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

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. In order 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@IrO₂is threefold that of IrO₂. While the activity volcano plots over wide range of materials have been reported, zooming into the top region to clarify the rate limiting steps of most active catalysts is important for further activity enhancement. 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.

View Accepted Manuscript (DOE)

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

Sponsoring Organization:: Major Basic Research Program of China; National Natural Science Foundation of China; National Natural Science Foundation of China (NNSF); USDOE Office of Energy Efficiency and Renewable Energy (EERE); USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Scientific User Facilities Division

Grant/Contract Number:: AC02-06CH11357; SC0012704

OSTI ID:: 1425009

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

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

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

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Core-shell
Electrolysis
IrO2
Oxygen evolution reaction mechanism
RuO2