Oxygen Coordination on Fe-N-C to Boost Oxygen Reduction Catalysis

被引：24

作者：

Shen, Hangjia ^{[1
]}

Peng, Hongjie ^{[2
]}

Cao, Rui ^{[3
]}

Yang, Liu ^{[4
]}

Gao, Yan ^{[5
]}

Turak, Ayse ^{[6
]}

Thomas, Tiju ^{[7
]}

Guo, Xuyun ^{[8
]}

Zhu, Ye ^{[8
]}

Wang, Jiacheng ^{[1
,9
]}

Yang, Minghui ^{[1
]}

机构：

[1] Chinese Acad Sci, Ningbo Inst Mat Technol & Engn, Solid State Funct Mat Res Lab, Ningbo 315201, Peoples R China

[2] Stanford Univ, Dept Chem Engn, Stanford, CA 94305 USA

[3] SLAC Natl Accelerator Lab, Stanford Synchrotron Radiat Lightsource, Menlo Pk, CA 94025 USA

[4] Beijing Univ Chem Technol, Beijing Adv Innovat Ctr Soft Matter Sci & Engn, Beijing 100029, Peoples R China

[5] Univ Elect Sci & Technol China, Sch Automat Engn, Chengdu 611731, Peoples R China

[6] McMaster Univ, Dept Engn Phys, Hamilton, ON L8S 4L7, Canada

[7] Indian Inst Technol Madras, Dept Met & Mat Engn, Chennai 600036, Tamil Nadu, India

[8] Hong Kong Polytech Univ, Dept Appl Phys, Hung Hom, Hong Kong, Peoples R China

[9] Chinese Acad Sci, Shanghai Inst Ceram, State Key Lab High Performance Ceram & Superfine, Shanghai 200050, Peoples R China

来源：

JOURNAL OF PHYSICAL CHEMISTRY LETTERS | 2021年 / 12卷 / 01期

基金：

中国博士后科学基金;

关键词：

ACTIVE-SITES; ELECTROCATALYSTS; OXIDATION; PERFORMANCE; SELECTIVITY;

D O I：

10.1021/acs.jpclett.0c02812

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 coordination environments of iron (Fe) in Fe-N-C catalysts determine their intrinsic activities toward oxygen reduction reactions (ORR). The precise atomic-level regulation of the local coordination environments is thus of critical importance yet quite challenging to achieve. Here, atomically dispersed Fe-N-C catalyst with O-Fe-N2C2 moieties is thoroughly studied for ORR catalysis. Advanced synchrotron X-ray characterizations, along with theoretical modeling, explicitly unraveled the penta-coordinated nature of the Fe center in the catalytic domain and the energetically optimized ORR pathways on the well-tailored O-Fe-N2C2 moieties. The combined structure identification from both experiments and theory provides an opportunity to understand the role of the coordination environments in directing the catalytic activity of single-atom or single-site catalysts; not only the center metal atom but also the whole coordinating atoms participate in the catalytic cycle.

引用

页码：517 / 524

页数：8

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