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Electrocatalytic reduction of protons to dihydrogen by the cobalt tetraazamacrocyclic complex [Co(N4H)Cl-2](+): mechanism and benchmarking of performances

Abstract : The cobalt tetraazamacrocyclic [Co(N4H)Cl-2](+) complex is becoming a popular and versatile catalyst for the electrocatalytic evolution of hydrogen, because of its stability and superior activity in aqueous conditions. We present here a benchmarking of its performances based on the thorough analysis of cyclic voltammograms recorded under various catalytic regimes in non-aqueous conditions allowing control of the proton concentration. This allowed a detailed mechanism to be proposed with quantitative determination of the rate-constants for the various protonation steps, as well as identification of the amine function of the tetraazamacrocyclic ligand to act as a proton relay during H-2 evolution.
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https://hal.archives-ouvertes.fr/hal-03489374
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Submitted on : Friday, December 17, 2021 - 4:50:35 PM
Last modification on : Sunday, June 26, 2022 - 3:26:39 AM

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Cheng-Bo Li, Andrew J. Bagnall, Dongyue Sun, Julia Rendon, Matthieu Koepf, et al.. Electrocatalytic reduction of protons to dihydrogen by the cobalt tetraazamacrocyclic complex [Co(N4H)Cl-2](+): mechanism and benchmarking of performances. Sustainable Energy & Fuels, Royal Society of Chemistry, 2022, 6 (1), pp.143-149. ⟨10.1039/d1se01267c⟩. ⟨hal-03489374⟩

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