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Promoting CO2 methanation via ligand-stabilized metal oxide clusters as hydrogen-donating motifs

Author

Listed:
  • Yuhang Li

    (University of Toronto
    East China University of Science and Technology)

  • Aoni Xu

    (University of Toronto)

  • Yanwei Lum

    (University of Toronto)

  • Xue Wang

    (University of Toronto)

  • Sung-Fu Hung

    (University of Toronto)

  • Bin Chen

    (University of Toronto)

  • Ziyun Wang

    (University of Toronto)

  • Yi Xu

    (University of Toronto)

  • Fengwang Li

    (University of Toronto)

  • Jehad Abed

    (University of Toronto
    University of Toronto)

  • Jianan Erick Huang

    (University of Toronto)

  • Armin Sedighian Rasouli

    (University of Toronto)

  • Joshua Wicks

    (University of Toronto)

  • Laxmi Kishore Sagar

    (University of Toronto)

  • Tao Peng

    (University of Toronto)

  • Alexander H. Ip

    (University of Toronto)

  • David Sinton

    (University of Toronto)

  • Hao Jiang

    (East China University of Science and Technology
    East China University of Science and Technology)

  • Chunzhong Li

    (East China University of Science and Technology
    East China University of Science and Technology)

  • Edward H. Sargent

    (University of Toronto)

Abstract

Electroreduction uses renewable energy to upgrade carbon dioxide to value-added chemicals and fuels. Renewable methane synthesized using such a route stands to be readily deployed using existing infrastructure for the distribution and utilization of natural gas. Here we design a suite of ligand-stabilized metal oxide clusters and find that these modulate carbon dioxide reduction pathways on a copper catalyst, enabling thereby a record activity for methane electroproduction. Density functional theory calculations show adsorbed hydrogen donation from clusters to copper active sites for the *CO hydrogenation pathway towards *CHO. We promote this effect via control over cluster size and composition and demonstrate the effect on metal oxides including cobalt(II), molybdenum(VI), tungsten(VI), nickel(II) and palladium(II) oxides. We report a carbon dioxide-to-methane faradaic efficiency of 60% at a partial current density to methane of 135 milliampere per square centimetre. We showcase operation over 18 h that retains a faradaic efficiency exceeding 55%.

Suggested Citation

  • Yuhang Li & Aoni Xu & Yanwei Lum & Xue Wang & Sung-Fu Hung & Bin Chen & Ziyun Wang & Yi Xu & Fengwang Li & Jehad Abed & Jianan Erick Huang & Armin Sedighian Rasouli & Joshua Wicks & Laxmi Kishore Saga, 2020. "Promoting CO2 methanation via ligand-stabilized metal oxide clusters as hydrogen-donating motifs," Nature Communications, Nature, vol. 11(1), pages 1-8, December.
  • Handle: RePEc:nat:natcom:v:11:y:2020:i:1:d:10.1038_s41467-020-20004-7
    DOI: 10.1038/s41467-020-20004-7
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    Cited by:

    1. 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).
    2. Zishan Han & Daliang Han & Zhe Chen & Jiachen Gao & Guangyi Jiang & Xinyu Wang & Shuaishuai Lyu & Yong Guo & Chuannan Geng & Lichang Yin & Zhe Weng & Quan-Hong Yang, 2022. "Steering surface reconstruction of copper with electrolyte additives for CO2 electroreduction," Nature Communications, Nature, vol. 13(1), pages 1-10, December.
    3. Cornelius A. Obasanjo & Guorui Gao & Jackson Crane & Viktoria Golovanova & F. Pelayo García de Arquer & Cao-Thang Dinh, 2023. "High-rate and selective conversion of CO2 from aqueous solutions to hydrocarbons," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
    4. Mengyang Fan & Rui Kai Miao & Pengfei Ou & Yi Xu & Zih-Yi Lin & Tsung-Ju Lee & Sung-Fu Hung & Ke Xie & Jianan Erick Huang & Weiyan Ni & Jun Li & Yong Zhao & Adnan Ozden & Colin P. O’Brien & Yuanjun Ch, 2023. "Single-site decorated copper enables energy- and carbon-efficient CO2 methanation in acidic conditions," Nature Communications, Nature, vol. 14(1), pages 1-8, December.
    5. Yizhou Dai & Huan Li & Chuanhao Wang & Weiqing Xue & Menglu Zhang & Donghao Zhao & Jing Xue & Jiawei Li & Laihao Luo & Chunxiao Liu & Xu Li & Peixin Cui & Qiu Jiang & Tingting Zheng & Songqi Gu & Yao , 2023. "Manipulating local coordination of copper single atom catalyst enables efficient CO2-to-CH4 conversion," Nature Communications, Nature, vol. 14(1), pages 1-12, December.

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