Atomically dispersed Cu coordinated Rh metallene arrays for simultaneously electrochemical aniline synthesis and biomass upgrading

Qiqi Mao, Xu Mu, Wenxin Wang, Kai Deng, Hongjie Yu, Ziqiang Wang, You Xu, Liang Wang and Hongjing Wang ()
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Qiqi Mao: Zhejiang University of Technology
Xu Mu: Zhejiang University of Technology
Wenxin Wang: Zhejiang University of Technology
Kai Deng: Zhejiang University of Technology
Hongjie Yu: Zhejiang University of Technology
Ziqiang Wang: Zhejiang University of Technology
You Xu: Zhejiang University of Technology
Liang Wang: Zhejiang University of Technology
Hongjing Wang: Zhejiang University of Technology

Nature Communications, 2023, vol. 14, issue 1, 1-12

Abstract: Abstract Organic electrocatalytic conversion is an essential pathway for the green conversion of low-cost organic compounds to high-value chemicals, which urgently demands the development of efficient electrocatalysts. Here, we report a Cu single-atom dispersed Rh metallene arrays on Cu foam for cathodic nitrobenzene electroreduction reaction and anodic methanol oxidation reaction. In the coupled electrocatalytic system, the Cusingle-atom-Rh metallene arrays on Cu foam requires only the low voltages of 1.18 V to reach current densities of 100 mA cm−2 for generating aniline and formate, with up to ~100% of nitrobenzene conversion/ aniline selectivity and over ~90% of formate Faraday efficiency, achieving synthesis of high-value chemicals. Density functional theory calculations reveal the electron effect between Cu single-atom and Rh host and catalytic reaction mechanism. The synergistic catalytic effect and H*-spillover effect can improve catalytic reaction process and reduce energy barrier for reaction process, thus enhancing electrocatalytic reaction activity and target product selectivity.

Date: 2023
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DOI: 10.1038/s41467-023-41423-2

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