Structure of Fe-Nx-C Defects in Oxygen Reduction Reaction Catalysts from First-Principles Modeling

被引：181

作者：

Holby, Edward F. ^{[1
]}

Wu, Gang ^{[2
]}

Zelenay, Piotr ^{[2
]}

Taylor, Christopher D. ^{[1
]}

机构：

[1] Los Alamos Natl Lab, Mat Sci & Technol Div, Los Alamos, NM 87545 USA

[2] Los Alamos Natl Lab, Mat Phys & Applicat Div, Los Alamos, NM 87545 USA

来源：

JOURNAL OF PHYSICAL CHEMISTRY C | 2014年 / 118卷 / 26期

基金：

美国国家科学基金会;

关键词：

INITIO MOLECULAR-DYNAMICS; ELECTROCATALYSTS; POLYANILINE; TRANSITION; GRAPHENE;

D O I：

10.1021/jp503266h

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：

The structure of active sites in Fe-based nonprecious metal oxygen reduction reaction catalysts remains unknown, limiting the ability to follow a rational design paradigm for catalyst improvement. Previous studies indicate that N-coordinated Fe defects at graphene edges are the most stable such sites. Density functional theory is used for determination of stable potential oxygen reduction reaction active sites. Clusters of Fe-N-x defects are found to have N-coordination-dependent stability. Previously reported interedge structures are found to be significantly less stable than in-edge defect structures under relevant synthesis conditions. Clusters that include Fe-N-3 defects are found to spontaneously cleave the O-O bond.

引用

页码：14388 / 14393

页数：6

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