How Metal Nuclearity Impacts Electrocatalytic H2 Production in Thiocarbohydrazone-based Complexes - Archive ouverte HAL Accéder directement au contenu
Article Dans Une Revue Inorganics Année : 2023

How Metal Nuclearity Impacts Electrocatalytic H2 Production in Thiocarbohydrazone-based Complexes

Résumé

Thiocarbohydrazone-based catalysts feature ligands that are potentially electrochemically active. From the synthesis point of view, these ligands can be easily tailored, opening multiple strategies for optimization, such as using different substituent groups or metal substitution. In this work, we show the possibility of a new strategy, involving nuclearity of the system, meaning different number of metal centers. We report the synthesis and characterization of a trinuclear nickel-thiocarbohydrazone complex displaying an improved turnover rate compared to its mononuclear counterpart. We use DFT calculations to show that the mechanism involved is metal-centered, unlike the metal-assisted ligand-centered mechanism found in the mononuclear complex. Finally, we show that two possible mechanisms can be assigned to this catalyst, all involving an initial double reduction of the system.
Fichier principal
Vignette du fichier
Inorganics-Ni3L-ms_revised.pdf (1.37 Mo) Télécharger le fichier
Origine : Fichiers produits par l'(les) auteur(s)

Dates et versions

hal-04061771 , version 1 (07-04-2023)

Identifiants

Citer

Michael Papadakis, Alexandre Barrozo, Léa Delmotte, Tatiana Straistari, Sergiu Shova, et al.. How Metal Nuclearity Impacts Electrocatalytic H2 Production in Thiocarbohydrazone-based Complexes. Inorganics, 2023, 11 (4), pp.149. ⟨10.3390/inorganics11040149⟩. ⟨hal-04061771⟩
11 Consultations
21 Téléchargements

Altmetric

Partager

Gmail Facebook X LinkedIn More