2026-04-17T10:14:52Zhttps://recercat.cat/oai/request

oai:recercat.cat:2072/4827512025-04-03T12:06:52Zcom_2072_98col_2072_378192

00925njm 22002777a 4500 dc Petersen, Amanda S. author Jensen, Kim D. author Wan, Hao author Bagger, Alexander author Chorkendorff, Ib author Stephens, Ifan E. L. author Rossmeisl, Jan author Escudero-Escribano, María author 2023 Electrolyte effects play an important role in the activity of the oxygen reduction reaction (ORR) of Pt-based electrodes. Herein, we combine a computational model and rotating disk electrode measurements to investigate the effects from phosphate anion poisoning for the ORR on well-defined extended Pt surfaces. We construct a model including the poisoning effect from phosphate species on Pt(111) and Cu/Pt(111) based on density functional theory simulations. By varying the subsurface Cu content of the Cu/Pt(111) alloy, we tune the *OH binding energies on the surface by means of ligand effects, and as a result, we tune the ORR activity. We have investigated the effect of adsorbed phosphate species at low overpotentials when tuning *OH binding energies. Our results display a direct scaling relationship between adsorbed *OH and phosphate species. From the model, we observe how the three-fold binding sites of phosphate anions limit the packing of poisoning phosphate on the surface, thus allowing for *OH adsorption even when poisoned. Our work shows that, regardless of surface site blockage from phosphate, the trend in the catalytic oxygen reduction activity is predominantly governed by the *OH binding. http://hdl.handle.net/2072/482751 Oxygen reduction reaction Platinum Near-surface alloys Density functional theory Anion Adsorption Modeling Anion Poisoning during Oxygen Reduction on Pt Near-Surface Alloys