TY - JOUR
T1 - Metal-Organic Framework-Derived Graphene Mesh
T2 - A Robust Scaffold for Highly Exposed Fe-N4Active Sites toward an Excellent Oxygen Reduction Catalyst in Acid Media
AU - Li, Jingjing
AU - Xia, Wei
AU - Tang, Jing
AU - Gao, Yong
AU - Jiang, Cheng
AU - Jia, Yining
AU - Chen, Tao
AU - Hou, Zhufeng
AU - Qi, Ruijuan
AU - Jiang, Dong
AU - Asahi, Toru
AU - Xu, Xingtao
AU - Wang, Tao
AU - He, Jianping
AU - Yamauchi, Yusuke
N1 - Funding Information:
This work was partly supported by the National Natural Science Foundation of China (22005099), the China Postdoctoral Science Foundation Funded Project (Project no.: 2021M701211), the Postgraduate Research & Practice Innovation Program of Jiangsu Province (KYCX21_0208), and the JST-ERATO Y.Y. Materials Space-Tectonics Project (JPMJER2003). We thank Beijing Light Source for the use of the instruments. J.L. also thanks to the China Scholarship Council (CSC) for financial support. This work was performed in part at the Queensland node of the Australian National Fabrication Facility, a company established under the National Collaborative Research Infrastructure Strategy to provide nano and microfabrication facilities for Australia’s researchers.
Publisher Copyright:
© 2022 American Chemical Society. All rights reserved.
PY - 2022/6/1
Y1 - 2022/6/1
N2 - This study demonstrates a special ultrathin N-doped graphene nanomesh (NGM) as a robust scaffold for highly exposed Fe-N4active sites. Significantly, the pore sizes of the NGM can be elaborately regulated by adjusting the thermal exfoliation conditions to simultaneously disperse and anchor Fe-N4moieties, 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-2in the H2/O2fuel cell test. First-principles calculations further elucidate the possible catalytic mechanism for ORR based on the identified Fe-N4active 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.
AB - This study demonstrates a special ultrathin N-doped graphene nanomesh (NGM) as a robust scaffold for highly exposed Fe-N4active sites. Significantly, the pore sizes of the NGM can be elaborately regulated by adjusting the thermal exfoliation conditions to simultaneously disperse and anchor Fe-N4moieties, 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-2in the H2/O2fuel cell test. First-principles calculations further elucidate the possible catalytic mechanism for ORR based on the identified Fe-N4active 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.
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U2 - 10.1021/jacs.2c00719
DO - 10.1021/jacs.2c00719
M3 - Article
C2 - 35604393
AN - SCOPUS:85131224856
SN - 0002-7863
VL - 144
SP - 9280
EP - 9291
JO - Journal of the American Chemical Society
JF - Journal of the American Chemical Society
IS - 21
ER -