Construction of a Pt‐CeO_x Interface for the Electrocatalytic Hydrogen Evolution Reaction

Abstract The creation of metal‐metal oxide interfaces is an important approach to fine‐tuning catalyst properties through strong interfacial interactions. This article presents the work on developing interfaces between Pt and CeO_x that improve Pt surface energetics for the hydrogen evolution reaction (HER) within an alkaline electrolyte. The Pt‐CeO_x interfaces are formed by depositing size‐controlled Pt nanoparticles onto a carbon support already coated with ultrathin CeO_x nanosheets. This interface structure facilitates substantial electron transfer from Pt to CeO_x, resulting in decreased hydrogen binding energies on Pt surfaces, and water dissociation for the HER, as predicted by the density functional theory (DFT) calculations. Electrochemical testing indicates that both Pt specific activity and mass activity are improved by a factor of 2 to 3 following the formation of Pt‐CeO_x interfaces. This study underscores the significance and potential of harnessing robust interfacial effects to enhance electrocatalytic reactions.