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Efficient CO and acrolein co-production via paired electrolysis

Nature Sustainability volume 7, pages 931–937 (2024)Cite this article

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Abstract

Paired electrolysis—the combination of a productive cathodic reaction, such as CO2 electroreduction (CO2RR), with selective oxidation on the anode—provides an electrified reaction with maximized atom and energy efficiencies. Unfortunately, direct electro-oxidation reactions typically exhibit limited Faradaic efficiencies (FEs) towards a single product. Here we apply paired electrolysis for acidic CO2RR and the model organic oxidation allyl alcohol oxidation reaction to acrolein. This CO2RR alcohol oxidation reaction system shows (96 ± 1)% FE of CO2 to CO on the cathode and (85 ± 1)% FE of allyl alcohol to acrolein on the anode. As a result of this pairing with organic oxidation on the anode, the full-cell voltage of the system is lowered by 0.7 V compared with the state-of-art acidic CO2-to-CO studies at the same 100 mA cm−2 current density. The acidic cathode avoids carbonate formation and enables a single-pass utilization of CO2 of 84% with a 6× improvement in the atom efficiency of CO2 utilization. Energy consumption analysis suggests that, when producing the same amount of CO, the system reduces energy consumption by an estimated 1.6× compared with the most energy-efficient prior acidic CO2-to-CO ambient-temperature electrolysis systems. The work suggests that paired electrolysis could be a decarbonization technology to contribute to a sustainable future.

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Fig. 1: A paired electrolysis system co-producing CO and acrolein.
Fig. 2: CO2RR performance in the CO2RR-OER system.
Fig. 3: AOR performance in the CO2RR-AOR system.
Fig. 4: AOR and CO2RR performance in the CO2RR-AOR system.
Fig. 5: Comparison of estimated energy consumption for the production of 1 kg of CO.

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All data are available within the paper, Supplementary Information and source data file. Source data are provided with this paper.

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Acknowledgements

This work was supported by the Natural Sciences and Engineering Research Council (NSERC) of Canada and the Ontario Research Fund – Research Excellence programme. D.S. acknowledges the NSERC E. W. R. Steacie Memorial Fellowship. The authors thank R. Wolowiec and D. Kopilovic for their kind technical assistance. Electron microscopy characterization was performed at the Open Centre for the Characterization of Advanced Materials (OCCAM) in University of Toronto.

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Author notes

  1. These authors contributed equally: Xue Wang, Peihao Li.

Authors and Affiliations

  1. Department of Electrical and Computer Engineering, University of Toronto, Toronto, Ontario, Canada

    Xue Wang, Peihao Li, Armin Sedighian Rasouli, Yuan Liu, Ke Xie & Edward H. Sargent

  2. School of Energy and Environment, City University of Hong Kong, Kowloon, Hong Kong, China

    Xue Wang

  3. Department of Materials Science and Engineering, University of Toronto, Toronto, Ontario, Canada

    Jason Tam & Jane Y. Howe

  4. Department of Chemical Engineering and Applied Chemistry, University of Toronto, Toronto, Ontario, Canada

    Jane Y. Howe

  5. Department of Mechanical and Industrial Engineering, University of Toronto, Toronto, Ontario, Canada

    Colin P. O’Brien, Rui Kai Miao, Adnan Ozden, Jinhong Wu & David Sinton

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Contributions

E.H.S. supervised the project. X.W. conceived the idea and designed the experiments. P.L. prepared the samples and carried out the electrochemical experiments. J.T. and J.Y.H. contributed to the SEM and TEM characterization. X.W., C.P.O., K.X. and J.W. did the analysis of energy consumption. A.S.R. carried out XPS measurements. X.W. and Y.L. performed XRD measurements. X.W., P.L. and E.H.S. co-wrote the manuscript. R.K.M., A.O. and D.S. assisted with the discussions. All authors discussed the results and assisted during manuscript preparation.

Corresponding author

Correspondence to Edward H. Sargent.

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Nature Sustainability thanks Ki Tae Nam and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Supplementary information

Supplementary Information

Supplementary Figs. 1–23, Tables 1–8 and References 1–10.

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Source data

Source Data Fig. 5

Source data for anodic liquid product separation in Fig. 5.

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Wang, X., Li, P., Tam, J. et al. Efficient CO and acrolein co-production via paired electrolysis. Nat Sustain 7, 931–937 (2024). https://doi.org/10.1038/s41893-024-01363-1

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