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CO2 electroreduction to multicarbon products in strongly acidic electrolyte via synergistically modulating the local microenvironment

Author

Listed:
  • Zesong Ma

    (Hunan University)

  • Zhilong Yang

    (Hunan University)

  • Wenchuan Lai

    (Hunan University)

  • Qiyou Wang

    (Central South University)

  • Yan Qiao

    (Hunan University)

  • Haolan Tao

    (East China University of Science and Technology)

  • Cheng Lian

    (East China University of Science and Technology)

  • Min Liu

    (Central South University)

  • Chao Ma

    (Hunan University)

  • Anlian Pan

    (Hunan University)

  • Hongwen Huang

    (Hunan University
    Shenzhen Research Institute of Hunan University)

Abstract

Electrochemical CO2 reduction to multicarbon products faces challenges of unsatisfactory selectivity, productivity, and long-term stability. Herein, we demonstrate CO2 electroreduction in strongly acidic electrolyte (pH ≤ 1) on electrochemically reduced porous Cu nanosheets by combining the confinement effect and cation effect to synergistically modulate the local microenvironment. A Faradaic efficiency of 83.7 ± 1.4% and partial current density of 0.56 ± 0.02 A cm−2, single-pass carbon efficiency of 54.4%, and stable electrolysis of 30 h in a flow cell are demonstrated for multicarbon products in a strongly acidic aqueous electrolyte consisting of sulfuric acid and KCl with pH ≤ 1. Mechanistically, the accumulated species (e.g., K+ and OH−) on the Helmholtz plane account for the selectivity and activity toward multicarbon products by kinetically reducing the proton coverage and thermodynamically favoring the CO2 conversion. We find that the K+ cations facilitate C-C coupling through local interaction between K+ and the key intermediate *OCCO.

Suggested Citation

  • Zesong Ma & Zhilong Yang & Wenchuan Lai & Qiyou Wang & Yan Qiao & Haolan Tao & Cheng Lian & Min Liu & Chao Ma & Anlian Pan & Hongwen Huang, 2022. "CO2 electroreduction to multicarbon products in strongly acidic electrolyte via synergistically modulating the local microenvironment," Nature Communications, Nature, vol. 13(1), pages 1-11, December.
  • Handle: RePEc:nat:natcom:v:13:y:2022:i:1:d:10.1038_s41467-022-35415-x
    DOI: 10.1038/s41467-022-35415-x
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    1. Min Liu & Yuanjie Pang & Bo Zhang & Phil De Luna & Oleksandr Voznyy & Jixian Xu & Xueli Zheng & Cao Thang Dinh & Fengjia Fan & Changhong Cao & F. Pelayo García de Arquer & Tina Saberi Safaei & Adam Me, 2016. "Enhanced electrocatalytic CO2 reduction via field-induced reagent concentration," Nature, Nature, vol. 537(7620), pages 382-386, September.
    2. David Wakerley & Sarah Lamaison & Joshua Wicks & Auston Clemens & Jeremy Feaster & Daniel Corral & Shaffiq A. Jaffer & Amitava Sarkar & Marc Fontecave & Eric B. Duoss & Sarah Baker & Edward H. Sargent, 2022. "Gas diffusion electrodes, reactor designs and key metrics of low-temperature CO2 electrolysers," Nature Energy, Nature, vol. 7(2), pages 130-143, February.
    3. Seung-Jae Shin & Dong Hyun Kim & Geunsu Bae & Stefan Ringe & Hansol Choi & Hyung-Kyu Lim & Chang Hyuck Choi & Hyungjun Kim, 2022. "On the importance of the electric double layer structure in aqueous electrocatalysis," Nature Communications, Nature, vol. 13(1), pages 1-8, December.
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    1. Kang Yang & Ming Li & Tianqi Gao & Guoliang Xu & Di Li & Yao Zheng & Qiang Li & Jingjing Duan, 2024. "An acid-tolerant metal-organic framework for industrial CO2 electrolysis using a proton exchange membrane," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    2. Jiaqi Feng & Limin Wu & Xinning Song & Libing Zhang & Shunhan Jia & Xiaodong Ma & Xingxing Tan & Xinchen Kang & Qinggong Zhu & Xiaofu Sun & Buxing Han, 2024. "CO2 electrolysis to multi-carbon products in strong acid at ampere-current levels on La-Cu spheres with channels," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    3. Linghu Meng & Cheng-Wei Kao & Zhen Wang & Jun Ma & Peifeng Huang & Nan Zhao & Xin Zheng & Ming Peng & Ying-Rui Lu & Yongwen Tan, 2024. "Alloying and confinement effects on hierarchically nanoporous CuAu for efficient electrocatalytic semi-hydrogenation of terminal alkynes," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    4. Hai-Gang Qin & Yun-Fan Du & Yi-Yang Bai & Fu-Zhi Li & Xian Yue & Hao Wang & Jian-Zhao Peng & Jun Gu, 2023. "Surface-immobilized cross-linked cationic polyelectrolyte enables CO2 reduction with metal cation-free acidic electrolyte," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    5. Weihua Guo & Siwei Zhang & Junjie Zhang & Haoran Wu & Yangbo Ma & Yun Song & Le Cheng & Liang Chang & Geng Li & Yong Liu & Guodan Wei & Lin Gan & Minghui Zhu & Shibo Xi & Xue Wang & Boris I. Yakobson , 2023. "Accelerating multielectron reduction at CuxO nanograins interfaces with controlled local electric field," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
    6. Shoujie Li & Xiao Dong & Gangfeng Wu & Yanfang Song & Jianing Mao & Aohui Chen & Chang Zhu & Guihua Li & Yiheng Wei & Xiaohu Liu & Jiangjiang Wang & Wei Chen & Wei Wei, 2024. "Ampere-level CO2 electroreduction with single-pass conversion exceeding 85% in acid over silver penetration electrodes," Nature Communications, Nature, vol. 15(1), pages 1-13, December.

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