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Article Dans Une Revue Angewandte Chemie International Edition Année : 2022

Molecular Inhibition for Selective CO 2 Conversion

Résumé

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 1 distributions. Combined experimental and computational results showed that anchoring of a thiolfunctionalised pyridine on Cu destabilises a surfacebound reaction intermediate to energetically block a COproducing 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.
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Dates et versions

hal-04031205 , version 1 (15-03-2023)

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Charles E Creissen, José Guillermo Rivera de la Cruz, Dilan Karapinar, Dario Taverna, Moritz W Schreiber, et al.. Molecular Inhibition for Selective CO 2 Conversion. Angewandte Chemie International Edition, 2022, 61 (32), ⟨10.1002/anie.202206279⟩. ⟨hal-04031205⟩
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