Electrocatalytic hydrogen evolution from water at low overpotentials with cobalt complexes supported by redox-active bipyridyl-NHC donors
نویسندگان
چکیده
Three cobalt complexes bearing tunable, redox-active bipyridyl N-heterocyclic carbene (NHC)-based ligands have been studied for electrocatalytic hydrogen evolution from aqueous solutions. The effect of structural modifications to the ligand framework is investigated across catalyst series, which includes a non-macrocyclic derivative (1-Co) and 16-(2-Co) 15-(3-Co) membered macrocycles. A structure-activity relationship demonstrated, in macrocyclic greater activity compared their counterpart with most rigid catalyst, supported by 15-membered macrocycle, performing best overall. Indeed, 3-Co catalyzes H2 pH 4 acetate buffer Faradaic efficiency 97% at low overpotential 330 mV. Mechanistic studies are consistent formation cobalt-hydride species that subsequently protonated evolve via heterolytic pathway.
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ژورنال
عنوان ژورنال: Chinese Journal of Catalysis
سال: 2022
ISSN: ['0253-9837', '1872-2067']
DOI: https://doi.org/10.1016/s1872-2067(22)64151-2