In situ observation of reactive oxygen species forming on oxygen-evolving iridium surfaces

Chemical Science
V PfeiferRobert Schlögl

Abstract

Water splitting performed in acidic media relies on the exceptional performance of iridium-based materials to catalyze the oxygen evolution reaction (OER). In the present work, we use in situ X-ray photoemission and absorption spectroscopy to resolve the long-standing debate about surface species present in iridium-based catalysts during the OER. We find that the surface of an initially metallic iridium model electrode converts into a mixed-valent, conductive iridium oxide matrix during the OER, which contains OII- and electrophilic OI- species. We observe a positive correlation between the OI- concentration and the evolved oxygen, suggesting that these electrophilic oxygen sites may be involved in catalyzing the OER. We can understand this observation by analogy with photosystem II; their electrophilicity renders the OI- species active in O-O bond formation, i.e. the likely potential- and rate-determining step of the OER. The ability of amorphous iridium oxyhydroxides to easily host such reactive, electrophilic species can explain their superior performance when compared to plain iridium metal or crystalline rutile-type IrO2.

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Citations

May 11, 2019·Physical Chemistry Chemical Physics : PCCP·Martin DillaRobert Schlögl
Nov 26, 2019·Advanced Materials·Douglas R MacFarlaneAlexandr N Simonov
Mar 5, 2020·Dalton Transactions : an International Journal of Inorganic Chemistry· AnamikaNanhai Singh
Apr 21, 2020·Chemical Society Reviews·Leigang LiXiaoqing Huang
May 6, 2020·Physical Chemistry Chemical Physics : PCCP·Francesco Nattino, Nicola Marzari
Jul 8, 2020·Advanced Materials·Taehyun KwonKwangyeol Lee
Jul 16, 2020·Advanced Materials·Hui ChenXiaoxin Zou
Jul 1, 2017·Chemical Communications : Chem Comm·D J AschaffenburgT Cuk
Mar 17, 2019·Optics Express·Ronglei FanMingrong Shen
Aug 28, 2020·Chemistry : a European Journal·Payam Salimi, Mohammad Mahdi Najafpour
Nov 20, 2020·Nature·Hong Nhan NongTravis E Jones
Jun 26, 2021·Nature Communications·Marine ElmaaloufJennifer Peron
Jul 24, 2021·Accounts of Chemical Research·Gang WanDillon D Fong
Aug 7, 2021·Journal of the American Chemical Society·Juan-Jesús Velasco-VélezTravis E Jones
Jan 3, 2020·ACS Applied Materials & Interfaces·Qi FengHaijiang Wang
Oct 28, 2020·ACS Applied Materials & Interfaces·Evgeniya KovalskaZdenek Sofer
Apr 2, 2019·Journal of the American Chemical Society·Rik MomRobert Schlögl
Apr 11, 2020·Chemical Reviews·Federica FratiFrank M F de Groot
Apr 18, 2020·The Journal of Physical Chemistry Letters·Zbynek NovotnyJürg Osterwalder
Jan 24, 2019·Journal of the American Chemical Society·Jiajian GaoBin Liu
May 19, 2018·The Journal of Physical Chemistry Letters·Viktoriia A SavelevaElena R Savinova
Aug 11, 2017·Journal of the American Chemical Society·Elena WillingerMarc Georg Willinger

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Methods Mentioned

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X-ray
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