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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_xthat improve Pt surface energetics for the hydrogen evolution reaction (HER) within an alkaline electrolyte. The Pt‐CeO_xinterfaces are formed by depositing size‐controlled Pt nanoparticles onto a carbon support already coated with ultrathin CeO_xnanosheets. 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_xinterfaces. This study underscores the significance and potential of harnessing robust interfacial effects to enhance electrocatalytic reactions. 

This study demonstrates an atomic composition manipulation on Pt–Ni nano-octahedra to enhance their electrocatalytic performance. By selectively extracting Ni atoms from the {111} facets of the Pt–Ni nano-octahedra using gaseous carbon monoxide at an elevated temperature, a Pt-rich shell is formed, resulting in an ∼2 atomic layer Pt-skin. The surface-engineered octahedral nanocatalyst exhibits a significant enhancement in both mass activity (∼1.8-fold) and specific activity (∼2.2-fold) toward the oxygen reduction reaction compared with its unmodified counterpart. After 20,000 potential cycles of durability tests, the surface-etched Pt–Ni nano-octahedral sample shows a mass activity of 1.50 A/mgPt, exceeding the initial mass activity of the unetched counterpart (1.40 A/mgPt) and outperforming the benchmark Pt/C (0.18 A/mgPt) by a factor of 8. DFT calculations predict this improvement with the Pt surface layers and support these experimental observations. This surface-engineering protocol provides a promising strategy for developing novel electrocatalysts with improved catalytic features.