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Enhanced multi-carbon alcohol electroproduction from CO via modulated hydrogen adsorption

Author

Listed:
  • Jun Li

    (University of Toronto
    University of Toronto)

  • Aoni Xu

    (University of Toronto
    University of Science and Technology Beijing)

  • Fengwang Li

    (University of Toronto)

  • Ziyun Wang

    (University of Toronto)

  • Chengqin Zou

    (University of Toronto
    Tianjin University)

  • Christine M. Gabardo

    (University of Toronto)

  • Yuhang Wang

    (University of Toronto)

  • Adnan Ozden

    (University of Toronto)

  • Yi Xu

    (University of Toronto)

  • Dae-Hyun Nam

    (University of Toronto)

  • Yanwei Lum

    (University of Toronto)

  • Joshua Wicks

    (University of Toronto)

  • Bin Chen

    (University of Toronto)

  • Zhiqiang Wang

    (University of Western Ontario)

  • Jiatang Chen

    (University of Western Ontario)

  • Yunzhou Wen

    (Fudan University)

  • Taotao Zhuang

    (University of Toronto)

  • Mingchuan Luo

    (University of Toronto)

  • Xiwen Du

    (Tianjin University)

  • Tsun-Kong Sham

    (University of Western Ontario)

  • Bo Zhang

    (Fudan University)

  • Edward H. Sargent

    (University of Toronto)

  • David Sinton

    (University of Toronto)

Abstract

Multi-carbon alcohols such as ethanol are valued as fuels in view of their high energy density and ready transport. Unfortunately, the selectivity toward alcohols in CO2/CO electroreduction is diminished by ethylene production, especially when operating at high current densities (>100 mA cm−2). Here we report a metal doping approach to tune the adsorption of hydrogen at the copper surface and thereby promote alcohol production. Using density functional theory calculations, we screen a suite of transition metal dopants and find that incorporating Pd in Cu moderates hydrogen adsorption and assists the hydrogenation of C2 intermediates, providing a means to favour alcohol production and suppress ethylene. We synthesize a Pd-doped Cu catalyst that achieves a Faradaic efficiency of 40% toward alcohols and a partial current density of 277 mA cm−2 from CO electroreduction. The activity exceeds that of prior reports by a factor of 2.

Suggested Citation

  • 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.
    • Handle: RePEc:nat:natcom:v:11:y:2020:i:1:d:10.1038_s41467-020-17499-5
    DOI: 10.1038/s41467-020-17499-5
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    Cited by:

    1. Xinyue Wang & Yuanjun Chen & Feng Li & Rui Kai Miao & Jianan Erick Huang & Zilin Zhao & Xiao-Yan Li & Roham Dorakhan & Senlin Chu & Jinhong Wu & Sixing Zheng & Weiyan Ni & Dongha Kim & Sungjin Park & , 2024. "Site-selective protonation enables efficient carbon monoxide electroreduction to acetate," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    2. Guifeng Ma & Olga A. Syzgantseva & Yan Huang & Dragos Stoian & Jie Zhang & Shuliang Yang & Wen Luo & Mengying Jiang & Shumu Li & Chunjun Chen & Maria A. Syzgantseva & Sen Yan & Ningyu Chen & Li Peng &, 2023. "A hydrophobic Cu/Cu2O sheet catalyst for selective electroreduction of CO to ethanol," Nature Communications, Nature, vol. 14(1), pages 1-9, December.
    3. Chen, Zhangsen & Zhang, Gaixia & Chen, Hangrong & Prakash, Jai & Zheng, Yi & Sun, Shuhui, 2022. "Multi-metallic catalysts for the electroreduction of carbon dioxide: Recent advances and perspectives," Renewable and Sustainable Energy Reviews, Elsevier, vol. 155(C).
    4. Jing Li & Haocheng Xiong & Xiaozhi Liu & Donghuan Wu & Dong Su & Bingjun Xu & Qi Lu, 2023. "Weak CO binding sites induced by Cu–Ag interfaces promote CO electroreduction to multi-carbon liquid products," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    5. 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.
    6. Di Wang & Hyun Dong Jung & Shikai Liu & Jiayi Chen & Haozhou Yang & Qian He & Shibo Xi & Seoin Back & Lei Wang, 2024. "Revealing the structural evolution of CuAg composites during electrochemical carbon monoxide reduction," Nature Communications, Nature, vol. 15(1), pages 1-13, December.
    7. Manjeet Chhetri & Mingyu Wan & Zehua Jin & John Yeager & Case Sandor & Conner Rapp & Hui Wang & Sungsik Lee & Cameron J. Bodenschatz & Michael J. Zachman & Fanglin Che & Ming Yang, 2023. "Dual-site catalysts featuring platinum-group-metal atoms on copper shapes boost hydrocarbon formations in electrocatalytic CO2 reduction," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
    8. Kaihang Yue & Yanyang Qin & Honghao Huang & Zhuoran Lv & Mingzhi Cai & Yaqiong Su & Fuqiang Huang & Ya Yan, 2024. "Stabilized Cu0 -Cu1+ dual sites in a cyanamide framework for selective CO2 electroreduction to ethylene," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    9. Wenzhe Niu & Jie Feng & Junfeng Chen & Lei Deng & Wen Guo & Huajing Li & Liqiang Zhang & Youyong Li & Bo Zhang, 2024. "High-efficiency C3 electrosynthesis on a lattice-strain-stabilized nitrogen-doped Cu surface," Nature Communications, Nature, vol. 15(1), pages 1-13, December.

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