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Molecular Inhibition for Selective CO2 Conversion.

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Abstract

Electrochemical CO2 reduction presents a sustainable route to the production of chemicals and fuels. Achieving a narrow product distribution with heterogeneous Cu catalysts is challenging and conventional material modifications offer limited control over selectivity. Here, we show that surface-immobilised molecular species can act as inhibitors for specific carbon products to provide rational control over product distributions. Combined experimental and computational results showed that anchoring of a thiol-functionalised pyridine on Cu destabilises a surface-bound reaction intermediate to energetically block a CO-producing pathway, thereby favouring formate production. The nitrogen atom was shown to be essential to the inhibition mechanism. The ability of molecules to control selectivity through inhibition of specific reaction pathways offers a unique approach to rationally modify heterogeneous catalysts.

Citation

Creissen, C., Rivera de la Cruz, J., Karapinar, D., Taverna, D., Schreiber, M., & Fontecave, M. (2022). Molecular Inhibition for Selective CO2 Conversion. Angewandte Chemie International Edition, e202206279 - ?. https://doi.org/10.1002/anie.202206279

Acceptance Date Jun 9, 2022
Publication Date Aug 8, 2022
Publicly Available Date Aug 9, 2023
Journal Angew Chem Int Ed Engl
Print ISSN 1433-7851
Publisher Wiley
Pages e202206279 - ?
DOI https://doi.org/10.1002/anie.202206279
Publisher URL https://onlinelibrary.wiley.com/doi/10.1002/anie.202206279

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