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Title: General synthesis and definitive structural identification of MN 4C 4 single-atom catalysts with tunable electrocatalytic activities

Abstract

Single-atom catalysts (SACs) have recently attracted broad research interest as they combine the merits of both homogeneous and heterogeneous catalysts. Rational design and synthesis of SACs are of immense significance but have so far been plagued by the lack of a definitive correlation between structure and catalytic properties. Here, we report a general approach to a series of monodispersed atomic transition metals (for example, Fe, Co, Ni) embedded in nitrogen-doped graphene with a common MNsub>4C 4 moiety, identified by systematic X-ray absorption fine structure analyses and direct transmission electron microscopy imaging. The unambiguous structure determination allows density functional theoretical prediction of MNsub>4C 4 moieties as efficient oxygen evolution catalysts with activities following the trend Ni > Co > Fe, which is confirmed by electrochemical measurements. Determination of atomistic structure and its correlation with catalytic properties represents a critical step towards the rational design and synthesis of precious or nonprecious SACs with exceptional atom utilization efficiency and catalytic activities.

Authors:
 [1]; ORCiD logo [2];  [3]; ORCiD logo [4];  [1];  [1];  [1];  [1];  [1]; ORCiD logo [1];  [2]; ORCiD logo [5];  [2];  [1];  [2];  [6];  [7];  [2];  [5];  [4] more »;  [1];  [1] « less
  1. Univ. of California, Los Angeles, CA (United States)
  2. Chinese Academy of Sciences (CAS), Beijing (China)
  3. Hunan Univ., Changsha (China)
  4. Univ. of Oxford (United Kingdom); Science and Technology Facilities Council (STFC), Harwell Campus, Oxford (United Kingdom). Diamond Light Source, Ltd.
  5. Tsinghua Univ., Beijing (China)
  6. King Saud Univ., Riyadh (Saudi Arabia)
  7. Brookhaven National Lab. (BNL), Upton, NY (United States)
Publication Date:
Research Org.:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1425042
Report Number(s):
BNL-200041-2018-JAAM
Journal ID: ISSN 2520-1158
Grant/Contract Number:  
SC0012704
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Nature Catalysis
Additional Journal Information:
Journal Volume: 1; Journal Issue: 1; Journal ID: ISSN 2520-1158
Country of Publication:
United States
Language:
English
Subject:
77 NANOSCIENCE AND NANOTECHNOLOGY; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Fei, Huilong, Dong, Juncai, Feng, Yexin, Allen, Christopher S., Wan, Chengzhang, Volosskiy, Boris, Li, Mufan, Zhao, Zipeng, Wang, Yiliu, Sun, Hongtao, An, Pengfei, Chen, Wenxing, Guo, Zhiying, Lee, Chain, Chen, Dongliang, Shakir, Imran, Liu, Mingjie, Hu, Tiandou, Li, Yadong, Kirkland, Angus I., Duan, Xiangfeng, and Huang, Yu. General synthesis and definitive structural identification of MN4C4 single-atom catalysts with tunable electrocatalytic activities. United States: N. p., 2018. Web. doi:10.1038/s41929-017-0008-y.
Fei, Huilong, Dong, Juncai, Feng, Yexin, Allen, Christopher S., Wan, Chengzhang, Volosskiy, Boris, Li, Mufan, Zhao, Zipeng, Wang, Yiliu, Sun, Hongtao, An, Pengfei, Chen, Wenxing, Guo, Zhiying, Lee, Chain, Chen, Dongliang, Shakir, Imran, Liu, Mingjie, Hu, Tiandou, Li, Yadong, Kirkland, Angus I., Duan, Xiangfeng, & Huang, Yu. General synthesis and definitive structural identification of MN4C4 single-atom catalysts with tunable electrocatalytic activities. United States. doi:10.1038/s41929-017-0008-y.
Fei, Huilong, Dong, Juncai, Feng, Yexin, Allen, Christopher S., Wan, Chengzhang, Volosskiy, Boris, Li, Mufan, Zhao, Zipeng, Wang, Yiliu, Sun, Hongtao, An, Pengfei, Chen, Wenxing, Guo, Zhiying, Lee, Chain, Chen, Dongliang, Shakir, Imran, Liu, Mingjie, Hu, Tiandou, Li, Yadong, Kirkland, Angus I., Duan, Xiangfeng, and Huang, Yu. Mon . "General synthesis and definitive structural identification of MN4C4 single-atom catalysts with tunable electrocatalytic activities". United States. doi:10.1038/s41929-017-0008-y.
@article{osti_1425042,
title = {General synthesis and definitive structural identification of MN4C4 single-atom catalysts with tunable electrocatalytic activities},
author = {Fei, Huilong and Dong, Juncai and Feng, Yexin and Allen, Christopher S. and Wan, Chengzhang and Volosskiy, Boris and Li, Mufan and Zhao, Zipeng and Wang, Yiliu and Sun, Hongtao and An, Pengfei and Chen, Wenxing and Guo, Zhiying and Lee, Chain and Chen, Dongliang and Shakir, Imran and Liu, Mingjie and Hu, Tiandou and Li, Yadong and Kirkland, Angus I. and Duan, Xiangfeng and Huang, Yu},
abstractNote = {Single-atom catalysts (SACs) have recently attracted broad research interest as they combine the merits of both homogeneous and heterogeneous catalysts. Rational design and synthesis of SACs are of immense significance but have so far been plagued by the lack of a definitive correlation between structure and catalytic properties. Here, we report a general approach to a series of monodispersed atomic transition metals (for example, Fe, Co, Ni) embedded in nitrogen-doped graphene with a common MNsub>4C4 moiety, identified by systematic X-ray absorption fine structure analyses and direct transmission electron microscopy imaging. The unambiguous structure determination allows density functional theoretical prediction of MNsub>4C4 moieties as efficient oxygen evolution catalysts with activities following the trend Ni > Co > Fe, which is confirmed by electrochemical measurements. Determination of atomistic structure and its correlation with catalytic properties represents a critical step towards the rational design and synthesis of precious or nonprecious SACs with exceptional atom utilization efficiency and catalytic activities.},
doi = {10.1038/s41929-017-0008-y},
journal = {Nature Catalysis},
number = 1,
volume = 1,
place = {United States},
year = {Mon Jan 08 00:00:00 EST 2018},
month = {Mon Jan 08 00:00:00 EST 2018}
}

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