Hydrogen Evolution Mediated by Cobalt Diimine-Dioxime Complexes: Insights into the Role of the Ligand Acid/Base Functionalities.

Dongyue Sun, Aparna Karippara Harshan, Jacques Pécaut, Sharon Hammes-Schiffer, Cyrille Costentin, Vincent Artero

Research output: Contribution to journalArticlepeer-review

10 Scopus citations

Abstract

The benchmarking of the performance for H2 evolution of cobalt diimine-dioxime catalysts is provided based on a comprehensive study of their catalytic mechanism. The latter follows an ECE'CC pathway with intermediate formation of a Co(II)-hydride intermediate and second protonation possibly at a basic site of the ligand, acting as a proton relay. This suggests an intramolecular coupling between the hydride and protonated ligand as the proton concentration-independent rate-determining step controlling the turnover frequency for H2 evolution.

Original languageEnglish (US)
Pages (from-to)2671-2679
Number of pages9
JournalChemElectroChem
Volume8
Issue number14
DOIs
StatePublished - Jul 14 2021
Externally publishedYes

All Science Journal Classification (ASJC) codes

  • Catalysis
  • Electrochemistry

Keywords

  • Cobalt hydride
  • Cyclic Voltammetry
  • Hydrogen
  • Mechanism
  • Molecular Catalysis
  • Proton Relay

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