Reaction mechanism for oxygen evolution on RuO2, IrO2, and RuO2@IrO2 core-shell nanocatalysts

Ma, Zhong; Zhang, Yu; Liu, Shizhong; Xu, Wenqian; Wu, Lijun; Hsieh, Yu-Chi; Liu, Ping; Zhu, Yimei; Sasaki, Kotaro; Renner, Julie N.; Ayers, Katherine E.; Adzic, Radoslav R.; Wang, Jia X.

doi:10.1016/j.jelechem.2017.10.062

Title: Reaction mechanism for oxygen evolution on RuO₂, IrO₂, and RuO₂@IrO₂ core-shell nanocatalysts

Journal Article · Sat Oct 28 00:00:00 EDT 2017 · Journal of Electroanalytical Chemistry

DOI:https://doi.org/10.1016/j.jelechem.2017.10.062· OSTI ID:1425009

^[1];

^[1]; Liu, Shizhong ^[1]; Xu, Wenqian ^[2]; Wu, Lijun ^[1]; Hsieh, Yu-Chi ^[1]; Liu, Ping ^[1]; Zhu, Yimei ^[1]; Sasaki, Kotaro ^[1]; Renner, Julie N. ^[3]; Ayers, Katherine E. ^[3]; Adzic, Radoslav R. ^[1];

^[1]

Brookhaven National Lab. (BNL), Upton, NY (United States). Chemistry Division
Argonne National Lab. (ANL), Argonne, IL (United States). X-ray Science Division
Proton OnSite, Wallingford, CT (United States)

Iridium dioxide, IrO2, is second to the most active RuO2 catalyst for the oxygen evolution reaction (OER) in acid, and is used in proton exchange membrane water electrolyzers due to its high durability. To improve the activity of IrO2-based catalysts, we prepared RuO2@IrO2 core-shell nanocatalysts using carbon-supported Ru as the template. At 1.48 V, the OER specific activity of RuO2@IrO2 is threefold that of IrO2. While the activity volcano plots over wide range materials have been reported, zooming into the top region to clarify the rate limiting steps of currently most active catalysts is important for further developing advanced OER catalysts. Here, we verified theory-proposed sequential water dissociation pathway in which the O-O bond forms on a single metal site, not via coupling of two adsorbed intermediates, by fitting measured polarization curves using a kinetic equation with the free energies of adsorption and activation as the parameters. Consistent with theoretical calculations, we show that the OER activities of IrO2 and RuO2@IrO2 are limited by the formation of O adsorbed phase, while the OOH formation on the adsorbed O limits the reaction rate on RuO2.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States); Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE); National Natural Science Foundation of China (NNSF); Major Basic Research Program of China; National Natural Science Foundation of China (NSFC); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division

Grant/Contract Number:: SC0012704; FG02-12ER86531; AC02-06CH11357; 21336003; 2014CB239703

OSTI ID:: 1425009

Alternate ID(s):: OSTI ID: 1460967; OSTI ID: 1549442

Report Number(s):: BNL-114508-2017-JAAM

Journal Information:: Journal of Electroanalytical Chemistry, Vol. 819, Issue C; ISSN 1572-6657

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 89 works

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37 INORGANIC
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Title: Reaction mechanism for oxygen evolution on RuO2, IrO2, and RuO2@IrO2 core-shell nanocatalysts

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Title: Reaction mechanism for oxygen evolution on RuO₂, IrO₂, and RuO₂@IrO₂ core-shell nanocatalysts