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

• Published in: Nature communications Vol. 14; no. 1; pp. 5679 - 12
• Main Authors: Mao, Qiqi, Mu, Xu, Wang, Wenxin, Deng, Kai, Yu, Hongjie, Wang, Ziqiang, Xu, You, Wang, Liang, Wang, Hongjing
• Format: Journal Article
• Language: English
• Published: London Nature Publishing Group UK 14.09.2023; Nature Publishing Group; Nature Portfolio
• Subjects: 119/118; 140/131; 140/146; 147/135; 147/137; 147/143; 147/3; 639/301/1023/1026; 639/638/224/685; 639/638/77/886; 639/925/357/1018; Alternative energy sources; Aniline; Anodizing; Arrays; Biomass; Chemical synthesis; Chemicals; Conversion; Copper; Density functional theory; Dispersion; Efficiency; Electrocatalysts; Electrochemistry; Energy consumption; Humanities and Social Sciences; Low cost; Metal foams; multidisciplinary; Nitrobenzene; Organic compounds; Oxidation; Reaction mechanisms; Renewable resources; Science; Science (multidisciplinary); Transmission electron microscopy
• ISSN: 2041-1723; 2041-1723
• DOI: 10.1038/s41467-023-41423-2

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 Cu single-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. Electrocatalytic conversion of low-cost organic compounds to high-value chemicals urgently demands the development of efficient electrocatalysts. Mao et al. report the synthesis of Cu single-atom dispersed Rh metallene arrays for electrochemical aniline synthesis and biomass upgrading with enhanced electrocatalytic activity.