C CATALYSTS; FUEL-CELLS; FE/N/C CATALYSTS; ELECTROCATALYSTS; ELECTROREDUCTION; POLYANILINE;
D O I
10.1021/acs.jpcc.7b00913
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
Development of effective nonprecious metal and nitrogen codoped carbon catalysts for the oxygen reduction reaction (ORR) requires a fundamental understanding of the mechanisms underlying their catalytic activity. In this study, we employed the first-principles density functional theory calculations to predict some key parameters (such as activation energy for O-O bond breaking and free-energy evolution as a function of electrode potential) of ORR on three FeN4-type active sites with different local carbon structures. We find that the FeN4 site surrounded by eight carbon atoms and at the edge of micropores has the lowest activation energy (about 0.20 eV) for O-O bond breaking among the three FeN4-type active sites for promoting a direct four-electron ORR. Consequently, our computational results suggest that introduction of micropores in the nonprecious metal catalysts could enhance their catalytic activity for ORR through facilitating the formation of FeN4-C-8 active sites with high specific activity.
引用
收藏
页码:11319 / 11324
页数:6
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