Pulsed-EPR Evidence of a Manganese(II) Hydroxycarbonyl Intermediate in the Electrocatalytic Reduction of Carbon Dioxide by a Manganese Bipyridyl Derivative
| Autor: | Maylis Orio, Alain Deronzier, Sylvie Chardon-Noblat, Florian Molton, Marc Bourrez, Hervé Vezin, Carole Duboc |
|---|---|
| Přispěvatelé: | Département de Chimie Moléculaire - Chimie Inorganique Redox Biomimétique (DCM - CIRE), Département de Chimie Moléculaire (DCM), Université Joseph Fourier - Grenoble 1 (UJF)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Université Joseph Fourier - Grenoble 1 (UJF)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS), Laboratoire Avancé de Spectroscopie pour les Intéractions la Réactivité et l'Environnement - UMR 8516 (LASIRE), Institut de Chimie du CNRS (INC)-Université de Lille-Centre National de la Recherche Scientifique (CNRS)-Centrale Lille Institut (CLIL), Département de Chimie Moléculaire - Chimie Inorganique Redox (DCM - CIRE), Institut de Chimie du CNRS (INC)-Université de Lille-Centre National de la Recherche Scientifique (CNRS) |
| Rok vydání: | 2013 |
| Předmět: |
Reaction mechanism
Inorganic chemistry chemistry.chemical_element Manganese Electrocatalyst Photochemistry 010402 general chemistry 01 natural sciences Catalysis Adduct chemistry.chemical_compound electrocatalysis 010405 organic chemistry carbon dioxide General Chemistry General Medicine Oxidative addition 0104 chemical sciences [CHIM.THEO]Chemical Sciences/Theoretical and/or physical chemistry chemistry Catalytic cycle 13. Climate action manganese EPR spectroscopy Carbon monoxide |
| Zdroj: | Angewandte Chemie International Edition Angewandte Chemie International Edition, Wiley-VCH Verlag, 2014, 53, pp.240-243. ⟨10.1002/anie.201306750⟩ Angewandte Chemie International Edition, 2014, 53, pp.240-243. ⟨10.1002/anie.201306750⟩ |
| ISSN: | 0044-8249 1433-7851 1521-3773 |
| DOI: | 10.1002/ange.201306750 |
| Popis: | A key intermediate in the electroconversion of carbon dioxide to carbon monoxide, catalyzed by a manganese tris(carbonyl) complex, is characterized. Different catalytic pathways and their potential reaction mechanisms are investigated using a large range of experimental and computational techniques. Sophisticated spectroscopic methods including UV/Vis absorption and pulsed-EPR techniques (2P-ESEEM and HYSCORE) were combined together with DFT calculations to successfully identify a key intermediate in the catalytic cycle of CO2 reduction. The results directly show the formation of a metal-carboxylic acid-CO2 adduct after oxidative addition of CO2 and H+ to a Mn0 carbonyl dimer, an unexpected intermediate. |
| Databáze: | OpenAIRE |
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