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

Nature Communications
Huan YanJiong Lu

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.

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Citations

Nov 16, 2019·Advanced Science·Bin ZhangHan Zhang
Feb 6, 2020·ACS Applied Materials & Interfaces·Rahman DaiyanRose Amal
Apr 4, 2020·Chemical Reviews·Shufang JiYadong Li
Aug 14, 2020·Chemical Reviews·Ruixuan QinNanfeng Zheng
Oct 22, 2020·Chemical Reviews·Selina K KaiserJavier Pérez-Ramírez
Oct 29, 2020·Chemical Reviews·Rui LangTao Zhang
Sep 26, 2021·Advanced Materials·Yunfei BuJong-Beom Baek
Sep 28, 2021·Frontiers in Chemistry·Thillai Govindaraja SenthamaraikannanSailaja Krishnamurty

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Methods Mentioned

BETA
X-ray

Software Mentioned

Demeter
FDMNES
Vienna ab - initio Simulation Package ( VASP )

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