Thermally Driven Structure and Performance Evolution of Atomically Dispersed FeN4 Sites for Oxygen Reduction

被引：483

作者：

Li, Jiazhan ^{[1
,2
]}

Zhang, Hanguang ^{[2
]}

Samarakoon, Widitha ^{[3
]}

Shan, Weitao ^{[4
]}

Cullen, David A. ^{[5
]}

Karakalos, Stavros ^{[6
]}

Chen, Mengjie ^{[2
]}

Gu, Daming ^{[1
]}

More, Karren L. ^{[5
]}

Wang, Guofeng ^{[4
]}

Feng, Zhenxing ^{[3
]}

Wang, Zhenbo ^{[1
]}

Wu, Gang ^{[2
]}

机构：

[1] Harbin Inst Technol, Sch Chem & Chem Engn, Dept MIIT Key Lab Crit Mat Technol New Energy Con, Harbin 150001, Heilongjiang, Peoples R China

[2] SUNY Buffalo, Dept Chem & Biol Engn, Buffalo, NY 14260 USA

[3] Oregon State Univ, Sch Chem Biol & Environm Engn, Corvallis, OR 97331 USA

[4] Univ Pittsburgh, Dept Mech Engn & Mat Sci, Pittsburgh, PA 15261 USA

[5] Oak Ridge Natl Lab, Ctr Nanophase Mat Sci, Oak Ridge, TN 37831 USA

[6] Univ South Carolina, Dept Chem Engn, Columbia, SC 29208 USA

来源：

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION | 2019年 / 58卷 / 52期

基金：

中国国家自然科学基金; 美国国家科学基金会;

关键词：

electrode materials; iron; nanomaterials; oxygen reduction reaction; proton-exchange membrane fuel cells; N-C CATALYSTS; ACTIVE-SITES; CATHODE CATALYSTS; METAL-CATALYSTS; DOPED CARBON; IRON; ELECTROCATALYSTS; GRAPHENE; ATOMS; POLYANILINE;

D O I：

10.1002/anie.201909312

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

FeN4 moieties embedded in partially graphitized carbon are the most efficient platinum group metal free active sites for the oxygen reduction reaction in acidic proton-exchange membrane fuel cells. However, their formation mechanisms have remained elusive for decades because the Fe-N bond formation process always convolutes with uncontrolled carbonization and nitrogen doping during high-temperature treatment. Here, we elucidate the FeN4 site formation mechanisms through hosting Fe ions into a nitrogen-doped carbon followed by a controlled thermal activation. Among the studied hosts, the ZIF-8-derived nitrogen-doped carbon is an ideal model with well-defined nitrogen doping and porosity. This approach is able to deconvolute Fe-N bond formation from complex carbonization and nitrogen doping, which correlates Fe-N bond properties with the activity and stability of FeN4 sites as a function of the thermal activation temperature.

引用

页码：18971 / 18980

页数：10

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