From Ligand‐ to Metal‐centered Reactivity: Metal Substitution Effect in Thiosemicarbazone‐based Complexes for H 2 Production - Archive ouverte HAL Access content directly
Journal Articles ChemPhysChem Year : 2022

From Ligand‐ to Metal‐centered Reactivity: Metal Substitution Effect in Thiosemicarbazone‐based Complexes for H 2 Production

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Abstract

The quest to develop and optimize catalysts for H2 production requires a thorough understanding in the possible catalytic mechanisms involved. Transition metals are very often the centers of reactivity in the catalysis, although this can change in the presence of a redox-active ligand. Investigating the differences in catalysis when considering ligand-and metal-centered reactivity is important to find the most optimal mechanisms for hydrogen evolution reaction. Here, we investigated this change of reactivity in two versions of a thiosemicarbazone-based complex, using Co and Ni metal centers. While the Ni version has a ligand-centered reactivity, Co switches it toward a metal-centered one. Comparison between the mechanisms show differences in rate-limiting steps, and shows the importance of identifying those steps in order to optimize the system for hydrogen production.
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Dates and versions

hal-03862130 , version 1 (30-11-2022)

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Alexandre Barrozo, Maylis Orio. From Ligand‐ to Metal‐centered Reactivity: Metal Substitution Effect in Thiosemicarbazone‐based Complexes for H 2 Production. ChemPhysChem, 2022, 23 (9), pp.e202200056. ⟨10.1002/cphc.202200056⟩. ⟨hal-03862130⟩
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