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High-rate electroreduction of carbon monoxide to multi-carbon products

Nature Catalysisvolume 1pages748755 (2018) | Download Citation

Abstract

Carbon monoxide electrolysis has previously been reported to yield enhanced multi-carbon (C2+) Faradaic efficiencies of up to ~55%, but only at low reaction rates. This is due to the low solubility of CO in aqueous electrolytes and operation in batch-type reactors. Here, we present a high-performance CO flow electrolyser with a well controlled electrode–electrolyte interface that can reach total current densities of up to 1 A cm–2, together with improved C2+ selectivities. Computational transport modelling and isotopic C18O reduction experiments suggest that the enhanced activity is due to a higher surface pH under CO reduction conditions, which facilitates the production of acetate. At optimal operating conditions, we achieve a C2+ Faradaic efficiency of ~91% with a C2+ partial current density over 630 mA cm–2. Further investigations show that maintaining an efficient triple-phase boundary at the electrode–electrolyte interface is the most critical challenge in achieving a stable CO/CO2 electrolysis process at high rates.

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Change history

  • 15 November 2018

    The original Supplementary Information file published with this Article had the diffusion coefficient values of carbonate and hydrogen carbonate ions switched in the table below equation (21). A new Supplementary Information file has been uploaded with the correct values.

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Acknowledgements

We thank B. Xu and M. Dunwell for useful discussion. We also thank B. Murphy for help with the GC–MS experiments and B. Setzler for help with the transport model. This material is based on work supported by the Department of Energy under award number DE-FE0029868. The authors also thank the National Science Foundation Faculty Early Career Development Program (award number CBET-1350911). This research used resources of the Advanced Photon Source, a US Department of Energy Office of Science user facility operated for the Department of Energy Office of Science by Argonne National Laboratory under contract number DE-AC02-06CH11357.

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Affiliations

  1. Center for Catalytic Science and Technology, Department of Chemical and Biomolecular Engineering, University of Delaware, Newark, DE, USA

    • Matthew Jouny
    • , Wesley Luc
    •  & Feng Jiao

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Contributions

M.J. synthesized the electrodes, performed the XAS characterization, designed and performed the flow electrolysis experiments, analysed the data, and wrote the manuscript. W.L. performed the SEM, XPS and XRD characterizations, and surface pH calculations. F.J. supervised the project. All authors contributed to discussion of the results and manuscript preparation.

Competing interests

The authors declare no competing interests.

Corresponding author

Correspondence to Feng Jiao.

Supplementary information

  1. Supplementary Information

    Supplementary Methods, Supplementary Figures 1–16, Supplementary Tables 1 and 2, Supplementary References

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https://doi.org/10.1038/s41929-018-0133-2

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