Issue 31, 2018

Reactant or reagent? Oxidation of H2 at electronically distinct nickel-thiolate sites [Ni2(μ-SR)2]+ and [Ni–SR]+

Abstract

The chemical bond between a Lewis-acidic metal and a Brønsted/Lewis-basic sulphur donor provides M–S structures with functional properties that are relevant for a variety of processes such as the heterolytic cleavage of H2. Direct comparison of reactivity properties between molecular M–S structures can be difficult owing to divergent electronic properties of stabilizing ligand scaffolds. This work reports on a mechanistic study of stoichiometric H2 oxidation at electronically distinct [Ni2(μ-SR)2]+ and [Ni–SR]+ structures that derive from the same 1,4-terphenyldithiophenol ligand. In this context, the effect of metal containing side-products such as [HNi(PMe3)4]+ on overall H2 oxidation reactivity displayed by Ni–S structures has been investigated quantitatively in addition to external parameters such as solvent and H2 pressure.

Graphical abstract: Reactant or reagent? Oxidation of H2 at electronically distinct nickel-thiolate sites [Ni2(μ-SR)2]+ and [Ni–SR]+

Supplementary files

Article information

Article type
Paper
Submitted
22 jan 2018
Accepted
19 feb 2018
First published
19 feb 2018

Dalton Trans., 2018,47, 10561-10568

Reactant or reagent? Oxidation of H2 at electronically distinct nickel-thiolate sites [Ni2(μ-SR)2]+ and [Ni–SR]+

F. Koch and A. Berkefeld, Dalton Trans., 2018, 47, 10561 DOI: 10.1039/C8DT00275D

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