The Implications of Coupling an Electron Transfer Mediated Oxidation with a Proton Coupled Electron Transfer Reduction in Hybrid Water Electrolysis

Biswajit Mondal, Soumitra Dinda, Neeta Karjule, Sanjit Mondal, Alagar Raja Kottaichamy, Michael Volokh, Menny Shalom

Research output: Contribution to journalArticlepeer-review

3 Scopus citations

Abstract

Electrolysis of water is a sustainable route to produce clean hydrogen. Full water-splitting requires a high applied potential, in part because of the pH-dependency of the H2 and O2 evolution reactions (HER and OER), which are proton-coupled electron transfer (PCET) reactions. Therefore, the minimum required potential will not change at different pHs. TEMPO [(2,2,6,6-tetramethyl-1-piperidin-1-yl)oxyl], a stable free-radical that undergoes fast electro-oxidation by a single-electron transfer (ET) process, is pH-independent. Here, we show that the combination of PCET and ET processes enables hydrogen production from water at low cell potentials below the theoretical value for full water-splitting by simple pH adjustment. As a case study, we combined the HER with the oxidation of benzylamine by anodically oxidized TEMPO. The pH-independent electrocatalytic oxidation of TEMPO permits the operation of a hybrid water-splitting cell that shows promise to perform at a low cell potential (≈1 V) and neutral pH conditions.

Original languageEnglish
Article numbere202202271
JournalChemSusChem
Volume16
Issue number10
DOIs
StatePublished - 19 May 2023

Keywords

  • benzylamine oxidation
  • electrocatalysis
  • hydrogen evolution reaction
  • proton-coupled electron transfer
  • single-electron transfer

ASJC Scopus subject areas

  • General Energy
  • General Chemical Engineering
  • General Materials Science
  • Environmental Chemistry

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