IDEAS home Printed from https://ideas.repec.org/a/nat/natcom/v6y2015i1d10.1038_ncomms9177.html
   My bibliography  Save this article

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
    as

    Download full text from publisher

    File URL: https://www.nature.com/articles/ncomms9177
    File Function: Abstract
    Download Restriction: no
    File URL: https://libkey.io/10.1038/ncomms9177?utm_source=ideas
    LibKey link: if access is restricted and if your library uses this service, LibKey will redirect you to where you can use your library subscription to access this item
    ---><---

    Citations

    Citations are extracted by the CitEc Project, subscribe to its RSS feed for this item.
    as


    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).

    More about this item

    Statistics

    Access and download statistics

    Corrections

    All material on this site has been provided by the respective publishers and authors. You can help correct errors and omissions. When requesting a correction, please mention this item's handle: RePEc:nat:natcom:v:6:y:2015:i:1:d:10.1038_ncomms9177. See general information about how to correct material in RePEc.

    If you have authored this item and are not yet registered with RePEc, we encourage you to do it here. This allows to link your profile to this item. It also allows you to accept potential citations to this item that we are uncertain about.

    We have no bibliographic references for this item. You can help adding them by using this form .

    If you know of missing items citing this one, you can help us creating those links by adding the relevant references in the same way as above, for each refering item. If you are a registered author of this item, you may also want to check the "citations" tab in your RePEc Author Service profile, as there may be some citations waiting for confirmation.

    For technical questions regarding this item, or to correct its authors, title, abstract, bibliographic or download information, contact: Sonal Shukla or Springer Nature Abstracting and Indexing (email available below). General contact details of provider: http://www.nature.com .

    Please note that corrections may take a couple of weeks to filter through the various RePEc services.

    IDEAS is a RePEc service. RePEc uses bibliographic data supplied by the respective publishers.