Activating Fe(I) Porphyrins for the Hydrogen Evolution Reaction Using Second-Sphere Proton Transfer Residues

Atanu Rana, Biswajit Mondal, Pritha Sen, Subal Dey, Abhishek Dey

Research output: Contribution to journalArticlepeer-review

79 Scopus citations

Abstract

Iron porphyrin complexes with second-sphere distal triazole residues show a hydrogen evolution reaction (HER) catalyzed by the Fe(I) state in both organic and aqueous media, whereas an analogous iron porphyrin complex without the distal residues catalyzes the HER in the formal Fe(0) state. This activation of the Fe(I) state by the second-sphere residues lowers the overpotential of the HER by these iron porphyrin complexes by 50%. Experimental data and theoretical calculations indicate that the distal triazole residues, once protonated, enhance the proton affinity of the iron center via formation of a dihydrogen bond with an Fe(III)-H- intermediate.

Original languageEnglish
Pages (from-to)1783-1793
Number of pages11
JournalInorganic Chemistry
Volume56
Issue number4
DOIs
StatePublished - 20 Feb 2017
Externally publishedYes

ASJC Scopus subject areas

  • Physical and Theoretical Chemistry
  • Inorganic Chemistry

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