Volume 63, Issue 41 e202407612
Research Article

Tensile-Strained Cu Penetration Electrode Boosts Asymmetric C−C Coupling for Ampere-Level CO2-to-C2+ Reduction in Acid

Shoujie Li

Shoujie Li

Low-Carbon Conversion Science and Engineering Center, Shanghai Advanced Research Institute, Chinese Academy of Sciences, 201210 Shanghai, China

State Key Laboratory of Low Carbon Catalysis and Carbon Dioxide Utilization, Shanghai Advanced Research Institute, Chinese Academy of Sciences, 201210 Shanghai, China

These authors contributed equally to this work.

Contribution: Conceptualization (lead), Data curation (lead), Formal analysis (lead), ​Investigation (lead), Methodology (lead), Resources (lead), Writing - original draft (lead), Writing - review & editing (lead)

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Gangfeng Wu

Gangfeng Wu

Low-Carbon Conversion Science and Engineering Center, Shanghai Advanced Research Institute, Chinese Academy of Sciences, 201210 Shanghai, China

University of Chinese Academy of Sciences, 100049 Beijing, China

State Key Laboratory of Low Carbon Catalysis and Carbon Dioxide Utilization, Shanghai Advanced Research Institute, Chinese Academy of Sciences, 201210 Shanghai, China

These authors contributed equally to this work.

Contribution: Data curation (equal), Writing - original draft (equal)

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Jianing Mao

Jianing Mao

University of Chinese Academy of Sciences, 100049 Beijing, China

Shanghai Institute of Applied Physics, Chinese Academy of Sciences, 201204 Shanghai, China

Shanghai Synchrotron Radiation Facility, Shanghai Advanced Research Institute, Chinese Academy of Sciences, 201204 Shanghai, China

These authors contributed equally to this work.

Contribution: Data curation (equal), Writing - original draft (equal)

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Aohui Chen

Aohui Chen

Low-Carbon Conversion Science and Engineering Center, Shanghai Advanced Research Institute, Chinese Academy of Sciences, 201210 Shanghai, China

State Key Laboratory of Low Carbon Catalysis and Carbon Dioxide Utilization, Shanghai Advanced Research Institute, Chinese Academy of Sciences, 201210 Shanghai, China

Contribution: Data curation (supporting)

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Xiaohu Liu

Xiaohu Liu

Low-Carbon Conversion Science and Engineering Center, Shanghai Advanced Research Institute, Chinese Academy of Sciences, 201210 Shanghai, China

State Key Laboratory of Low Carbon Catalysis and Carbon Dioxide Utilization, Shanghai Advanced Research Institute, Chinese Academy of Sciences, 201210 Shanghai, China

Contribution: Data curation (supporting)

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Jianrong Zeng

Jianrong Zeng

Shanghai Synchrotron Radiation Facility, Shanghai Advanced Research Institute, Chinese Academy of Sciences, 201204 Shanghai, China

Contribution: Data curation (supporting)

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Yiheng Wei

Yiheng Wei

Low-Carbon Conversion Science and Engineering Center, Shanghai Advanced Research Institute, Chinese Academy of Sciences, 201210 Shanghai, China

University of Chinese Academy of Sciences, 100049 Beijing, China

State Key Laboratory of Low Carbon Catalysis and Carbon Dioxide Utilization, Shanghai Advanced Research Institute, Chinese Academy of Sciences, 201210 Shanghai, China

Contribution: Data curation (supporting)

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Jiangjiang Wang

Jiangjiang Wang

Low-Carbon Conversion Science and Engineering Center, Shanghai Advanced Research Institute, Chinese Academy of Sciences, 201210 Shanghai, China

University of Chinese Academy of Sciences, 100049 Beijing, China

State Key Laboratory of Low Carbon Catalysis and Carbon Dioxide Utilization, Shanghai Advanced Research Institute, Chinese Academy of Sciences, 201210 Shanghai, China

Contribution: Data curation (supporting)

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Huanyi Zhu

Huanyi Zhu

Low-Carbon Conversion Science and Engineering Center, Shanghai Advanced Research Institute, Chinese Academy of Sciences, 201210 Shanghai, China

University of Chinese Academy of Sciences, 100049 Beijing, China

State Key Laboratory of Low Carbon Catalysis and Carbon Dioxide Utilization, Shanghai Advanced Research Institute, Chinese Academy of Sciences, 201210 Shanghai, China

Contribution: Data curation (supporting)

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Jiayu Xia

Jiayu Xia

Low-Carbon Conversion Science and Engineering Center, Shanghai Advanced Research Institute, Chinese Academy of Sciences, 201210 Shanghai, China

University of Chinese Academy of Sciences, 100049 Beijing, China

State Key Laboratory of Low Carbon Catalysis and Carbon Dioxide Utilization, Shanghai Advanced Research Institute, Chinese Academy of Sciences, 201210 Shanghai, China

