Atomic engineering of high-density isolated Co atoms on graphene with proximal-atom controlled reaction selectivity

Huan Yan, Xiaoxu Zhao, Na Guo, Zhiyang Lyu, Yonghua Du, Shibo Xi, Rui Guo, Cheng Chen, Zhongxin Chen, Wei Liu, Chuanhao Yao, Jing Li, Stephen J. Pennycook, Wei Chen, Chenliang Su (), Chun Zhang () and Jiong Lu ()
Additional contact information
Huan Yan: Shenzhen University
Xiaoxu Zhao: National University of Singapore
Na Guo: National University of Singapore
Zhiyang Lyu: National University of Singapore
Yonghua Du: Institute of Chemical and Engineering Sciences
Shibo Xi: Institute of Chemical and Engineering Sciences
Rui Guo: National University of Singapore
Cheng Chen: National University of Singapore
Zhongxin Chen: National University of Singapore
Wei Liu: National University of Singapore
Chuanhao Yao: Shenzhen University
Jing Li: Shenzhen University
Stephen J. Pennycook: National University of Singapore
Wei Chen: National University of Singapore
Chenliang Su: Shenzhen University
Chun Zhang: National University of Singapore
Jiong Lu: Shenzhen University

Nature Communications, 2018, vol. 9, issue 1, 1-9

Abstract: Abstract Controllable synthesis of single atom catalysts (SACs) with high loading remains challenging due to the aggregation tendency of metal atoms as the surface coverage increases. Here we report the synthesis of graphene supported cobalt SACs (Co1/G) with a tuneable high loading by atomic layer deposition. Ozone treatment of the graphene support not only eliminates the undesirable ligands of the pre-deposited metal precursors, but also regenerates active sites for the precise tuning of the density of Co atoms. The Co1/G SACs also demonstrate exceptional activity and high selectivity for the hydrogenation of nitroarenes to produce azoxy aromatic compounds, attributable to the formation of a coordinatively unsaturated and positively charged catalytically active center (Co–O–C) arising from the proximal-atom induced partial depletion of the 3d Co orbitals. Our findings pave the way for the precise engineering of the metal loading in a variety of SACs for superior catalytic activities.

Date: 2018
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DOI: 10.1038/s41467-018-05754-9

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