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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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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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.
The authors declare no competing interests.
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Supplementary Figs. 1–17, Supplementary Tables 1–3, Supplementary Notes 1 and 2 and Supplementary References.