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

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 nit...

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Published inNature 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
LanguageEnglish
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
Online AccessGet full text
ISSN2041-1723
2041-1723
DOI10.1038/s41467-023-41423-2

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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 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.
AbstractList 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.
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.
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.
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.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.
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.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.
ArticleNumber 5679
Author Yu, Hongjie
Mu, Xu
Wang, Ziqiang
Deng, Kai
Mao, Qiqi
Wang, Wenxin
Xu, You
Wang, Hongjing
Wang, Liang
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Snippet Organic electrocatalytic conversion is an essential pathway for the green conversion of low-cost organic compounds to high-value chemicals, which urgently...
Abstract Organic electrocatalytic conversion is an essential pathway for the green conversion of low-cost organic compounds to high-value chemicals, which...
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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
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Title Atomically dispersed Cu coordinated Rh metallene arrays for simultaneously electrochemical aniline synthesis and biomass upgrading
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Volume 14
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