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

[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 setu...

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Autores principales: de Vos, Sander D., Otten, Maartje, Wissink, Tim, Broere, Daniël L. J., Hensen, Emiel J. M., Klein Gebbink, Robertus J. M.
Formato: Online Artículo Texto
Lenguaje:English
Publicado: John Wiley and Sons Inc. 2022
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9828534/
https://www.ncbi.nlm.nih.gov/pubmed/36111965
http://dx.doi.org/10.1002/cssc.202201308
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author de Vos, Sander D.
Otten, Maartje
Wissink, Tim
Broere, Daniël L. J.
Hensen, Emiel J. M.
Klein Gebbink, Robertus J. M.
author_facet de Vos, Sander D.
Otten, Maartje
Wissink, Tim
Broere, Daniël L. J.
Hensen, Emiel J. M.
Klein Gebbink, Robertus J. M.
author_sort de Vos, Sander D.
collection PubMed
description [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.
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spelling pubmed-98285342023-01-10 Hydrogen Evolution Electrocatalysis with a Molecular Cobalt Bis(alkylimidazole)methane Complex in DMF: a Critical Activity Analysis de Vos, Sander D. Otten, Maartje Wissink, Tim Broere, Daniël L. J. Hensen, Emiel J. M. Klein Gebbink, Robertus J. M. ChemSusChem Research Articles [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. John Wiley and Sons Inc. 2022-10-26 2022-11-22 /pmc/articles/PMC9828534/ /pubmed/36111965 http://dx.doi.org/10.1002/cssc.202201308 Text en © 2022 The Authors. ChemSusChem published by Wiley-VCH GmbH https://creativecommons.org/licenses/by/4.0/This is an open access article under the terms of the http://creativecommons.org/licenses/by/4.0/ (https://creativecommons.org/licenses/by/4.0/) License, which permits use, distribution and reproduction in any medium, provided the original work is properly cited.
spellingShingle Research Articles
de Vos, Sander D.
Otten, Maartje
Wissink, Tim
Broere, Daniël L. J.
Hensen, Emiel J. M.
Klein Gebbink, Robertus J. M.
Hydrogen Evolution Electrocatalysis with a Molecular Cobalt Bis(alkylimidazole)methane Complex in DMF: a Critical Activity Analysis
title Hydrogen Evolution Electrocatalysis with a Molecular Cobalt Bis(alkylimidazole)methane Complex in DMF: a Critical Activity Analysis
title_full Hydrogen Evolution Electrocatalysis with a Molecular Cobalt Bis(alkylimidazole)methane Complex in DMF: a Critical Activity Analysis
title_fullStr Hydrogen Evolution Electrocatalysis with a Molecular Cobalt Bis(alkylimidazole)methane Complex in DMF: a Critical Activity Analysis
title_full_unstemmed Hydrogen Evolution Electrocatalysis with a Molecular Cobalt Bis(alkylimidazole)methane Complex in DMF: a Critical Activity Analysis
title_short Hydrogen Evolution Electrocatalysis with a Molecular Cobalt Bis(alkylimidazole)methane Complex in DMF: a Critical Activity Analysis
title_sort hydrogen evolution electrocatalysis with a molecular cobalt bis(alkylimidazole)methane complex in dmf: a critical activity analysis
topic Research Articles
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9828534/
https://www.ncbi.nlm.nih.gov/pubmed/36111965
http://dx.doi.org/10.1002/cssc.202201308
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