Journal
JOURNAL OF PHYSICAL CHEMISTRY C
Volume 126, Issue 34, Pages 14509-14517Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpcc.2c05169
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Funding
- Department of Energy, Office of Energy Efficiency and Renewable Energy, Fuel Cell Technologies Office (FCTO) [DE EE0008434]
- U.S. Department of Energy, Office of Energy Efficiency and Renewable Energy, FCTO
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Ionic liquid interlayers and hydrophobic cations improve the oxygen reduction reaction kinetics on Pt(111) catalyst. The incorporation of a modified Frumkin isotherm accurately simulates the disorder-order transition observed in hydroxyl and bisulfate adsorption. Ionic liquids impact solvation to break scaling relations between OHad and O-ad adsorption strength, resulting in higher availability of active sites.
Ionic liquid interlayers improve the oxygen reduction reaction (ORR) kinetics on bulk and nanostructured catalysts for both Pt and alloyed-Pt materials. Despite the demonstrated performance enhancement at the half-cell and membrane electrode assembly level, the mechanism of the improvement is not fully understood. In this work, we combine single-crystal experiments with microkinetic modeling to uncover the origin of the ORR kinetic improvement on Pt(111) in the presence of ionic liquids and hydrophobic cations. With the incorporation of a modified Frumkin isotherm, our model accurately simulates the disorder-order transition observed in hydroxyl and bisulfate adsorption on Pt(111) under acidic conditions. Voltametric analysis shows that ionic liquids impact solvation to break so-called scaling relations between the adsorption strength of OHad and O-ad, but these effects have little impact on ORR activity. Instead, destabilized OHad reduces the overall hydroxyl (spectator) coverage, resulting in higher availability of active sites.
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