General synthesis and definitive structural identification of MN4C4 single-atom catalysts with tunable electrocatalytic activities

DOI: 10.1038/s41929-017-0008-y

Authors: Huilong Fei (University of California) , Juncai Dong (Institute of High Energy Physics, Chinese Academy of Sciences) , Yexin Feng (Hunan University) , Christopher Allen (Diamond Light Source; University of Oxford) , Chengzhang Wan (University of California) , Boris Volosskiy (University of California) , Mufan Li (University of California) , Zipeng Zhao (University of California) , Yiliu Wang (University of California) , Hongtao Sun (University of California) , Pengfei An (Institute of High Energy Physics, Chinese Academy of Sciences) , Wenxing Chen (Tsinghua University) , Zhiying Guo (Institute of High Energy Physics, Chinese Academy of Sciences) , Chain Lee (University of California) , Dongliang Chen (Institute of High Energy Physics, Chinese Academy of Sciences) , Imran Shakir (King Saud University) , Mingjie Liu (Brookhaven National Laboratory) , Tiandou Hu (of High Energy Physics, Chinese Academy of Sciences) , Yadong Li (Tsinghua University) , Angus I. Kirkland (University of Oxford) , Xiangfeng Duan (University of California) , Yu Huang (University of California)
Co-authored by industrial partner: No

Type: Journal Paper
Journal: Nature Catalysis , VOL 1 , PAGES 63 - 72

State: Published (Approved)
Published: January 2018
Diamond Proposal Number(s): 16967

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 MN4C4 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 MN4C4 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.

Journal Keywords: Catalyst synthesis; Catalytic mechanisms; Electrocatalysis; Heterogeneous catalysis

Subject Areas: Chemistry

Diamond Offline Facilities: Electron Physical Sciences Imaging Center (ePSIC)
Instruments: E02-JEM ARM 300CF

Added On: 09/01/2018 09:33

Discipline Tags:

Physical Chemistry Catalysis Chemistry

Technical Tags:

Microscopy Electron Microscopy (EM) Scanning Electron Microscopy (SEM) Transmission Electron Microscopy (TEM)