A Highly Efficient Fe-N-C Electrocatalyst with Atomically Dispersed FeN4 Sites for the Oxygen Reduction Reaction

被引:12
|
作者
Jin, Xinxin [1 ,2 ]
Xie, Yan [1 ]
Fu, Junhong [1 ]
Zhao, Chaoyue [1 ]
Xu, Yinghao [3 ]
Lv, Yang [3 ]
Zhang, Bingsen [4 ]
Sun, Keju [5 ]
Si, Rui [6 ]
Huang, Jiahui [1 ]
机构
[1] Chinese Acad Sci, Dalian Inst Chem Phys, Dalian Natl Lab Clean Energy, Dalian 116023, Peoples R China
[2] Univ Chinese Acad Sci, Beijing 100049, Peoples R China
[3] Dalian Univ Technol, Dalian 116024, Peoples R China
[4] Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci, Shenyang 110016, Peoples R China
[5] Yanshan Univ, Coll Environm & Chem Engn, Qinhuangdao 066004, Hebei, Peoples R China
[6] Chinese Acad Sci, Shanghai Inst Appl Phys, Shanghai Synchrotron Radiat Facil, Shanghai 201204, Peoples R China
基金
中国国家自然科学基金;
关键词
Single atom electrocatalyst; N-doped carbon; Porous structure; Oxygen reduction reaction; Density functional theory calculations; DOPED POROUS CARBONS; MOSSBAUER-SPECTROSCOPY; METAL-CATALYSTS; IRON; ALKALINE; NANOPARTICLES; RICH; ORR;
D O I
10.1002/cctc.202100132
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
Atomically dispersed Fe-N-C electrocatalysts have displayed excellent catalytic performances towards the oxygen reduction reaction (ORR), while the identification of the genuine active sites remains a challenge. Herein, we report a Fe-N-C electrocatalyst of FeSA/HNPC featuring single-atomic FeN4 sites on hierarchically N-doped porous carbon (HNPC), which shows a very competitive ORR activity in alkaline solution even at a low electrocatalyst loading of 0.2 mg cm(-2) on the working electrode. A comparison of energy barriers in ORR reveals that the single-atomic FeN4 active sites in FeSA/HNPC existing in the form of pyrrole-N-4-Fe is more favorable than that of pyridine-N-4-Fe for the enhanced ORR activity. Understanding the nature of FeN4 active sites will greatly benefit the design of Fe-N-C electrocatalysts with highly effective ORR performances.
引用
收藏
页码:2683 / 2690
页数:8
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