• 文献标题:   Metal-Organic Framework-Derived Graphene Mesh: a Robust Scaffold for Highly Exposed Fe-N-4 Active Sites toward an Excellent Oxygen Reduction Catalyst in Acid Media
  • 文献类型:   Article
  • 作  者:   LI JJ, XIA W, TANG J, GAO Y, JIANG C, JIA YN, CHEN T, HOU ZF, QI RJ, JIANG D, ASAHI T, XU XT, WANG T, HE JP, YAMAUCHI Y
  • 作者关键词:  
  • 出版物名称:   JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
  • ISSN:   0002-7863 EI 1520-5126
  • 通讯作者地址:  
  • 被引频次:   46
  • DOI:   10.1021/jacs.2c00719 EA MAY 2022
  • 出版年:   2022

▎ 摘  要

This study demonstrates a special ultrathin N-doped graphene nanomesh (NGM) as a robust scaffold for highly exposed Fe-N-4 active sites. Significantly, the pore sizes of the NGM can be elaborately regulated by adjusting the thermal exfoliation conditions to simultaneously disperse and anchor Fe-N4 moieties, ultimately leading to highly loaded Fe single-atom catalysts (SA-Fe-NGM) and a highly exposed morphology. The SA-Fe-NGM is found to deliver a superior oxygen reduction reaction (ORR) activity in acidic media (half-wave potential = 0.83 V vs RHE) and a high power density of 634 mW cm(-2) in the H-2/O-2 fuel cell test. First-principles calculations further elucidate the possible catalytic mechanism for ORR based on the identified Fe-N-4 active sites and the pore size distribution analysis. This work provides a novel strategy for constructing highly exposed transition metals and nitrogen co-doped carbon materials (M-N-C) catalysts for extended electrocatalytic and energy storage applications.