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

The Journal of Physical Chemistry Letters
V A SavelevaE R Savinova

Abstract

Progress in the development of proton exchange membrane (PEM) water electrolysis technology requires decreasing the anode overpotential, where the sluggish multistep oxygen evolution reaction (OER) occurs. This calls for an 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. Analysis of the O K-edge and Ir 4f 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.

References

Sep 30, 2009·Journal of Physics. Condensed Matter : an Institute of Physics Journal·Paolo GiannozziRenata M Wentzcovitch
Jun 4, 2014·Angewandte Chemie·Hernan G Sanchez CasalongueAnders Nilsson
Aug 19, 2015·The Journal of Physical Chemistry Letters·Nemanja DanilovicNenad M Markovic
Aug 2, 2016·The Journal of Physical Chemistry Letters·Viktoriia A SavelevaElena R Savinova
Jan 4, 2017·Chemical Science·Verena PfeiferRobert Schlögl
Feb 1, 2017·The Journal of Physical Chemistry. C, Nanomaterials and Interfaces·C J PowellD G Castner
May 17, 2017·Chemical Science·Verena PfeiferRobert Schlögl

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Citations

Jun 5, 2019·Molecules : a Journal of Synthetic Chemistry and Natural Product Chemistry·Aikaterini TouniSotirios Sotiropoulos
Jan 3, 2020·Chemical Communications : Chem Comm·Khezar H SaeedAlexander J Cowan
May 6, 2020·Physical Chemistry Chemical Physics : PCCP·Francesco Nattino, Nicola Marzari
Apr 29, 2021·Physical Chemistry Chemical Physics : PCCP·Evgeniia S VikulovaKseniya V Zherikova
Jun 26, 2021·Nature Communications·Marine ElmaaloufJennifer Peron
Jun 3, 2019·Nano-micro Letters·Maoyu WangZhenxing Feng
Aug 7, 2021·Journal of the American Chemical Society·Juan-Jesús Velasco-VélezTravis E Jones
Apr 11, 2020·Chemical Reviews·Federica FratiFrank M F de Groot
Apr 18, 2020·The Journal of Physical Chemistry Letters·Zbynek NovotnyJürg Osterwalder
Mar 20, 2020·The Journal of Physical Chemistry Letters·Alexandra Zagalskaya, Vitaly Alexandrov

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