Two-Dimensional New Phase Zirconium Dioxide Supported Platinum Interface for Acidic Hydrogen Evolution Reaction

Platinum (Pt) is the benchmark catalyst for acidic hydrogen evolution (HER) but suffers from high cost and suboptimal adsorption-desorption kinetics. Interface engineering offers a solution, yet support selection remains critical. Here, we propose a new two-dimensional trigonal metastable phase zirconium dioxide (Tri-ZrO₂, space group: <i>P</i>3̅<i>m</i>1 (164)) as an advanced support for anchoring Pt nanoparticles (Pt NPs). Tri-ZrO₂ induces significant charge enrichment in the supported Pt NPs (Pt/Tri-ZrO₂). When evaluated for acidic HER, Pt/Tri-ZrO₂ exhibits a low overpotential of 9 mV at -10 mA cm^-2 and a Tafel slope of 18.7 mV dec^-1. Theoretical calculations and experimental results reveal that the Tri-ZrO₂ support modulates the electronic structure of Pt NPs, stabilizing the charge-enriched Pt species. The resulting downshifted <i>d</i>-band center of Pt weakens hydrogen intermediate (H*) binding, thereby accelerating H₂ production. This work provides a novel strategy for synthesizing unconventional-phase oxides and advances the electronic engineering of Pt-based materials for efficient electrocatalysis.