Wenbo Li

Controllable chemical doping is an effective strategy to tailor electronic structure and charge‐carrier dynamics in semiconductors, especially in one‐step‐excitation semiconductor photocatalysts. However, achieving a controllable dopant distribution within a single‐particle photocatalyst without compromising its well‐defined redox facets remains a significant challenge. Here, using a two‐step molten‐salt synthesis as a controlled platform, we reveal facet‐selective Al ³⁺ incorporation in SrTiO ₃ while preserving the desired cuboctahedron morphology with exposed {100}/{111} facets. Increasing the Al ³⁺ supply within this morphology‐preserving window leads to a pronounced facet‐anisotropic distribution within individual particles, with the Al content along {111} exceeding that along {100} by more than twofold from the surface toward the bulk. This facet‐anisotropic distribution enhances the inter‐facet electrostatic asymmetry associated with the intrinsic built‐in electric field. As a demonstration, 4.0 mol% Al‐doped SrTiO ₃ delivers an apparent quantum yield of 81.1% at 335 nm for overall water splitting, producing H ₂ and O ₂ in a stoichiometric 2:1 ratio with a hydrogen evolution rate of 3364.13 µmol·h ⁻¹ . This work establishes facet‐resolved dopant distribution as a spatial design parameter for efficient particulate photocatalysis.

Strain relaxation in atomically thin two-dimensional (2D) materials typically leads to geometric wrinkles or ripples. These intrinsic structural features can significantly influence the material’s electronic and mechanical properties, playing a crucial role in modifying catalytic behavior. Here, we report a strain-induced wrinkling strategy to construct synergistic active sites in Pt-doped Pd metallenes for efficient acidic hydrogen evolution reaction. Controlled Pt doping generates lattice mismatch and internal stress, driving spontaneous wrinkle formation. Characterization reveals that these wrinkled regions integrate electron transfer with localized strain effects, serving as efficient active sites. This geometry-electron synergy lowers the activation barrier, shifting reaction kinetics toward the efficient Volmer–Tafel pathway. Consequently, the optimized Pt_5.0-Pd ML achieves an ultralow overpotential of 18 mV at 10 mA cm^–2, significantly outperforming commercial benchmarks. This work highlights wrinkle engineering as a key strategy for tuning metallene catalytic performance, offering a rational design route for advanced 2D electrocatalysts.