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Dopant-tuned stabilization of intermediates promotes electrosynthesis of valuable C3 products

Author

Listed:
  • Tao-Tao Zhuang

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

  • Dae-Hyun Nam

    (University of Toronto)

  • Ziyun Wang

    (University of Toronto)

  • Hui-Hui Li

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

  • Christine M. Gabardo

    (University of Toronto)

  • Yi Li

    (University of Science and Technology of China)

  • Zhi-Qin Liang

    (University of Toronto)

  • Jun Li

    (University of Toronto
    University of Toronto)

  • Xiao-Jing Liu

    (University of Science and Technology of China)

  • Bin Chen

    (University of Toronto)

  • Wan Ru Leow

    (University of Toronto)

  • Rui Wu

    (University of Science and Technology of China)

  • Xue Wang

    (University of Toronto)

  • Fengwang Li

    (University of Toronto)

  • Yanwei Lum

    (University of Toronto)

  • Joshua Wicks

    (University of Toronto)

  • Colin P. O’Brien

    (University of Toronto)

  • Tao Peng

    (University of Toronto)

  • Alexander H. Ip

    (University of Toronto)

  • Tsun-Kong Sham

    (University of Western Ontario)

  • Shu-Hong Yu

    (University of Science and Technology of China)

  • David Sinton

    (University of Toronto)

  • Edward H. Sargent

    (University of Toronto)

Abstract

The upgrading of CO2/CO feedstocks to higher-value chemicals via energy-efficient electrochemical processes enables carbon utilization and renewable energy storage. Substantial progress has been made to improve performance at the cathodic side; whereas less progress has been made on improving anodic electro-oxidation reactions to generate value. Here we report the efficient electroproduction of value-added multi-carbon dimethyl carbonate (DMC) from CO and methanol via oxidative carbonylation. We find that, compared to pure palladium controls, boron-doped palladium (Pd-B) tunes the binding strength of intermediates along this reaction pathway and favors DMC formation. We implement this doping strategy and report the selective electrosynthesis of DMC experimentally. We achieve a DMC Faradaic efficiency of 83 ± 5%, fully a 3x increase in performance compared to the corresponding pure Pd electrocatalyst.

Suggested Citation

  • Tao-Tao Zhuang & Dae-Hyun Nam & Ziyun Wang & Hui-Hui Li & Christine M. Gabardo & Yi Li & Zhi-Qin Liang & Jun Li & Xiao-Jing Liu & Bin Chen & Wan Ru Leow & Rui Wu & Xue Wang & Fengwang Li & Yanwei Lum , 2019. "Dopant-tuned stabilization of intermediates promotes electrosynthesis of valuable C3 products," Nature Communications, Nature, vol. 10(1), pages 1-7, December.
    • Handle: RePEc:nat:natcom:v:10:y:2019:i:1:d:10.1038_s41467-019-12788-0
    DOI: 10.1038/s41467-019-12788-0
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