skip to main content

DOE PAGESDOE PAGES

This content will become publicly available on January 8, 2019

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

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:
Report Number(s):
BNL-200041-2018-JAAM
Journal ID: ISSN 2520-1158
Grant/Contract Number:
SC0012704
Type:
Accepted Manuscript
Journal Name:
Nature Catalysis
Additional Journal Information:
Journal Volume: 1; Journal Issue: 1; Journal ID: ISSN 2520-1158
Research Org:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
77 NANOSCIENCE AND NANOTECHNOLOGY; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
OSTI Identifier:
1425042