Contribution: Data curation (supporting)

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Xiaotong Wang

Xiaotong Wang

Low-Carbon Conversion Science and Engineering Center, Shanghai Advanced Research Institute, Chinese Academy of Sciences, 201210 Shanghai, China

University of Chinese Academy of Sciences, 100049 Beijing, China

State Key Laboratory of Low Carbon Catalysis and Carbon Dioxide Utilization, Shanghai Advanced Research Institute, Chinese Academy of Sciences, 201210 Shanghai, China

Contribution: Data curation (supporting)

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Guihua Li

Guihua Li

Low-Carbon Conversion Science and Engineering Center, Shanghai Advanced Research Institute, Chinese Academy of Sciences, 201210 Shanghai, China

State Key Laboratory of Low Carbon Catalysis and Carbon Dioxide Utilization, Shanghai Advanced Research Institute, Chinese Academy of Sciences, 201210 Shanghai, China

Contribution: Data curation (supporting)

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Yanfang Song

Yanfang Song

Low-Carbon Conversion Science and Engineering Center, Shanghai Advanced Research Institute, Chinese Academy of Sciences, 201210 Shanghai, China

University of Chinese Academy of Sciences, 100049 Beijing, China

State Key Laboratory of Low Carbon Catalysis and Carbon Dioxide Utilization, Shanghai Advanced Research Institute, Chinese Academy of Sciences, 201210 Shanghai, China

Contribution: Data curation (supporting)

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Xiao Dong

Corresponding Author

Xiao Dong

Low-Carbon Conversion Science and Engineering Center, Shanghai Advanced Research Institute, Chinese Academy of Sciences, 201210 Shanghai, China

University of Chinese Academy of Sciences, 100049 Beijing, China

State Key Laboratory of Low Carbon Catalysis and Carbon Dioxide Utilization, Shanghai Advanced Research Institute, Chinese Academy of Sciences, 201210 Shanghai, China

Contribution: Conceptualization (equal), Supervision (equal), Writing - review & editing (equal)

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Wei Wei

Corresponding Author

Wei Wei

Low-Carbon Conversion Science and Engineering Center, Shanghai Advanced Research Institute, Chinese Academy of Sciences, 201210 Shanghai, China

University of Chinese Academy of Sciences, 100049 Beijing, China

State Key Laboratory of Low Carbon Catalysis and Carbon Dioxide Utilization, Shanghai Advanced Research Institute, Chinese Academy of Sciences, 201210 Shanghai, China

Contribution: Supervision (equal)

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Wei Chen

Corresponding Author

Wei Chen

Low-Carbon Conversion Science and Engineering Center, Shanghai Advanced Research Institute, Chinese Academy of Sciences, 201210 Shanghai, China

University of Chinese Academy of Sciences, 100049 Beijing, China

State Key Laboratory of Low Carbon Catalysis and Carbon Dioxide Utilization, Shanghai Advanced Research Institute, Chinese Academy of Sciences, 201210 Shanghai, China

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First published: 15 July 2024
Citations: 21

Graphical Abstract

Tensile-strained copper hollow-fiber penetration electrode (Cu HPE) enhances the asymmetric C−C coupling to steer the selectivity and activity of multicarbon (C2+) products. A faradaic efficiency of 84.5 % and a partial current density as high as 3.1 A cm−2 for C2+ products, alongside a single-pass carbon efficiency of 81.5 % and stable electrolysis for 240 h were demonstrated in a strong acidic electrolyte (pH=1).

Abstract

The synthesis of multicarbon (C2+) products remains a substantial challenge in sustainable CO2 electroreduction owing to the need for sufficient current density and faradaic efficiency alongside carbon efficiency. Herein, we demonstrate ampere-level high-efficiency CO2 electroreduction to C2+ products in both neutral and strongly acidic (pH=1) electrolytes using a hierarchical Cu hollow-fiber penetration electrode (HPE). High concentration of K+ could concurrently suppress hydrogen evolution reaction and facilitate C−C coupling, thereby promoting C2+ production in strong acid. By optimizing the K+ and H+ concentration and CO2 flow rate, a faradaic efficiency of 84.5 % and a partial current density as high as 3.1 A cm−2 for C2+ products, alongside a single-pass carbon efficiency of 81.5 % and stable electrolysis for 240 h were demonstrated in a strong acidic solution of H2SO4 and KCl (pH=1). Experimental measurements and density functional theory simulations suggested that tensile-strained Cu HPE enhances the asymmetric C−C coupling to steer the selectivity and activity of C2+ products.

Conflict of Interests

The authors declare no conflict of interest.

Data Availability Statement

The data that support the findings of this study are available in the supplementary material of this article.

The full text of this article hosted at iucr.org is unavailable due to technical difficulties.