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Tuning the Selectivity and Activity of Electrochemical Interfaces with Defective Graphene Oxide and Reduced Graphene Oxide

Year: 2019

Journal: ACS Appl. Mater. Interfaces, Volume 11, 1-Sep, page 34517–34525

Authors: Genorio, Bostjan; Harrison, Katharine L.; Connell, Justin G.; Drazic, Goran; Zavadil, Kevin R.; Markovic, Nenad M.; Strmcnik, Dusan

Organizations: Joint Center for Energy Storage Research (JCESR), an Energy Innovation Hub - U.S. Department of Energy, Office of Science, Basic Energy SciencesUnited States Department of Energy (DOE); U.S. Department of Energy Office of Science laboratoryUnited States Department of Energy (DOE) [DE-ACO2-06CH11357]; U.S. Department of Energy, Basic Energy Science, Materials Science and Engineering DivisionUnited States Department of Energy (DOE); Slovenian Research Agency (ARRS) through the Research Core Funding Programme [P1-0175, BI-US/18-19-041]

Keywords: graphene oxide; reduced graphene oxide; interface; electrocatalysis; oxygen reduction reaction; hydrogen oxidation reaction; selectivity

Engineered solid-liquid interfaces will play an important role in the development of future energy storage and conversion (ESC) devices. In the present study, defective graphene oxide (GO) and reduced graphene oxide (rGO) structures were used as engineered interfaces to tune the selectivity and activity of Pt disk electrodes. GO was deposited on Pt electrodes via the Langmuir-Blodgett technique, which provided compact and uniform GO films, and these films were subsequently converted to rGO by thermal reduction. Electrochemical measurements revealed that both GO and rGO interfaces on Pt electrodes exhibit selectivity toward the oxygen reduction reaction (ORR), but they do not have an impact on the activity of the hydrogen oxidation reaction in acidic environments. Scanning transmission electron microscopy at atomic resolution, along with Raman spectroscopy, X-ray photoelectron spectroscopy (XPS), and scanning electron microscopy (SEM), revealed possible diffusion sites for H-2 and O-2 gas molecules and functional groups relevant to the selectivity and activity of these surfaces. Based on these insights, rGO interfaces are further demonstrated to exhibit enhanced activity for the ORR in nonaqueous environments and demonstrate the power of our ex situ engineering approach for the development of next-generation ESC devices.