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Electrochemical CO2 Reduction to C2+ Products with Ampere-Level Current on Carbon-Modified Copper Catalysts

Xue Dong1, Xiaofu Sun2, Shuaiqiang Jia1, Shitao Han1, Dawei Zhou1, Ting Yao1, Min Wang1, Minghui Fang1, Haihong Wu1, Buxing Han1,2   

  • 收稿日期:2024-04-08 修回日期:2024-05-07 录用日期:2024-05-07
  • 通讯作者: Xiaofu Sun, Haihong Wu, Buxing Han E-mail:sunxiaofu@iccas.ac.cn;hhwu@chem.ecnu.edu.cn;hanbx@iccas.ac.cn
  • 基金资助:
    The work was supported by the National Key Research and Development Program of China (2023YFA1507901, 2020YFA0710201) and National Natural Science Foundation of China (22293015, 22121002).

Electrochemical CO2 Reduction to C2+ Products with Ampere-Level Current on Carbon-Modified Copper Catalysts

Xue Dong1, Xiaofu Sun2, Shuaiqiang Jia1, Shitao Han1, Dawei Zhou1, Ting Yao1, Min Wang1, Minghui Fang1, Haihong Wu1, Buxing Han1,2   

  1. 1 Shanghai Key Laboratory of Green Chemistry and Chemical Processes, East China Normal University, Shanghai 200062, China;
    2 Beijing National Laboratory for Molecular Sciences, Key Laboratory of Colloid and Interface and Thermodynamics, Center for Carbon Neutral Chemistry, Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, China
  • Received:2024-04-08 Revised:2024-05-07 Accepted:2024-05-07
  • Contact: Xiaofu Sun, Haihong Wu, Buxing Han E-mail:sunxiaofu@iccas.ac.cn;hhwu@chem.ecnu.edu.cn;hanbx@iccas.ac.cn
  • Supported by:
    The work was supported by the National Key Research and Development Program of China (2023YFA1507901, 2020YFA0710201) and National Natural Science Foundation of China (22293015, 22121002).

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摘要： Copper-based electrocatalysts have great potential to produce high-value products in CO2 reduction reaction (CO2RR), offering a promising way to achieve negative carbon emissions. Additionally, achieving ampere-level currents is crucial for realizing the industrialization of multi-carbon (C2+) products. However, the C2+ selectivity at industrial current densities remains unsatisfactory due to complex electron transport processes and inevitable side reactions. Herein, we developed a carbon-modification strategy aimed at optimizing the local environment and regulating the adsorption of intermediates at Cu active sites. Our findings demonstrated the effectiveness of Cu-Cx catalysts (where ‘x’ denoted the atomic percentage of C in the catalysts) in facilitating CO2RR for producing C2+ products. Especially, over Cu-C6%, the current density could reach to 1.25 A?cm?2 at ?0.72 V vs. RHE (versus reversible hydrogen electrode) in a flow cell, and the Faradaic efficiency (FE) of C2H4 and C2+ products could reach to 54.4% and 80.2%, respectively. In situ spectral analysis and density functional theory (DFT) calculations showed that the presence of C regulated the adsorption of *CO on Cu surface, reduced the energy barrier of C–C coupling, thus promoting the production of C2+ products

关键词: CO2 reduction, Electrocatalysis, Multi-carbon products, Green chemistry, Ampere-level current

Abstract: Copper-based electrocatalysts have great potential to produce high-value products in CO2 reduction reaction (CO2RR), offering a promising way to achieve negative carbon emissions. Additionally, achieving ampere-level currents is crucial for realizing the industrialization of multi-carbon (C2+) products. However, the C2+ selectivity at industrial current densities remains unsatisfactory due to complex electron transport processes and inevitable side reactions. Herein, we developed a carbon-modification strategy aimed at optimizing the local environment and regulating the adsorption of intermediates at Cu active sites. Our findings demonstrated the effectiveness of Cu-Cx catalysts (where ‘x’ denoted the atomic percentage of C in the catalysts) in facilitating CO2RR for producing C2+ products. Especially, over Cu-C6%, the current density could reach to 1.25 A?cm?2 at ?0.72 V vs. RHE (versus reversible hydrogen electrode) in a flow cell, and the Faradaic efficiency (FE) of C2H4 and C2+ products could reach to 54.4% and 80.2%, respectively. In situ spectral analysis and density functional theory (DFT) calculations showed that the presence of C regulated the adsorption of *CO on Cu surface, reduced the energy barrier of C–C coupling, thus promoting the production of C2+ products

Key words: CO2 reduction, Electrocatalysis, Multi-carbon products, Green chemistry, Ampere-level current