期刊
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
卷 16, 期 27, 页码 13800-13806出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/c4cp01634c
关键词
-
资金
- DOE-EPSCoR Implementation Program: Materials for Energy Conversion
- DOE-EERE Fuel Cell Technology Program
- National Science Foundation [DMR TG-110093]
First-principles density functional theory (DFT) calculations were performed to explain the stability of catalytically active sites in Fe-N-x-C electrocatalysts, their ORR activity and ORR mechanism. The results show that the formation of graphitic in-plane Fe-N-4 sites in a carbon matrix is energetically favorable over the formation of Fe-N-2 sites. Chemisorption of ORR species O-2, O, OH, OOH, and H2O and O-O bond breaking in peroxide occur on both Fe-N-2 and Fe-N-4 sites. In addition to the favorable interaction of ORR species, the computed free energy diagrams show that elementary ORR reaction steps on Fe-N-x sites are downhill. Thus, a complete ORR is predicted to occur via a single site 4e(-) mechanism on graphitic Fe-N-x (x = 2, 4) sites. Because of their higher stability and working potential for ORR, Fe-N-4 sites are predicted to be prime candidate sites for ORR in pyrolyzed Fe-N-x-C electrocatalysts.
作者
我是这篇论文的作者
点击您的名字以认领此论文并将其添加到您的个人资料中。
推荐
暂无数据