>>Metal-Organic Framework-Derived Graphene Mesh: A Robust Scaffold for Highly Exposed Fe-N4Active Sites toward an Excellent Oxygen Reduction Catalyst in Acid Media
题名:Metal-Organic Framework-Derived Graphene Mesh: A Robust Scaffold for Highly Exposed Fe-N4Active Sites toward an Excellent Oxygen Reduction Catalyst in Acid Media
来源:Journal of the American Chemical Society
发表年代:2022年
作者:Jingjing Li, Wei Xia,* Jing Tang,* Yong Gao, Cheng Jiang, Yining Jia, Tao Chen, Zhufeng Hou, Ruijuan Qi, Dong Jiang, Toru Asahi, Xingtao Xu, Tao Wang, Jianping He,* and Yusuke Yamauchi*
Abstract : This study demonstrates a special ultrathin N-dopedgraphene nanomesh (NGM) as a robust scaffold for highly exposedFe−N4 active sites. Signifcantly, the pore sizes of the NGM can beelaborately regulated by adjusting the thermal exfoliation conditions tosimultaneously disperse and anchor Fe−N4 moieties, ultimately leadingto highly loaded Fe single-atom catalysts (SA-Fe-NGM) and a highlyexposed morphology. The SA-Fe-NGM is found to deliver a superioroxygen reduction reaction (ORR) activity in acidic media (half-wavepotential = 0.83 V vs RHE) and a high power density of 634 mW cm−2 in the H2 /O2 fuel cell test. First-principles calculations further elucidatethe possible catalytic mechanism for ORR based on the identified Fe−N4 active sites and the pore size distribution analysis. This workprovides a novel strategy for constructing highly exposed transitionmetals and nitrogen co-doped carbon materials (M−N−C) catalysts for extended electrocatalytic and energy storage applications.