Hydrogen Evolution Electrocatalysis with a Molecular Cobalt Bis(alkylimidazole)methane Complex in DMF: a Critical Activity Analysis.

Autor: de Vos SD; Organic Chemistry and Catalysis, Institute for Sustainable and Circular Chemistry, Utrecht University, Universiteitsweg 99, 3584 CG, Utrecht (The, Netherlands., Otten M; Organic Chemistry and Catalysis, Institute for Sustainable and Circular Chemistry, Utrecht University, Universiteitsweg 99, 3584 CG, Utrecht (The, Netherlands., Wissink T; Chemical Engineering and Chemistry, Laboratory of Inorganic Materials and Catalysis, Department of Chemical Engineering and Chemistry, Eindhoven University of Technology, P.O. Box 513, 5600 MB, Eindhoven (The, Netherlands., Broere DLJ; Organic Chemistry and Catalysis, Institute for Sustainable and Circular Chemistry, Utrecht University, Universiteitsweg 99, 3584 CG, Utrecht (The, Netherlands., Hensen EJM; Chemical Engineering and Chemistry, Laboratory of Inorganic Materials and Catalysis, Department of Chemical Engineering and Chemistry, Eindhoven University of Technology, P.O. Box 513, 5600 MB, Eindhoven (The, Netherlands., Klein Gebbink RJM; Organic Chemistry and Catalysis, Institute for Sustainable and Circular Chemistry, Utrecht University, Universiteitsweg 99, 3584 CG, Utrecht (The, Netherlands.
Jazyk: angličtina
Zdroj: ChemSusChem [ChemSusChem] 2022 Nov 22; Vol. 15 (22), pp. e202201308. Date of Electronic Publication: 2022 Oct 26.
DOI: 10.1002/cssc.202201308
Abstrakt: [Co(HBMIM Ph2 ) 2 ](BF 4 ) 2 (1) [HBMIM Ph2 =bis(1-methyl-4,5-diphenyl-1H-imidazol-2-yl)methane] was investigated for its electrocatalytic hydrogen evolution performance in DMF using voltammetry and during controlled potential/current electrolysis (CPE/CCE) in a novel in-line product detection setup. Performances were benchmarked against three reported molecular cobalt hydrogen evolution reaction (HER) electrocatalysts, [Co(dmgBF 2 ) 2 (solv) 2 ] (2) (dmgBF 2 =difluoroboryldimethylglyoximato), [Co(TPP)] (3) (TPP=5,10,15,20-tetraphenylporphyrinato), and [Co(bapbpy)Cl](Cl) (4) [bapbpy=6,6'-bis-(2-aminopyridyl)-2,2'-bipyridine], showing distinct performances differences with 1 being the runner up in H 2 evolution during CPE and the best catalyst in terms of overpotential and Faradaic efficiency during CCE. After bulk electrolysis, for all of the complexes, a deposit on the glassy carbon electrode was observed, and post-electrolysis X-ray photoelectron spectroscopy (XPS) analysis of the deposit formed from 1 demonstrated only a minor cobalt contribution (0.23 %), mainly consisting of Co 2+ . Rinse tests on the deposits derived from 1 and 2 showed that the initially observed distinct activity was (partly) preserved for the deposits. These observations indicate that the molecular design of the complexes dictates the features of the formed deposit and therewith the observed activity.
(© 2022 The Authors. ChemSusChem published by Wiley-VCH GmbH.)
Databáze: MEDLINE
Externí odkaz: