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Electrochemically Driven Reduction of Carbon Dioxide Mediated by Mono‐Reduced Mo‐Diimine Tetracarbonyl Complexes: Electrochemical, Spectroelectrochemical and Theoretical Studies
Author(s) -
Garcia Bellido Carlos,
ÁlvarezMiguel Lucía,
Miguel Daniel,
Lalaoui Noémie,
Cabon Nolwenn,
Gloaguen Frédéric,
Le Poul Nicolas
Publication year - 2021
Publication title -
chemelectrochem
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 1.182
H-Index - 59
ISSN - 2196-0216
DOI - 10.1002/celc.202100359
Subject(s) - diimine , electrochemistry , chemistry , ligand (biochemistry) , photochemistry , electrochemical reduction of carbon dioxide , electron transfer , carbon dioxide , redox , bipyridine , inorganic chemistry , electrode , catalysis , organic chemistry , carbon monoxide , crystal structure , biochemistry , receptor
The activation of carbon dioxide by three different Mo‐diimine complexes [Mo(CO) 4 (L)] (L=bipyridine (bpy), 1,10‐phenantroline (phen) or pyridylindolizine (py‐indz)) has been investigated by electrochemistry and spectroelectrochemistry. Under an inert atmosphere, monoreduction of the complexes is ligand‐centered and leads to tetracarbonyl [Mo(CO) 4 (L)] .− species, whereas double reduction induces CO release. Under CO 2 , [Mo(CO) 4 (L)] complexes undergo unexpected coupled chemical‐electrochemical reactions at the first reduction step, leading to the formation of reduced CO 2 derivatives. The experimental results obtained from IR, NIR and UV‐Vis spectroelectrochemistry, as well as DFT calculations, demonstrate an electron‐transfer reaction whose rate is ligand‐dependent.