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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.
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.
Affiliation
  • Li J; College of Materials Science and Technology, Jiangsu Key Laboratory of Electrochemical Energy Storage Technologies, Nanjing University of Aeronautics and Astronautics, Nanjing 210016, China.
  • Xia W; School of Chemistry and Molecular Engineering, Shanghai Key Laboratory of Green Chemistry and Chemical Processes, Institute of Eco-Chongming, East China Normal University, Shanghai 200062, China.
  • Tang J; School of Chemistry and Molecular Engineering, Shanghai Key Laboratory of Green Chemistry and Chemical Processes, Institute of Eco-Chongming, East China Normal University, Shanghai 200062, China.
  • Gao Y; College of Materials Science and Technology, Jiangsu Key Laboratory of Electrochemical Energy Storage Technologies, Nanjing University of Aeronautics and Astronautics, Nanjing 210016, China.
  • Jiang C; College of Materials Science and Technology, Jiangsu Key Laboratory of Electrochemical Energy Storage Technologies, Nanjing University of Aeronautics and Astronautics, Nanjing 210016, China.
  • Jia Y; School of Chemistry and Molecular Engineering, Shanghai Key Laboratory of Green Chemistry and Chemical Processes, Institute of Eco-Chongming, East China Normal University, Shanghai 200062, China.
  • Chen T; Research Center for Biomedical Optics and Molecular Imaging, Shenzhen, Institutes of Advanced Technology, Chinese Academy of Sciences, 1068, Xueyuan Avenue, Shenzhen 518055, China.
  • Hou Z; State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou 350002, China.
  • Qi R; School of Chemistry and Molecular Engineering, Shanghai Key Laboratory of Green Chemistry and Chemical Processes, Institute of Eco-Chongming, East China Normal University, Shanghai 200062, China.
  • Jiang D; Kagami Memorial Institute for Materials Science and Engineering, Waseda University, Nishi-Waseda 2-8-26, Shinjuku-ku, Tokyo 169-0051, Japan.
  • Asahi T; Kagami Memorial Institute for Materials Science and Engineering, Waseda University, Nishi-Waseda 2-8-26, Shinjuku-ku, Tokyo 169-0051, Japan.
  • Xu X; International Center for Materials Nanoarchitectonics (WPI-MANA), National Institute for Materials Science (NIMS), 1-1 Namiki, Tsukuba 305-0044, Ibaraki, Japan.
  • Wang T; College of Materials Science and Technology, Jiangsu Key Laboratory of Electrochemical Energy Storage Technologies, Nanjing University of Aeronautics and Astronautics, Nanjing 210016, China.
  • He J; College of Materials Science and Technology, Jiangsu Key Laboratory of Electrochemical Energy Storage Technologies, Nanjing University of Aeronautics and Astronautics, Nanjing 210016, China.
  • Yamauchi Y; Kagami Memorial Institute for Materials Science and Engineering, Waseda University, Nishi-Waseda 2-8-26, Shinjuku-ku, Tokyo 169-0051, Japan.
J Am Chem Soc ; 144(21): 9280-9291, 2022 Jun 01.
Article in En | MEDLINE | ID: mdl-35604393
ABSTRACT
This study demonstrates a special ultrathin N-doped graphene nanomesh (NGM) as a robust scaffold for highly exposed Fe-N4 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 H2/O2 fuel cell test. First-principles calculations further elucidate the possible catalytic mechanism for ORR based on the identified Fe-N4 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.

Full text: 1 Collection: 01-internacional Database: MEDLINE Language: En Journal: J Am Chem Soc Year: 2022 Type: Article Affiliation country: China

Full text: 1 Collection: 01-internacional Database: MEDLINE Language: En Journal: J Am Chem Soc Year: 2022 Type: Article Affiliation country: China