Anisotropic Facet Doping Amplifies Built‐In Electric Field in Single‐Particle Photocatalysts

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Abstract
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.
Funding Information
  • National Key Research and Development Program of China (2023YFA1507102)
  • National Natural Science Foundation of China (22239001)
  • National Natural Science Foundation of China (22376062)
  • National Natural Science Foundation of China (22379043)
  • National Natural Science Foundation of China (92577119)
  • Science and Technology Commission of Shanghai Municipality (23520710700)
  • Science and Technology Commission of Shanghai Municipality (25DZ3000301)
  • Science and Technology Commission of Shanghai Municipality (24DX1400200)
  • Science and Technology Commission of Shanghai Municipality (22ZR1415700)

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