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Isolated copper single sites for high-performance electroreduction of carbon monoxide to multicarbon products

Author

Listed:
  • Haihong Bao

    (Tianjin University of Technology)

  • Yuan Qiu

    (Tianjin University of Technology)

  • Xianyun Peng

    (Tianjin University of Technology)

  • Jia-ao Wang

    (University of Jinan)

  • Yuying Mi

    (Tianjin University of Technology)

  • Shunzheng Zhao

    (University of Science and Technology Beijing)

  • Xijun Liu

    (Tianjin University of Technology
    Civil Aviation University of China)

  • Yifan Liu

    (Shenzhen University)

  • Rui Cao

    (Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory)

  • Longchao Zhuo

    (Xi’an University of Technology)

  • Junqiang Ren

    (Lanzhou University of Technology)

  • Jiaqiang Sun

    (Institute of Coal Chemistry, Chinese Academy of Sciences)

  • Jun Luo

    (Tianjin University of Technology)

  • Xuping Sun

    (University of Electronic Science and Technology of China)

Abstract

Electrochemical carbon monoxide reduction is a promising strategy for the production of value-added multicarbon compounds, albeit yielding diverse products with low selectivities and Faradaic efficiencies. Here, copper single atoms anchored to Ti3C2Tx MXene nanosheets are firstly demonstrated as effective and robust catalysts for electrochemical carbon monoxide reduction, achieving an ultrahigh selectivity of 98% for the formation of multicarbon products. Particularly, it exhibits a high Faradaic efficiency of 71% towards ethylene at −0.7 V versus the reversible hydrogen electrode, superior to the previously reported copper-based catalysts. Besides, it shows a stable activity during the 68-h electrolysis. Theoretical simulations reveal that atomically dispersed Cu–O3 sites favor the C–C coupling of carbon monoxide molecules to generate the key *CO-CHO species, and then induce the decreased free energy barrier of the potential-determining step, thus accounting for the high activity and selectivity of copper single atoms for carbon monoxide reduction.

Suggested Citation

  • Haihong Bao & Yuan Qiu & Xianyun Peng & Jia-ao Wang & Yuying Mi & Shunzheng Zhao & Xijun Liu & Yifan Liu & Rui Cao & Longchao Zhuo & Junqiang Ren & Jiaqiang Sun & Jun Luo & Xuping Sun, 2021. "Isolated copper single sites for high-performance electroreduction of carbon monoxide to multicarbon products," Nature Communications, Nature, vol. 12(1), pages 1-9, December.
    • Handle: RePEc:nat:natcom:v:12:y:2021:i:1:d:10.1038_s41467-020-20336-4
    DOI: 10.1038/s41467-020-20336-4
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    Cited by:

    1. Yongxiang Liang & Jiankang Zhao & Yu Yang & Sung-Fu Hung & Jun Li & Shuzhen Zhang & Yong Zhao & An Zhang & Cheng Wang & Dominique Appadoo & Lei Zhang & Zhigang Geng & Fengwang Li & Jie Zeng, 2023. "Stabilizing copper sites in coordination polymers toward efficient electrochemical C-C coupling," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    2. Ting Zhang & Zhe Sun & Shiyan Li & Baojun Wang & Yuefeng Liu & Riguang Zhang & Zhongkui Zhao, 2022. "Regulating electron configuration of single Cu sites via unsaturated N,O-coordination for selective oxidation of benzene," Nature Communications, Nature, vol. 13(1), pages 1-8, December.
    3. Dong Cao & Haoxiang Xu & Hongliang Li & Chen Feng & Jie Zeng & Daojian Cheng, 2022. "Volcano-type relationship between oxidation states and catalytic activity of single-atom catalysts towards hydrogen evolution," Nature Communications, Nature, vol. 13(1), pages 1-11, December.
    4. Jie Ding & Zhiming Wei & Fuhua Li & Jincheng Zhang & Qiao Zhang & Jing Zhou & Weijue Wang & Yuhang Liu & Zhen Zhang & Xiaozhi Su & Runze Yang & Wei Liu & Chenliang Su & Hong Bin Yang & Yanqiang Huang , 2023. "Atomic high-spin cobalt(II) center for highly selective electrochemical CO reduction to CH3OH," Nature Communications, Nature, vol. 14(1), pages 1-10, December.

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