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

Huilong Fei, Juncai Dong, Yexin Feng, Christopher S. Allen, Chengzhang Wan, Boris Volosskiy, Mufan Li, Zipeng Zhao, Yiliu Wang, Hongtao Sun, Pengfei An, Wenxing Chen, Zhiying Guo, Chain Lee, Dongliang Chen, Imran Shakir, Mingjie Liu, Tiandou Hu, Yadong Li, Angus I. KirklandXiangfeng Duan, Yu Huang

Research output: Contribution to journalArticle

210 Citations (Scopus)

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 MN 4 C 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 MN 4 C 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.

Original languageEnglish (US)
Pages (from-to)63-72
Number of pages10
JournalNature Catalysis
Volume1
Issue number1
DOIs
StatePublished - Jan 1 2018

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Graphite
Transmission Electron Microscopy
Catalyst activity
Nitrogen
Metals
X-Rays
Oxygen
Atoms
Catalysts
Research
X ray absorption
Graphene
Transition metals
Transmission electron microscopy
Imaging techniques

All Science Journal Classification (ASJC) codes

  • Catalysis
  • Bioengineering
  • Biochemistry
  • Process Chemistry and Technology

Cite this

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 MN 4 C 4 single-atom catalysts with tunable electrocatalytic activities In: Nature Catalysis. 2018 ; Vol. 1, No. 1. pp. 63-72.
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title = "General synthesis and definitive structural identification of MN 4 C 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 MN 4 C 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 MN 4 C 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.",
author = "Huilong Fei and Juncai Dong and Yexin Feng and Allen, {Christopher S.} and Chengzhang Wan and Boris Volosskiy and Mufan Li and Zipeng Zhao and Yiliu Wang and Hongtao Sun and Pengfei An and Wenxing Chen and Zhiying Guo and Chain Lee and Dongliang Chen and Imran Shakir and Mingjie Liu and Tiandou Hu and Yadong Li and Kirkland, {Angus I.} and Xiangfeng Duan and Yu Huang",
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Fei, H, Dong, J, Feng, Y, Allen, CS, Wan, C, Volosskiy, B, Li, M, Zhao, Z, Wang, Y, Sun, H, An, P, Chen, W, Guo, Z, Lee, C, Chen, D, Shakir, I, Liu, M, Hu, T, Li, Y, Kirkland, AI, Duan, X & Huang, Y 2018, ' General synthesis and definitive structural identification of MN 4 C 4 single-atom catalysts with tunable electrocatalytic activities ', Nature Catalysis, vol. 1, no. 1, pp. 63-72. https://doi.org/10.1038/s41929-017-0008-y

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

In: Nature Catalysis, Vol. 1, No. 1, 01.01.2018, p. 63-72.

Research output: Contribution to journalArticle

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T1 - General synthesis and definitive structural identification of MN 4 C 4 single-atom catalysts with tunable electrocatalytic activities

AU - Fei, Huilong

AU - Dong, Juncai

AU - Feng, Yexin

AU - Allen, Christopher S.

AU - Wan, Chengzhang

AU - Volosskiy, Boris

AU - Li, Mufan

AU - Zhao, Zipeng

AU - Wang, Yiliu

AU - Sun, Hongtao

AU - An, Pengfei

AU - Chen, Wenxing

AU - Guo, Zhiying

AU - Lee, Chain

AU - Chen, Dongliang

AU - Shakir, Imran

AU - Liu, Mingjie

AU - Hu, Tiandou

AU - Li, Yadong

AU - Kirkland, Angus I.

AU - Duan, Xiangfeng

AU - Huang, Yu

PY - 2018/1/1

Y1 - 2018/1/1

N2 - 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 MN 4 C 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 MN 4 C 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.

AB - 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 MN 4 C 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 MN 4 C 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.

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