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: P3̅m1 (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 d-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.
Li et al. (Sun,) studied this question.