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CO electrolysis to multicarbon products over grain boundary-rich Cu nanoparticles in membrane electrode assembly electrolyzers

Author

Listed:
  • Hefei Li

    (Chinese Academy of Sciences
    University of Chinese Academy of Sciences)

  • Pengfei Wei

    (Chinese Academy of Sciences)

  • Tianfu Liu

    (Chinese Academy of Sciences)

  • Mingrun Li

    (Chinese Academy of Sciences)

  • Chao Wang

    (Chinese Academy of Sciences)

  • Rongtan Li

    (Chinese Academy of Sciences
    University of Chinese Academy of Sciences)

  • Jinyu Ye

    (Xiamen University)

  • Zhi-You Zhou

    (Xiamen University)

  • Shi-Gang Sun

    (Xiamen University)

  • Qiang Fu

    (Chinese Academy of Sciences)

  • Dunfeng Gao

    (Chinese Academy of Sciences)

  • Guoxiong Wang

    (Chinese Academy of Sciences)

  • Xinhe Bao

    (Chinese Academy of Sciences)

Abstract

Producing valuable chemicals like ethylene via catalytic carbon monoxide conversion is an important nonpetroleum route. Here we demonstrate an electrochemical route for highly efficient synthesis of multicarbon (C2+) chemicals from CO. We achieve a C2+ partial current density as high as 4.35 ± 0.07 A cm−2 at a low cell voltage of 2.78 ± 0.01 V over a grain boundary-rich Cu nanoparticle catalyst in an alkaline membrane electrode assembly (MEA) electrolyzer, with a C2+ Faradaic efficiency of 87 ± 1% and a CO conversion of 85 ± 3%. Operando Raman spectroscopy and density functional theory calculations reveal that the grain boundaries of Cu nanoparticles facilitate CO adsorption and C − C coupling, thus rationalizing a qualitative trend between C2+ production and grain boundary density. A scale-up demonstration using an electrolyzer stack with five 100 cm2 MEAs achieves high C2+ and ethylene formation rates of 118.9 mmol min−1 and 1.2 L min−1, respectively, at a total current of 400 A (4 A cm−2) with a C2+ Faradaic efficiency of 64%.

Suggested Citation

  • Hefei Li & Pengfei Wei & Tianfu Liu & Mingrun Li & Chao Wang & Rongtan Li & Jinyu Ye & Zhi-You Zhou & Shi-Gang Sun & Qiang Fu & Dunfeng Gao & Guoxiong Wang & Xinhe Bao, 2024. "CO electrolysis to multicarbon products over grain boundary-rich Cu nanoparticles in membrane electrode assembly electrolyzers," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
  • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-49095-2
    DOI: 10.1038/s41467-024-49095-2
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    References listed on IDEAS

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    1. Rosa M. Arán-Ais & Fabian Scholten & Sebastian Kunze & Rubén Rizo & Beatriz Roldan Cuenya, 2020. "The role of in situ generated morphological motifs and Cu(i) species in C2+ product selectivity during CO2 pulsed electroreduction," Nature Energy, Nature, vol. 5(4), pages 317-325, April.
    2. Miao Zhong & Kevin Tran & Yimeng Min & Chuanhao Wang & Ziyun Wang & Cao-Thang Dinh & Phil De Luna & Zongqian Yu & Armin Sedighian Rasouli & Peter Brodersen & Song Sun & Oleksandr Voznyy & Chih-Shan Ta, 2020. "Accelerated discovery of CO2 electrocatalysts using active machine learning," Nature, Nature, vol. 581(7807), pages 178-183, May.
    3. Hao Sun & Ling Chen & Likun Xiong & Kun Feng & Yufeng Chen & Xiang Zhang & Xuzhou Yuan & Baiyu Yang & Zhao Deng & Yu Liu & Mark H. Rümmeli & Jun Zhong & Yan Jiao & Yang Peng, 2021. "Promoting ethylene production over a wide potential window on Cu crystallites induced and stabilized via current shock and charge delocalization," Nature Communications, Nature, vol. 12(1), pages 1-11, December.
    4. Yao Yang & Sheena Louisia & Sunmoon Yu & Jianbo Jin & Inwhan Roh & Chubai Chen & Maria V. Fonseca Guzman & Julian Feijóo & Peng-Cheng Chen & Hongsen Wang & Christopher J. Pollock & Xin Huang & Yu-Tsun, 2023. "Operando studies reveal active Cu nanograins for CO2 electroreduction," Nature, Nature, vol. 614(7947), pages 262-269, February.
    5. Xiaohui Sun & Alma I. Olivos Suarez & Mark Meijerink & Tom Deelen & Samy Ould-Chikh & Jovana Zečević & Krijn P. Jong & Freek Kapteijn & Jorge Gascon, 2017. "Manufacture of highly loaded silica-supported cobalt Fischer–Tropsch catalysts from a metal organic framework," Nature Communications, Nature, vol. 8(1), pages 1-8, December.
    6. Jun Li & Aoni Xu & Fengwang Li & Ziyun Wang & Chengqin Zou & Christine M. Gabardo & Yuhang Wang & Adnan Ozden & Yi Xu & Dae-Hyun Nam & Yanwei Lum & Joshua Wicks & Bin Chen & Zhiqiang Wang & Jiatang Ch, 2020. "Enhanced multi-carbon alcohol electroproduction from CO via modulated hydrogen adsorption," Nature Communications, Nature, vol. 11(1), pages 1-8, December.
    7. Christina W. Li & Jim Ciston & Matthew W. Kanan, 2014. "Electroreduction of carbon monoxide to liquid fuel on oxide-derived nanocrystalline copper," Nature, Nature, vol. 508(7497), pages 504-507, April.
    8. Haeun Shin & Kentaro U. Hansen & Feng Jiao, 2021. "Techno-economic assessment of low-temperature carbon dioxide electrolysis," Nature Sustainability, Nature, vol. 4(10), pages 911-919, October.
    9. Jian Jin & Joshua Wicks & Qiuhong Min & Jun Li & Yongfeng Hu & Jingyuan Ma & Yu Wang & Zheng Jiang & Yi Xu & Ruihu Lu & Gangzheng Si & Panagiotis Papangelakis & Mohsen Shakouri & Qunfeng Xiao & Pengfe, 2023. "Constrained C2 adsorbate orientation enables CO-to-acetate electroreduction," Nature, Nature, vol. 617(7962), pages 724-729, May.
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