Bisulfate as a redox-active ligand in vanadium-based electrocatalysis for CH4functionalization
Journal
Chemical Communications
Journal Volume
58
Journal Issue
15
Pages
2524-2527
Date Issued
2022
Author(s)
Abstract
The roles of unforgiving H2SO4 solvent in CH4 activation with molecular catalysts have not been experimentally well-illustrated despite computational predictions. Here, we provide experimental evidence that metal-bound bisulfate ligand introduced by H2SO4 solvent is redox-active in vanadium-based electrocatalytic CH4 activation discovered recently. Replacing one of the two terminal bisulfate ligands with redox-inert dihydrogen phosphate in the pre-catalyst vanadium (V)-oxo dimer completely quenches its activity towards CH4, which may inspire environmentally benign catalysis with minimal use of H2SO4. This journal is © The Royal Society of Chemistry.
SDGs
Other Subjects
Catalysts; Dimers; Electrocatalysis; Ligands; Redox reactions; Vanadium compounds; CH 4; Computational predictions; Electrocatalytic; Experimental evidence; Functionalizations; Metal bounds; Molecular catalysts; Redox-active; Redox-active ligand; Two terminals; Chemical activation; bisulfate; dihydrogen phosphate; dimer; electrolyte; methane; phosphate; sulfate; unclassified drug; Article; catalysis; chemical composition; chemical interaction; chemical structure; concentration (parameter); electrocatalysis; experimental study; ligand binding; oxidation; oxidation reduction potential; solvent effect; substitution reaction; ultraviolet visible spectroscopy; validation process; X ray absorption spectroscopy
Type
journal article