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Electrocatalytic reduction of carbon dioxide to carbon monoxide and methane at an immobilized cobalt protoporphyrin

Author

Listed:
  • Jing Shen

    (Leiden Institute of Chemistry, Leiden University)

  • Ruud Kortlever

    (Leiden Institute of Chemistry, Leiden University)

  • Recep Kas

    (PhotoCatalytic Synthesis Group, MESA+ Institute for Nanotechnology, Faculty of Science and Technology, University of Twente)

  • Yuvraj Y. Birdja

    (Leiden Institute of Chemistry, Leiden University)

  • Oscar Diaz-Morales

    (Leiden Institute of Chemistry, Leiden University)

  • Youngkook Kwon

    (Leiden Institute of Chemistry, Leiden University)

  • Isis Ledezma-Yanez

    (Leiden Institute of Chemistry, Leiden University)

  • Klaas Jan P. Schouten

    (Leiden Institute of Chemistry, Leiden University)

  • Guido Mul

    (PhotoCatalytic Synthesis Group, MESA+ Institute for Nanotechnology, Faculty of Science and Technology, University of Twente)

  • Marc T. M. Koper

    (Leiden Institute of Chemistry, Leiden University)

Abstract

The electrochemical conversion of carbon dioxide and water into useful products is a major challenge in facilitating a closed carbon cycle. Here we report a cobalt protoporphyrin immobilized on a pyrolytic graphite electrode that reduces carbon dioxide in an aqueous acidic solution at relatively low overpotential (0.5 V), with an efficiency and selectivity comparable to the best porphyrin-based electrocatalyst in the literature. While carbon monoxide is the main reduction product, we also observe methane as by-product. The results of our detailed pH-dependent studies are explained consistently by a mechanism in which carbon dioxide is activated by the cobalt protoporphyrin through the stabilization of a radical intermediate, which acts as Brønsted base. The basic character of this intermediate explains how the carbon dioxide reduction circumvents a concerted proton–electron transfer mechanism, in contrast to hydrogen evolution. Our results and their mechanistic interpretations suggest strategies for designing improved catalysts.

Suggested Citation

  • Jing Shen & Ruud Kortlever & Recep Kas & Yuvraj Y. Birdja & Oscar Diaz-Morales & Youngkook Kwon & Isis Ledezma-Yanez & Klaas Jan P. Schouten & Guido Mul & Marc T. M. Koper, 2015. "Electrocatalytic reduction of carbon dioxide to carbon monoxide and methane at an immobilized cobalt protoporphyrin," Nature Communications, Nature, vol. 6(1), pages 1-8, November.
    • Handle: RePEc:nat:natcom:v:6:y:2015:i:1:d:10.1038_ncomms9177
    DOI: 10.1038/ncomms9177
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    Cited by:

    1. Xiao, Shuai & Fu, Qian & Xiong, Kerui & Li, Zhuo & Li, Jun & Zhang, Liang & Liao, Qiang & Zhu, Xun, 2020. "Parametric study of biocathodes in microbial electrosynthesis for CO2 reduction to CH4 with a direct electron transfer pathway," Renewable Energy, Elsevier, vol. 162(C), pages 438-446.
    2. Hidalgo, D. & Martín-Marroquín, J.M., 2020. "Power-to-methane, coupling CO2 capture with fuel production: An overview," Renewable and Sustainable Energy Reviews, Elsevier, vol. 132(C).
    3. Zhang, Xue & Li, Fanghua & Wang, Jiahong & Zhao, Haitao & Yu, Xue-Feng, 2021. "Strategy for improving the activity and selectivity of CO2 electroreduction on flexible carbon materials for carbon neutral," Applied Energy, Elsevier, vol. 298(C).
    4. Subhabrata Mukhopadhyay & Muhammad Saad Naeem & G. Shiva Shanker & Arnab Ghatak & Alagar R. Kottaichamy & Ran Shimoni & Liat Avram & Itamar Liberman & Rotem Balilty & Raya Ifraemov & Illya Rozenberg &, 2024. "Local CO2 reservoir layer promotes rapid and selective electrochemical CO2 reduction," Nature Communications, Nature, vol. 15(1), pages 1-14, December.

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