Dr Charles Creissen c.e.creissen@keele.ac.uk
Molecular Inhibition for Selective CO 2 Conversion
Creissen, Charles E.; Rivera de la Cruz, José Guillermo; Karapinar, Dilan; Taverna, Dario; Schreiber, Moritz W.; Fontecave, Marc
Authors
José Guillermo Rivera de la Cruz
Dilan Karapinar
Dario Taverna
Moritz W. Schreiber
Marc Fontecave
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. E., Rivera de la Cruz, J. G., Karapinar, D., Taverna, D., Schreiber, M. W., & Fontecave, M. (2022). Molecular Inhibition for Selective CO 2 Conversion. Angewandte Chemie, 134(32), https://doi.org/10.1002/ange.202206279
Journal Article Type | Article |
---|---|
Acceptance Date | Jun 9, 2022 |
Online Publication Date | Jul 4, 2022 |
Publication Date | Aug 8, 2022 |
Deposit Date | May 30, 2023 |
Journal | Angewandte Chemie |
Print ISSN | 0044-8249 |
Electronic ISSN | 1521-3757 |
Publisher | Wiley |
Peer Reviewed | Peer Reviewed |
Volume | 134 |
Issue | 32 |
DOI | https://doi.org/10.1002/ange.202206279 |
Keywords | General Medicine |
Additional Information | Received: 2022-04-29; Published: 2022-07-04 |
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