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Electrochemically converting carbon monoxide to liquid fuels by directing selectivity with electrode surface area

Nature Catalysis volume 2, pages 702–708 (2019)Cite this article

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Abstract

Using renewable electricity to convert CO/CO2 into liquid products is touted as a sustainable process to produce fuels and chemicals, yet requires further advances in electrocatalyst understanding, development and device integration. The roughness factor of an electrode has generally been used to increase total rates of production, although rarely as a means to improve selectivity. Here we demonstrate that increasing the roughness factor of Cu electrodes is an effective design principle to direct the selectivity of CO reduction towards multicarbon oxygenates at low overpotentials and concurrently suppressing hydrocarbon and hydrogen production. The nanostructured Cu electrodes are capable of achieving almost full selectivity towards multicarbon oxygenates at an electrode potential of only –0.23 V versus the reversible hydrogen electrode. The successful implementation of this catalytic system has enabled an excellent CO reduction performance and elucidated viable pathways to improve the energy efficiency towards liquid fuels in high-power conversion electrolysers.

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Fig. 1: COR electrode development strategy.
Fig. 2: Surface characterization of Cu nanoflower electrodes under different stages.
Fig. 3: COR by Cu nanoflower electrodes in 0.1 M KOH saturated with 1 atm of CO at ambient temperature.
Fig. 4: Activity comparison between the Cu nanoflower electrode and planar pc-Cu (ref. 22), OD-Cu (ref. 20) and NW-Cu (ref. 21).
Fig. 5: COR on several different porous Cu materials in 0.1 M KOH at a potential of ~0.33 V versus the RHE.

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The data that support the results and other findings of this study are available from the corresponding authors upon reasonable request.

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Acknowledgements

This material is based on work performed by the Joint Center for Artificial Photosynthesis, a DOE Energy Innovation Hub, supported through the Office of Science of the US Department of Energy under Award no. DE-SC0004993. Part of this work was performed at the Stanford Nano Shared Facilities (SNSF), supported by the National Science Foundation under Award ECCS-1542152. Additional thanks go to the Stanford NMR Facility. We thank S. Xu for the constructive discussions. L.W. thanks the Knut & Alice Wallenberg Foundation for financial support.

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Authors and Affiliations

  1. SUNCAT Center for Interface Science and Catalysis, Department of Chemical Engineering, Stanford University, Stanford, CA, USA

    Lei Wang, Stephanie Nitopi, Andrew B. Wong, Jonathan L. Snider, Adam C. Nielander, Carlos G. Morales-Guio, Marat Orazov, Drew C. Higgins & Thomas F. Jaramillo

  2. SUNCAT Center for Interface Science and Catalysis, SLAC National Accelerator Laboratory, Menlo Park, CA, USA

    Drew C. Higgins, Christopher Hahn & Thomas F. Jaramillo

  3. Department of Chemical Engineering, McMaster University, Hamilton, ON, Canada

    Drew C. Higgins

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Contributions

L.W. synthesized the Cu nanoflower electrodes, and designed and performed the electrochemistry experiments. S.A.N., C.G.M.-G., M.O. and D.C.H. conducted the electrochemistry experiments. L.W. and A.C.N. carried out the SEM and XPS measurements. A.B.W. and J.L.S. performed the TEM experiments. All the authors analysed the experimental data. T.F.J. and C.H. conceived the project and supervised the research work. L.W., C.H. and T.F.J. wrote the manuscript with input from the other authors.

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Correspondence to Christopher Hahn or Thomas F. Jaramillo.

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Supplementary Figs. 1–17, Supplementary Tables 1–3, Supplementary Notes 1 and 2 and Supplementary References.

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Wang, L., Nitopi, S., Wong, A.B. et al. Electrochemically converting carbon monoxide to liquid fuels by directing selectivity with electrode surface area. Nat Catal 2, 702–708 (2019). https://doi.org/10.1038/s41929-019-0301-z

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