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Kilowatt-scale tandem CO2 electrolysis for enhanced acetate and ethylene production

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Abstract

The conversion of carbon dioxide (CO2) into valuable chemicals is a key strategy for carbon utilization. Although tandem CO2 electrolysis has shown promise, it has been largely confined to watt-scale studies and larger-scale studies are needed to accelerate commercialization. In this work, we demonstrate a tandem CO2 electrolyzer engineered for the production of multicarbon products, acetate and ethylene, at the kilowatt (kW) scale. Here, from insights gained at the watt scale, we have successfully designed and operated a 1,000 cm2 CO electrolyzer at 0.71 kW and a 500 cm2 CO2 electrolyzer at 0.40 kW. The kW-scale CO electrolyzer stack demonstrated a stable current of 300 A over 125 h, yielding 98 l of 1.2 M acetate at 96% purity. The system exhibited resilience against typical industrial impurities, maintaining high performance. These results mark a crucial advancement in scaling tandem CO2 electrolysis systems toward industrial feasibility. Finally, an experimentally informed techno-economic analysis is offered to provide a pathway for commercially viable tandem CO2 electrolysis at an industrial scale.

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Fig. 1: Two-step CO2 electrolysis stack for multicarbon chemical production.
Fig. 2: Watt-scale CO2 and CO electrolyzer performance.
Fig. 3: kW-scale two-step CO2 electrolysis.
Fig. 4: Effect of impurity content in CO electrolysis feed gas.
Fig. 5: Techno-economic analysis of tandem CO2 electrolysis.

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Data availability

All data needed to evaluate the conclusions in the paper are present in the paper and/or Supplementary Information. Source data for Figs. 2–4 have been included. Additional data related to this paper may be requested from the authors. Source data are provided with this paper.

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Acknowledgements

This work was supported by the US Department of Energy under award number DE-FE0031910. K. U. Hansen is acknowledged for his contributions to the integration of critical auxiliary safety components into the system that were necessary to mitigate the hazards associated with large-scale CO electrolysis experiments.

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Authors and Affiliations

  1. Center for Carbon Management, Department of Energy, Environmental, and Chemical Engineering, Washington University in St. Louis, St. Louis, MO, USA

    Bradie S. Crandall, Ahryeon Lee & Feng Jiao

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

    Bradie S. Crandall, Byung Hee Ko, Sean Overa, Luke Cherniack, Ahryeon Lee & Izak Minnie

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  1. Bradie S. Crandall
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Contributions

B.S.C., B.H.K., S.O. and F.J. designed all experiments. B.S.C. and B.H.K. wrote the paper. B.H.K. and S.O. conducted CO2 and CO electrolysis experiments up to 100 cm2. B.S.C. and S.O. designed the electrolyzer stack and conducted CO2 and CO electrolysis experiments for large reactors. B.H.K. and A.L. collected XPS measurements. L.C. conducted SEM and EDS measurements. B.S.C. and I.M. carried out material preparation for stack testing. F.J. supervised the whole project. All authors participated in the discussion and the preparation of the paper.

Corresponding author

Correspondence to Feng Jiao.

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Nature Chemical Engineering thanks Ming Ma, **gjie Wu and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Supplementary Discussions 1 and 2, Figs. 1–25 and Tables 1–5.

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Crandall, B.S., Ko, B.H., Overa, S. et al. Kilowatt-scale tandem CO2 electrolysis for enhanced acetate and ethylene production. Nat Chem Eng 1, 421–429 (2024). https://doi.org/10.1038/s44286-024-00076-8

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