CO2 electrolysis to multi-carbon products in strong acid at ampere-current levels on La-Cu spheres with channels

Jiaqi Feng; Limin Wu; Xinning Song; Libing Zhang; Shunhan Jia; Xiaodong Ma; Xingxing Tan; Xinchen Kang; Qinggong Zhu; Xiaofu Sun; Buxing Han

doi:10.1038/s41467-024-49308-8

CO₂ electrolysis to multi-carbon products in strong acid at ampere-current levels on La-Cu spheres with channels

Nat Commun. 2024 Jun 6;15(1):4821. doi: 10.1038/s41467-024-49308-8.

Authors

Jiaqi Feng^{1

2}, Limin Wu^{1

3}, Xinning Song^{1

3}, Libing Zhang^{1

3}, Shunhan Jia^{1

3}, Xiaodong Ma^{1

3}, Xingxing Tan^{1

3}, Xinchen Kang^{1

3}, Qinggong Zhu^{1

3}, Xiaofu Sun^{4

5}, Buxing Han^{6

7

8}

Affiliations

¹ 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.
² College of Chemical Engineering and Environment, China University of Petroleum (Beijing), Beijing, 102249, China.
³ School of Chemical Sciences, University of Chinese Academy of Sciences, Beijing, 100049, China.
⁴ 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. sunxiaofu@iccas.ac.cn.
⁵ School of Chemical Sciences, University of Chinese Academy of Sciences, Beijing, 100049, China. sunxiaofu@iccas.ac.cn.
⁶ 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. hanbx@iccas.ac.cn.
⁷ School of Chemical Sciences, University of Chinese Academy of Sciences, Beijing, 100049, China. hanbx@iccas.ac.cn.
⁸ Shanghai Key Laboratory of Green Chemistry and Chemical Processes, State Key Laboratory of Petroleum Molecular & Process Engineering, School of Chemistry and Molecular Engineering, East China Normal University, Shanghai, 200062, China. hanbx@iccas.ac.cn.

Abstract

Achieving satisfactory multi-carbon (C₂₊) products selectivity and current density under acidic condition is a key issue for practical application of electrochemical CO₂ reduction reaction (CO₂RR), but is challenging. Herein, we demonstrate that combining microenvironment modulation by porous channel structure and intrinsic catalytic activity enhancement via doping effect could promote efficient CO₂RR toward C₂₊ products in acidic electrolyte (pH ≤ 1). The La-doped Cu hollow sphere with channels exhibits a C₂₊ products Faradaic efficiency (FE) of 86.2% with a partial current density of -775.8 mA cm^-2. CO₂ single-pass conversion efficiency for C₂₊ products can reach 52.8% at -900 mA cm^-2. Moreover, the catalyst still maintains a high C₂₊ FE of 81.3% at -1 A cm^-2. The channel structure plays a crucial role in accumulating K⁺ and OH^- species near the catalyst surface and within the channels, which effectively suppresses the undesired hydrogen evolution and promotes C-C coupling. Additionally, the La doping enhances the generation of *CO intermediate, and also facilitates C₂₊ products formation.

Abstract

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