Abstract
Electrochemical reduction of carbon monoxide is a promising carbonate-free approach to produce ethylene using renewable electricity. However, the performance of this process suffers from low selectivity and energy efficiency. A priority has been to weaken water dissociation with the aim of inhibiting the competing hydrogen evolution reaction but when this path was examined by replacing H2O with D2O, a further-reduced selectivity toward ethylene was observed. Here we examine approaches to promote water adsorption and to decrease the energy barrier to the ensuing water dissociation step, which could promote C–O cleavage in *CHCOH hydrogenation to *CCH. We modified a copper catalyst with the strong electron acceptor 7,7,8,8-tetracyanoquinodimethane, which made the catalyst surface electron deficient. The observed ethylene Faradaic efficiency was 75%, 1.3 times greater than that of unmodified copper control catalysts. A full-cell energy efficiency of 32% was achieved for a total projected energy cost of 154 GJ t−1 in ethylene electrosynthesis in a membrane electrode assembly.
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Acknowledgements
The authors acknowledge funding from the Natural Sciences and Engineering Research Council of Canada (NSERC) and TotalEnergies SE (TotalEnergies Research & Technology Feluy (an affiliate of TotalEnergies SE, France)). J.Z. acknowledges support from NSFC (22250007, 22361162655). J.Z. and Fengwang Li are grateful to the International Partnership Program of the Chinese Academy of Sciences (123GJHZ2022101GC). W.N. acknowledges financial support from the Swiss National Science Foundation (SNSF) for a Postdoctoral Mobility Fellowship (202906).
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Contributions
E.H.S, D.S., J.Z. and Fengwang Li supervised the project. Y. Liang synthesized the catalysts and performed all the electrochemical experiments. Feng Li carried out the DFT calculations, ab initio molecular dynamics simulation, and multiphysics simulation. P.O. and X.-Y.L. participated in the computational data analysis. R.K.M performed the cascade system modelling and calculated the energy cost. S.H. performed transmission electron microscopy, high-resolution transmission electron microscopy and energy-dispersive X-ray spectroscopy mapping experiments. W.N. and S.P. assisted in electrochemical and operando Raman experiments. S.Z. conducted the operando XAS experiments. Y. Liu carried out the XPS experiments. Y.B. contributed to the CORR isotope experiments and data analysis. H.W. assisted in the X-ray diffraction experiments. N.W. provided the NiFe-B anode catalysts. Y. Liang, E.H.S., Fengwang Li and D.S. co-wrote and edited the manuscript. All authors discussed the results and assisted during the manuscript preparation.
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Nature Synthesis thanks Yongji Gong and the other, anonymous, reviewer(s) for their contribution to the peer review of this work. Primary Handling Editor: Alexandra Groves, in collaboration with the Nature Synthesis team.
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Liang, Y., Li, F., Miao, R.K. et al. Efficient ethylene electrosynthesis through C–O cleavage promoted by water dissociation. Nat. Synth 3, 1104–1112 (2024). https://doi.org/10.1038/s44160-024-00568-8
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DOI: https://doi.org/10.1038/s44160-024-00568-8
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