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Nano Research 2022, 15(10): 8872-8879 https://doi.org/10.1007/s12274-022-4698-3
Research Article | Issue | Published: 27 July 2022

Confined interface engineering of self-supported Cu@N-doped graphene for electrocatalytic CO2 reduction with enhanced selectivity towards ethanol

Show Author's Information Dejin Zang1,§ ( ),  Xuejiao J. Gao3,§,  Leyun Li3,  Yongge Wei4,  Haiqing Wang2( )
Institute of Materia Medica, Shandong First Medical University & Shandong Academy of Medical Sciences, Jinan 250117, China
Institute for Advanced Interdisciplinary Research (iAIR), School of Chemistry and Chemical Engineering, University of Jinan, Jinan 250022, China
College of Chemistry and Chemical Engineering, Jiangxi Normal University, Nanchang 330022, China
Key Lab of Organic Optoelectronics & Molecular Engineering of Ministry of Education, Department of Chemistry, Tsinghua University, Beijing 100084, China

§ Dejin Zang and Xuejiao J. Gao contributed equally to this work.

Keywords:
CO2 reduction, interface engineering, Cu-based catalyst, Cu/N-doped carbon, C2 production
Topics:
Electrocatalysis
Cite this article:
Zang D, Gao XJ, Li L, et al. Confined interface engineering of self-supported Cu@N-doped graphene for electrocatalytic CO2 reduction with enhanced selectivity towards ethanol. Nano Research, 2022, 15(10): 8872-8879. https://doi.org/10.1007/s12274-022-4698-3
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Abstract Full text Electronic supplementary material About this article

Electroreduction of greenhouse gas CO2 into value-added fuels and chemicals provides a promising pathway to address the issues of energy crisis and environmental change. However, the regulations of the selectivity towards C2 product and the competing hydrogen evolution reaction (HER) are major challenges for CO2 reduction reaction (CO2RR). Here, we develop an interface-enhanced strategy by depositing a thin layer of nitrogen-doped graphene (N-G) on a Cu foam surface (Cu-N-G) to selectively promote the ethanol pathway in CO2RR. Compared to the undetectable ethanol selectivity of pure Cu and Cu@graphene (Cu-G), Cu-N-G has boosted the ethanol selectivity to 33.1% in total Faradic efficiency (FE) at −0.8 V vs. reversible hydrogen electrode (RHE). The experimental and density functional theory (DFT) results verify that the interconnected graphene coating can not only serve as the fast charge transport channel but also provide confined nanospace for mass transfer. The N doping can not only trigger the intrinsic interaction between N in N-G and CO2 molecule for enriching the local concentration of reactants but also promote the average valence state of Cu for C–C coupling pathways. The confinement effect at the interface of Cu-N-G can not only provide high adsorbed hydrogen (Had) coverage but also stabilize the key *HCCHOH intermediate towards ethanol pathway. The provided interface-enhanced strategy herein is expected to inspire the design of Cu-based CO2RR electrocatalysts towards multi-carbon products.


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Electronic supplementary material
About this article

Confined interface engineering of self-supported Cu@N-doped graphene for electrocatalytic CO2 reduction with enhanced selectivity towards ethanol

Show Author's information Dejin Zang1,§ ( ), Xuejiao J. Gao3,§, Leyun Li3, Yongge Wei4, Haiqing Wang2( )
Institute of Materia Medica, Shandong First Medical University & Shandong Academy of Medical Sciences, Jinan 250117, China
Institute for Advanced Interdisciplinary Research (iAIR), School of Chemistry and Chemical Engineering, University of Jinan, Jinan 250022, China
College of Chemistry and Chemical Engineering, Jiangxi Normal University, Nanchang 330022, China
Key Lab of Organic Optoelectronics & Molecular Engineering of Ministry of Education, Department of Chemistry, Tsinghua University, Beijing 100084, China

§ Dejin Zang and Xuejiao J. Gao contributed equally to this work.

Abstract

Electroreduction of greenhouse gas CO2 into value-added fuels and chemicals provides a promising pathway to address the issues of energy crisis and environmental change. However, the regulations of the selectivity towards C2 product and the competing hydrogen evolution reaction (HER) are major challenges for CO2 reduction reaction (CO2RR). Here, we develop an interface-enhanced strategy by depositing a thin layer of nitrogen-doped graphene (N-G) on a Cu foam surface (Cu-N-G) to selectively promote the ethanol pathway in CO2RR. Compared to the undetectable ethanol selectivity of pure Cu and Cu@graphene (Cu-G), Cu-N-G has boosted the ethanol selectivity to 33.1% in total Faradic efficiency (FE) at −0.8 V vs. reversible hydrogen electrode (RHE). The experimental and density functional theory (DFT) results verify that the interconnected graphene coating can not only serve as the fast charge transport channel but also provide confined nanospace for mass transfer. The N doping can not only trigger the intrinsic interaction between N in N-G and CO2 molecule for enriching the local concentration of reactants but also promote the average valence state of Cu for C–C coupling pathways. The confinement effect at the interface of Cu-N-G can not only provide high adsorbed hydrogen (Had) coverage but also stabilize the key *HCCHOH intermediate towards ethanol pathway. The provided interface-enhanced strategy herein is expected to inspire the design of Cu-based CO2RR electrocatalysts towards multi-carbon products.

Keywords: CO2 reduction, interface engineering, Cu-based catalyst, Cu/N-doped carbon, C2 production

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Publication history
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Publication history

Received: 01 June 2022
Revised: 20 June 2022
Accepted: 23 June 2022
Published: 27 July 2022
Issue date: October 2022

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