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Operando Evidence for a Universal Oxygen Evolution Mechanism on Thermal and Electrochemical Iridium Oxides

Saveleva, Viktoriia A. and Wang, Li and Teschner, Detre and Jones, Travis and Gago, Aldo and Friedrich, K. Andreas and Zafeiratos, Spyridon and Schlögl, Robert and Savinova, Elena R. (2018) Operando Evidence for a Universal Oxygen Evolution Mechanism on Thermal and Electrochemical Iridium Oxides. Journal of Physical Chemistry Letters, 9 (11), pp. 3154-3160. ACS Publications. DOI: 10.1021/acs.jpclett.8b00810 ISSN 1948-7185

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Official URL: https://pubs.acs.org/doi/abs/10.1021/acs.jpclett.8b00810

Abstract

Progress in the development of the proton exchange membrane (PEM) water electrolysis technology requires decreasing the anode overpotential, where the sluggish multistep oxygen evolution reaction (OER) occurs. This calls for the understanding of the nature of the active OER sites and reaction intermediates, which are still being debated. In this work, we apply synchrotron radiation-based near ambient pressure X-ray photoelectron and absorption spectroscopies under operando conditions in order to unveil the nature of the reaction intermediates and shed light on the OER mechanism on electrocatalysts most widely used in PEM electrolyzers-electrochemical and thermal iridium oxides. The analysis of the O K-edge and Ir4f spectra backed by density functional calculations reveals a universal oxygen anion red-ox mechanism regardless of the nature (electrochemical or thermal) of the iridium oxide. The formation of molecular oxygen is considered to occur through a chemical step from the electrophilic OI- species, which itself is formed in an electrochemical step.

Item URL in elib:https://elib.dlr.de/122876/
Document Type:Article
Title:Operando Evidence for a Universal Oxygen Evolution Mechanism on Thermal and Electrochemical Iridium Oxides
Authors:
AuthorsInstitution or Email of AuthorsAuthors ORCID iD
Saveleva, Viktoriia A.University of StrasbourgUNSPECIFIED
Wang, Lili.wang (at) dlr.dehttps://orcid.org/0000-0002-4129-7125
Teschner, DetreFHI BerlinUNSPECIFIED
Jones, TravisFHI Berlinhttps://orcid.org/0000-0001-8921-7641
Gago, Aldoaldo.gago (at) dlr.deUNSPECIFIED
Friedrich, K. Andreasandreas.friedrich (at) dlr.dehttps://orcid.org/0000-0002-2968-5029
Zafeiratos, SpyridonUniversity of StarsbourgUNSPECIFIED
Schlögl, RobertFHI BerlinUNSPECIFIED
Savinova, Elena R.University Strasbourghttps://orcid.org/0000-0001-7304-6825
Date:18 May 2018
Journal or Publication Title:Journal of Physical Chemistry Letters
Refereed publication:Yes
Open Access:No
Gold Open Access:No
In SCOPUS:Yes
In ISI Web of Science:Yes
Volume:9
DOI :10.1021/acs.jpclett.8b00810
Page Range:pp. 3154-3160
Editors:
EditorsEmail
Schatz, Georgeeic@jpc.acs.org
Publisher:ACS Publications
ISSN:1948-7185
Status:Published
Keywords:Oxygen evolution reaction (OER), Proton Exchange Membrane (PEM) water electrolysis, Near-Ambient Pressure XPS (NAP-XPS), soft X-ray absorption spectroscopy, O K-edge, active sites
HGF - Research field:Energy
HGF - Program:Storage and Cross-linked Infrastructures
HGF - Program Themes:Electrolysis and Hydrogen
DLR - Research area:Energy
DLR - Program:E SP - Energy Storage
DLR - Research theme (Project):E - Elektrochemical Processes (Electrolysis)
Location: Stuttgart
Institutes and Institutions:Institute of Engineering Thermodynamics > Electrochemical Energy Technology
Deposited By: Wang, Li
Deposited On:19 Dec 2018 16:59
Last Modified:19 Dec 2018 16:59

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