Proceedings of MATSUS23 & Sustainable Technology Forum València (STECH23) (MATSUS23)
DOI: https://doi.org/10.29363/nanoge.matsus.2023.307
Publication date: 22nd December 2022
Enzymatic systems have evolved complex strategies to maximize the efficiency and product selectivity in small molecule activation, among which CO2 reduction. Beside unique active sites containing by definition earth-abundant elements, enzyme further control catalytic activity through second sphere interactions and a fine control of electron transfer chains. In this talk, we will introduce a series of bio-inspired strategies for the design of electrocatalytic systems for CO2 reduction. We will highlight a series of earth-abundant metal based molecular catalysts inspired by the active sites of enzymatic systems and will introduce a new strategy for the electrocatalytic metal hydride generation using synthetic Fe4S4 clusters acting as concerted proton electron transfer (CPET) mediators. We will demonstrate that the combination of synthetic Fe4S4 clusters with the CO2 electroreduction catalyst [MnI(bpy)(CO)3Br] (bpy = 2,2’-bipyridine) allows the preparation of a benchmark catalytic system for HCOOH generation. We will finally introduce the preparation of the first complete redox series of Fe4S4 complexes and their use to generate potent strong reducing agents via entatic activation strategies. References: 4. L. Grunwald, M. Clémancey, D. Klose, L. Dubois, S. Gambarelli, G. Jeschke, M. Wörle, G. Blondin, V. Mougel* A complete biomimetic iron-sulfur cubane redox series PNAS, 2022, 119 (31), e2122677119 3. S. Dey, F. Masero, E. Brack, M. Fontecave, V. Mougel* Electrocatalytic metal hydride generation using CPET mediators Nature, 2022, 607 (7919), 499-506 2. S. Dey, T. Todorova, M. Fontecave*, V. Mougel* Electroreduction of CO2 to Formate with low overpotential using Cobalt Pyridine Thiolate Complexes Angew. Chem. Int. Ed., 2020, 59(36), 15726-15733 1. A. Mouchfiq, T. Todorova, S. Dey , M. Fontecave*, V. Mougel* A Bioinspired Molybdenum-Copper Molecular Catalyst for CO2 Electroreduction Chem. Sci., 2020, 11, 5503-5510
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