Metal-Organic Framework-Derived Graphene Mesh: a Robust Scaffold for Highly Exposed Fe-N4 Active Sites toward an Excellent Oxygen Reduction Catalyst in Acid Media

作者：Li, Jingjing; Xia, Wei^*; Tang, Jing^*; Gao, Yong; Jiang, Cheng; Jia, Yining; Chen, Tao; Hou, Zhufeng; Qi, Ruijuan; Jiang, Dong; Asahi, Toru; Xu, Xingtao; Wang, Tao; He, Jianping^*; Yamauchi, Yusuke^*

来源：Journal of the American Chemical Society, 2022, 144(21): 9280-9291.

DOI：10.1021/jacs.2c00719

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.

• 单位
  中国科学院; y; 中国科学院福建物质结构研究所; 南京航空航天大学