Citation: Xue Dong, Xiaofu Sun, Shuaiqiang Jia, Shitao Han, Dawei Zhou, Ting Yao, Min Wang, Minghui Fang, Haihong Wu, Buxing Han. Electrochemical CO₂ Reduction to C₂₊ Products with Ampere-Level Current on Carbon-Modified Copper Catalysts[J]. Acta Physico-Chimica Sinica, ;2025, 41(3): 240401. doi: 10.3866/PKU.WHXB202404012 shu

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

Xue Dong ¹ ,
Xiaofu Sun ^2,, ,
Shuaiqiang Jia ¹ ,
Shitao Han ¹ ,
Dawei Zhou ¹ ,
Ting Yao ¹ ,
Min Wang ¹ ,
Minghui Fang ¹ ,
Haihong Wu ^1,, ,
Buxing Han ^{1, 2,,}

1.
Shanghai Key Laboratory of Green Chemistry and Chemical Processes, School of Chemistry and Molecular Engineering, East China Normal University, Shanghai 200062, China
2.
Beijing National Laboratory for Molecular Sciences, CAS Key Laboratory of Colloid, Interface and Chemical Thermodynamics, CAS Research/Education Center for Excellence in Molecular Sciences, Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, China

Corresponding author: Xiaofu Sun, sunxiaofu@iccas.ac.cn Haihong Wu, hhwu@chem.ecnu.edu.cn Buxing Han, hanbx@iccas.ac.cn
Received Date: 8 April 2024
Revised Date: 7 May 2024
Accepted Date: 7 May 2024

Fund Project: the National Key Research and Development Program of China 2023YFA1507901the National Key Research and Development Program of China 2020YFA0710201National Natural Science Foundation of China 22293015National Natural Science Foundation of China 22121002

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-C_x catalysts (where 'x' denoted the atomic percentage of C in the catalysts) in facilitating CO₂RR for producing C₂₊ products. Especially, over Cu-C_6%, 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.
- CO₂ reduction,
- Electrocatalysis,
- Multi-carbon products,
- Green chemistry,
- Ampere-level current
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Electrochemical CO₂ Reduction to C₂₊ Products with Ampere-Level Current on Carbon-Modified Copper Catalysts