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On the role of metal cations in CO2 electrocatalytic reduction

Nature Catalysis volume 5, pages 977–978 (2022)Cite this article

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Matters Arising to this article was published on 28 November 2022

The Original Article was published on 26 July 2021

arising from M. C. O. Monteiro et al. Nature Catalysis https://doi.org/10.1038/s41929-021-00655-5 (2021)

Metal cations are widely considered to influence the electrocatalytic reduction of CO2, however, their roles are still being identified. Recently, Monteiro et al.1 proposed a mechanism in which the main effect of the cations is to stabilize CO2 adsorption on the electrode surface based on evidence from experiments and ab initio molecular dynamics (AIMD) simulations. This Matters Arising points to an essential constraint applied in the AIMD simulations, which calls into question the conclusions that are drawn and suggests the need for unrestricted AIMD simulations for electrocatalytic reactions.

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Fig. 1: AIMD simulations of CO2 desorption from the Au(111) surface.

Data availability

The dataset generated and analysed in the current study are available at https://doi.org/10.5281/zenodo.7122467.

References

  1. Monteiro, M. C. O. et al. Absence of CO2 electroreduction on copper, gold and silver electrodes without metal cations in solution. Nat. Catal. 4, 654–662 (2021).

    Article  CAS  Google Scholar 

  2. Farkas, A. P. & Solymosi, F. Activation and Reactions of CO2 on a K-Promoted Au(111) Surface. J. Phys. Chem. C 113, 19930–19936 (2009).

    Article  CAS  Google Scholar 

  3. Farkas, A. P. & Solymosi, F. Photolysis of the CO2 + K/Au(111) System. J. Phys. Chem. C 114, 16979–16982 (2010).

    Article  CAS  Google Scholar 

  4. Dattila, F. Cation-effect-CO2-reduction. ioChem-BD https://doi.org/10.19061/iochem-bd-1-194 (2021).

  5. Marcandalli, G., Villalba, M. & Koper, M. T. M. The importance of acid–base equilibria in bicarbonate electrolytes for CO2 electrochemical reduction and CO reoxidation studied on Au(hkl) electrodes. Langmuir 37, 5707–5716 (2021).

    Article  CAS  PubMed  PubMed Central  Google Scholar 

  6. Qin, X., Vegge, T. & Hansen, H. A. CO2 activation at Au(110)–water interfaces: An ab initio molecular dynamics study. J. Chem. Phys. 155, 134703 (2021).

    Article  CAS  PubMed  Google Scholar 

  7. Sundararaman, R., Goddard, W. A. & Arias, T. A. Grand canonical electronic density-functional theory: Algorithms and applications to electrochemistry. J. Chem. Phys. 146, 114104 (2017).

    Article  PubMed  Google Scholar 

  8. Sundararaman, R. & Arias, T. A. In Atomic‐Scale Modelling of Electrochemical Systems (eds M. M. Melander et al.) 139–172 (John Wiley & Sons, 2021).

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Acknowledgements

This work is supported in part by National Science Foundation under grant CHE1955343 and UCF Trustee Chair Professorship. Simulations were performed using the computing resources at the Advanced Research Computing Center at University of Central Florida and the National Energy Research Scientific Computing Center.

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Authors and Affiliations

  1. Department of Physics, University of Central Florida, Orlando, FL, USA

    Duy Le & Talat S. Rahman

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  1. Duy Le
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  2. Talat S. Rahman
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Contributions

D.L. carried out the simulations. D.L. and T.S.R. wrote and edited the manuscript.

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Correspondence to Duy Le.

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Nature Catalysis thanks Hyungjun Kim for their contribution to the peer review of this work.

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Extended data

Supplementary information

Supplementary Information

Supplementary methods and references.

Supplementary Video 1

AIMD simulation of Au-H2O-CO2 system.

Supplementary Video 2

AIMD simulation of Au-H2O-K+-CO2 system.

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Le, D., Rahman, T.S. On the role of metal cations in CO2 electrocatalytic reduction. Nat Catal 5, 977–978 (2022). https://doi.org/10.1038/s41929-022-00876-2

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