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Reply to: On the role of metal cations in CO2 electrocatalytic reduction

Nature Catalysis volume 5, pages 979–981 (2022)Cite this article

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The Original Article was published on 28 November 2022

replying to: D. Le et al. Nature Catalysis https://doi.org/10.1038/s41929-022-00876-2 (2021)

In our recent publication1, we demonstrated the absence of CO2 electroreduction on copper, gold and silver electrodes without alkali metal cations in solution through unequivocal experimental evidence. Additionally, we proposed a mechanism for CO2 electroreduction in which the metal cation is key to stabilizing CO2 adsorption, thus enabling its activation and reduction. This last finding is supported by ab initio molecular dynamics (AIMD) simulations on Au/solvent/cation/CO2 supercells. In their Matters Arising2, Le and Rahman point out a constraint included in our computational setup, suggesting that it may affect our main conclusions. We here confirm that, although our computational framework was minimal, it is robust enough to support the proposed mechanism and thus our main conclusions.

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Fig. 1: CO2 activation with and without alkali cations and excess electrons.

Data availability

Computational details are available in the Supplementary Information. The new datasets generated through DFT simulations and analysed during the current study are available in the ioChem-BD database3 at https://doi.org/10.19061/iochem-bd-1-2437.

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Acknowledgements

This work was supported by the European Commission (Innovative Training Network ELCoREL, 722614-ELCOREL). F.D. and N.L. further acknowledge the Barcelona Supercomputing Center (BSC-RES) for providing generous computational resources.

Author information

Author notes

  1. Mariana C. O. Monteiro

    Present address: Fritz Haber Institute of the Max Planck Society, Berlin, Germany

Authors and Affiliations

  1. Department of Applied Science and Technology, Politecnico di Torino, Turin, Italy

    Federico Dattila

  2. Leiden Institute of Chemistry, Leiden University, Leiden, The Netherlands

    Mariana C. O. Monteiro & Marc T. M. Koper

  3. Institute of Chemical Research of Catalonia, The Barcelona Institute of Science and Technology, Tarragona, Spain

    Núria López

Authors
  1. Federico Dattila
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  2. Mariana C. O. Monteiro
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  3. Marc T. M. Koper
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  4. Núria López
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Contributions

F.D. and N.L. wrote the manuscript with input from all the authors. F.D. and N.L. designed the density functional theory simulations, which were carried out by F.D. All the authors contributed to the definition of the modeling framework, read and commented on the manuscript.

Corresponding authors

Correspondence to Marc T. M. Koper or Núria López.

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The authors declare no competing interests.

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

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Supplementary information

Supplementary Information

Supplementary equation 1 and Methods.

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Dattila, F., Monteiro, M.C.O., Koper, M.T.M. et al. Reply to: On the role of metal cations in CO2 electrocatalytic reduction. Nat Catal 5, 979–981 (2022). https://doi.org/10.1038/s41929-022-00877-1

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