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Single-site decorated copper enables energy- and carbon-efficient CO2 methanation in acidic conditions

Author

Listed:
  • Mengyang Fan

    (University of Toronto)

  • Rui Kai Miao

    (University of Toronto)

  • Pengfei Ou

    (University of Toronto)

  • Yi Xu

    (University of Toronto)

  • Zih-Yi Lin

    (National Yang Ming Chiao Tung University)

  • Tsung-Ju Lee

    (National Yang Ming Chiao Tung University)

  • Sung-Fu Hung

    (National Yang Ming Chiao Tung University)

  • Ke Xie

    (University of Toronto)

  • Jianan Erick Huang

    (University of Toronto)

  • Weiyan Ni

    (University of Toronto)

  • Jun Li

    (University of Toronto)

  • Yong Zhao

    (University of Toronto)

  • Adnan Ozden

    (University of Toronto)

  • Colin P. O’Brien

    (University of Toronto)

  • Yuanjun Chen

    (University of Toronto)

  • Yurou Celine Xiao

    (University of Toronto)

  • Shijie Liu

    (University of Toronto)

  • Joshua Wicks

    (University of Toronto)

  • Xue Wang

    (University of Toronto)

  • Jehad Abed

    (University of Toronto)

  • Erfan Shirzadi

    (University of Toronto)

  • Edward H. Sargent

    (University of Toronto)

  • David Sinton

    (University of Toronto)

Abstract

Renewable CH4 produced from electrocatalytic CO2 reduction is viewed as a sustainable and versatile energy carrier, compatible with existing infrastructure. However, conventional alkaline and neutral CO2-to-CH4 systems suffer CO2 loss to carbonates, and recovering the lost CO2 requires input energy exceeding the heating value of the produced CH4. Here we pursue CH4-selective electrocatalysis in acidic conditions via a coordination method, stabilizing free Cu ions by bonding Cu with multidentate donor sites. We find that hexadentate donor sites in ethylenediaminetetraacetic acid enable the chelation of Cu ions, regulating Cu cluster size and forming Cu-N/O single sites that achieve high CH4 selectivity in acidic conditions. We report a CH4 Faradaic efficiency of 71% (at 100 mA cm−2) with

Suggested Citation

  • 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.
    • Handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-38935-2
    DOI: 10.1038/s41467-023-38935-2
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    References listed on IDEAS

    as
    1. Yanming Cai & Jiaju Fu & Yang Zhou & Yu-Chung Chang & Qianhao Min & Jun-Jie Zhu & Yuehe Lin & Wenlei Zhu, 2021. "Insights on forming N,O-coordinated Cu single-atom catalysts for electrochemical reduction CO2 to methane," Nature Communications, Nature, vol. 12(1), pages 1-9, December.
    2. Chanyeon Kim & Justin C. Bui & Xiaoyan Luo & Jason K. Cooper & Ahmet Kusoglu & Adam Z. Weber & Alexis T. Bell, 2021. "Tailored catalyst microenvironments for CO2 electroreduction to multicarbon products on copper using bilayer ionomer coatings," Nature Energy, Nature, vol. 6(11), pages 1026-1034, November.
    3. Yi Xu & Fengwang Li & Aoni Xu & Jonathan P. Edwards & Sung-Fu Hung & Christine M. Gabardo & Colin P. O’Brien & Shijie Liu & Xue Wang & Yuhang Li & Joshua Wicks & Rui Kai Miao & Yuan Liu & Jun Li & Jia, 2021. "Low coordination number copper catalysts for electrochemical CO2 methanation in a membrane electrode assembly," Nature Communications, Nature, vol. 12(1), pages 1-7, December.
    4. Gorre, Jachin & Ortloff, Felix & van Leeuwen, Charlotte, 2019. "Production costs for synthetic methane in 2030 and 2050 of an optimized Power-to-Gas plant with intermediate hydrogen storage," Applied Energy, Elsevier, vol. 253(C), pages 1-1.
    5. Ghaib, Karim & Ben-Fares, Fatima-Zahrae, 2018. "Power-to-Methane: A state-of-the-art review," Renewable and Sustainable Energy Reviews, Elsevier, vol. 81(P1), pages 433-446.
    6. Danieli, Piero & Lazzaretto, Andrea & Al-Zaili, Jafar & Sayma, Abdulnaser & Masi, Massimo & Carraro, Gianluca, 2022. "The potential of the natural gas grid to accommodate hydrogen as an energy vector in transition towards a fully renewable energy system," Applied Energy, Elsevier, vol. 313(C).
    7. 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.
    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. Zhe Weng & Yueshen Wu & Maoyu Wang & Jianbing Jiang & Ke Yang & Shengjuan Huo & Xiao-Feng Wang & Qing Ma & Gary W. Brudvig & Victor S. Batista & Yongye Liang & Zhenxing Feng & Hailiang Wang, 2018. "Active sites of copper-complex catalytic materials for electrochemical carbon dioxide reduction," Nature Communications, Nature, vol. 9(1), pages 1-9, December.
    10. Vladimir Litvinenko, 2020. "The Role of Hydrocarbons in the Global Energy Agenda: The Focus on Liquefied Natural Gas," Resources, MDPI, vol. 9(5), pages 1-22, May.
    11. Sung-Fu Hung & Aoni Xu & Xue Wang & Fengwang Li & Shao-Hui Hsu & Yuhang Li & Joshua Wicks & Eduardo González Cervantes & Armin Sedighian Rasouli & Yuguang C. Li & Mingchuan Luo & Dae-Hyun Nam & Ning W, 2022. "A metal-supported single-atom catalytic site enables carbon dioxide hydrogenation," Nature Communications, Nature, vol. 13(1), pages 1-9, December.
    12. Adnan Ozden & F. Pelayo García de Arquer & Jianan Erick Huang & Joshua Wicks & Jared Sisler & Rui Kai Miao & Colin P. O’Brien & Geonhui Lee & Xue Wang & Alexander H. Ip & Edward H. Sargent & David Sin, 2022. "Carbon-efficient carbon dioxide electrolysers," Nature Sustainability, Nature, vol. 5(7), pages 563-573, July.
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