TY - JOUR
T1 - The Implications of Coupling an Electron Transfer Mediated Oxidation with a Proton Coupled Electron Transfer Reduction in Hybrid Water Electrolysis
AU - Mondal, Biswajit
AU - Dinda, Soumitra
AU - Karjule, Neeta
AU - Mondal, Sanjit
AU - Raja Kottaichamy, Alagar
AU - Volokh, Michael
AU - Shalom, Menny
N1 - Funding Information:
This research was partially funded through the Planning & Budgeting Committee/Israel Council for Higher Education (CHE) and Fuel Choice Initiative (Prime Minister Office of Israel), within the framework of “Israel National Research Center for Electrochemical Propulsion” (INREP). BM acknowledges the Planning and Budgeting Committee (PBC) of the Council for Higher Education of Israel for a fellowship. BM and SD acknowledge IIT Gandhinagar internal grant for funding and fellowship, respectively. We thank Prof. Idan Hod for fruitful discussion.
Publisher Copyright:
© 2022 The Authors. ChemSusChem published by Wiley-VCH GmbH.
PY - 2022/1/1
Y1 - 2022/1/1
N2 - 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.
AB - 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.
KW - benzylamine oxidation
KW - electrocatalysis
KW - hydrogen evolution reaction
KW - proton-coupled electron transfer
KW - single-electron transfer
UR - http://www.scopus.com/inward/record.url?scp=85147097027&partnerID=8YFLogxK
U2 - 10.1002/cssc.202202271
DO - 10.1002/cssc.202202271
M3 - Article
C2 - 36576299
AN - SCOPUS:85147097027
SN - 1864-5631
JO - ChemSusChem
JF - ChemSusChem
ER -
