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Dilute alloy electrocatalysts enable asymmetric C–C coupling for ethylene production from a CO2 post-capture liquid

Abstract

Direct air capture of CO2 often uses alkali hydroxides to form carbonate; however, releasing CO2 and regenerating alkali hydroxides requires an energy-intensive thermal cycle at ~900 °C. Reactive capture systems instead seek to integrate CO2 release with its chemical reduction in the pathway to fuels and chemicals. Here we focus on a purely electrosynthetic route, beginning by examining why previous attempts at electrified ethylene synthesis from carbonate post-capture liquids have suffered from low overall energy efficiencies. We find that a hydrophilic environment and limited rate of CO2 generation in situ lead to low CO2 availability and consequently low *CO coverage on the catalyst surface, and that this hinders C–C coupling. We identify dilute alloy catalysts that implement asymmetric CO–CHO coupling, a lower-barrier route to C–C coupling compared with the conventional symmetric pathway. We report a 51% ± 2% ethylene Faradaic efficiency, a 66 wt% ± 2% concentrated ethylene stream and a 20% end-to-end energy efficiency at 200 mA cm−2. The energy efficiency is a twofold improvement over the most efficient prior report of ethylene production via electrified reactive capture.

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Fig. 1: Electrosynthesis of ethylene by using captured CO2 from air.
Fig. 2: Catalyst design for CO2-starved local environment.
Fig. 3: Catalytic behaviour of BiCu catalysts studied using dilute gas-fed electrocatalytic performance and operando Raman.
Fig. 4: Performance of ethylene production in a reactive capture carbonate electrolysis system.

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The authors declare that all data supporting the findings of this study are available within the Article and its Supplementary Information.

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Acknowledgements

This research received financial support from Saudi Aramco Technologies Company under agreement no. SATC-2022-016. Z.W. acknowledges the Marsden Fund Council from Government funding (21-UOA-237) and Catalyst: Seeding General Grant (22-UOA-031-CGS), managed by Royal Society Te Apārangi. Y.M. and Z.W. acknowledge the use of New Zealand eScience Infrastructure (NeSI) high-performance computing facilities, consulting support and/or training services as part of this research. This work made use of the EPIC facility of Northwestern University’s NUANCE Center, which has received support from the SHyNE Resource (NSF ECCS-2025633), the IIN, and Northwestern’s MRSEC programme (NSF DMR-2308691). This research used the beamline 9-BM of the Advanced Photon Source, a US Department of Energy (DOE) Office of Science user facility at Argonne National Laboratory and is based on research supported by the US DOE Office of Science-Basic Energy Sciences, under contract no. DE-AC02-06CH11357. This work also acknowledges valuable discussions on data analysis with S. Lee from beamline 12-BM of the Advanced Photon Source.

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E.H.S. and K.X. supervised the project. Z.W. supervised the DFT calculations. Y.C. conceived the idea, designed and synthesized materials, conducted the experiments and wrote the manuscript. P.W. assisted in material synthesis, electrocatalytic performance evaluation and material characterization. Y.M. performed the DFT calculations. G.S. conducted techno-economic analysis and life cycle assessment calculations under the supervision of J.B.D. H.L. and L.F. contributed to data analysis and discussions. B.P., Z.L. Y.W. and X.H. contributed to TEM measurements. H.Z. assisted with operando Raman measurements. J.L. and S.L. contributed to XAS measurements and data analysis. A.A., A.J. and I.G. supervised the project and contributed to manuscript preparation. All authors discussed the results and assisted during manuscript preparation.

Corresponding authors

Correspondence to Ziyun Wang, Ke Xie or Edward H. Sargent.

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Competing interests

There is a US provisional patent application titled ‘Energy-efficient electrified ethylene production from carbonate capture liquid’, filed by the authors Y.C., I.G., A.A., K.X. and E.H.S. of this Article and their institutions. The other authors declare no competing interests.

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Nature Synthesis thanks Yanqiang Huang 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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The atomic coordinates of the optimized models.

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Chen, Y., Wang, P., Mao, Y. et al. Dilute alloy electrocatalysts enable asymmetric C–C coupling for ethylene production from a CO2 post-capture liquid. Nat. Synth (2026). https://doi.org/10.1038/s44160-026-01024-5

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