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Organic electrolyte cations promote non-aqueous CO2 reduction by mediating interfacial electric fields

Nature Catalysis volume 8, pages 79–91 (2025)Cite this article

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Abstract

The electrochemical reduction of CO2 is sensitive to the microenvironment surrounding catalytic active sites. Although the impact of changing electrolyte composition on rates has been studied intensively in aqueous electrolytes, less is known about the influence of the electrochemical environment in non-aqueous solvents. Here we demonstrate that organic alkylammonium cations influence catalytic performance in non-aqueous media and describe a physical model that rationalizes these observations. Using results from kinetic, spectroscopic and computational techniques, we argue that the strength of the electric field at the catalyst surface is sensitive to the molecular identity of the organic cation in the electrolyte. This is true irrespective of solvent, electrolyte ionic strength or electrolyte anion. Our results suggest that changes in the interfacial electric field strength can be attributed to differences in the cation–electrode distance. Changes in the electric field strength affect CO formation rates as they modify the energetics of the kinetically relevant CO2 activation step.

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Fig. 1: Effect of organic cations on CO2R in aprotic electrolytes.
Fig. 2: Effect of changing electrolyte ionic strength on CO2R rates.
Fig. 3: Effect of changing electrolyte counteranion.
Fig. 4: Proposed model of the impact of organic alkylammonium cations on CO2R reactivity.
Fig. 5: Understanding the mechanism of CO2R to CO in aprotic electrolytes.
Fig. 6: Spectroscopic probes of cation-mediated field strength.
Fig. 7: Computationally probing the effect of cation size on interfacial fields.
Fig. 8: Isolating the effect of cation–electrode distance on CO2R reactivity.

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Data availability

Computational datasets are available at the UCPH repository: https://sid.erda.dk/sharelink/hxqah2G0De. This includes all trajectory files from both relaxation and molecular dynamics simulations and covers initial and final configurations. Experimental datasets can be obtained from the corresponding author upon reasonable request.

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Acknowledgements

J.M. gratefully acknowledges the support of ExxonMobil Corporation through the Future Leaders Academy Ph.D. Fellowship. Findings and conclusions are those of the author and do not reflect the views of ExxonMobil Corporation. J.F.B and J. Resasco gratefully acknowledge support from the Robert A. Welch Foundation (Grants F-1945 and F-2076, respectively). We thank A. Kennedy from the University of Texas at Austin Dept. of Chemistry’s Glass Shop for the construction of electrochemistry glass cell components and D. Davies for assistance with graphic design. J.T.B. gratefully acknowledges the support of the National Science Foundation Graduate Research Fellowship Program (NSF-GRFP) under Grant Nos. DGE-1610403 and DGE-2137420. A.S.P and J. Rossmeisl thank the Center for High Entropy Alloy (CHEAC) funded by the Danish National Research Foundation (DNRF 149) and the Villum Foundation through the Villum Center for the Science of Sustainable Fuels and Chemicals (#9444) for funding this work.

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Authors and Affiliations

  1. McKetta Department of Chemical Engineering, University of Texas at Austin, Austin, TX, USA

    Jon-Marc McGregor, Jay T. Bender, Louise Cañada, Joan F. Brennecke & Joaquin Resasco

  2. Department of Chemistry, University of Copenhagen, Copenhagen, Denmark

    Amanda S. Petersen & Jan Rossmeisl

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  1. Jon-Marc McGregor
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  2. Jay T. Bender
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Contributions

J.M. conducted all electrochemical experiments and wrote the paper. J.T.B. collected all the vibrational spectroscopy data. A.S.P. performed all the computational calculations and J. Rossmeisl guided the computational efforts. L.C. synthesized and characterized the asymmetric quaternary cations. J. Resasco conceptualized the paper. J.F.B and J. Resasco guided the work. All authors contributed to the discussion, review and editing of the paper.

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Correspondence to Joaquin Resasco.

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McGregor, JM., Bender, J.T., Petersen, A.S. et al. Organic electrolyte cations promote non-aqueous CO2 reduction by mediating interfacial electric fields. Nat Catal 8, 79–91 (2025). https://doi.org/10.1038/s41929-024-01278-2

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