Rapid Hole Transfer and Molecular Enrichment at Amorphous‐Crystalline Interfaces of Pt_0.25%/TO(B)‐FCP for Efficient Photocatalysis

Abstract The construction of amorphous‐crystalline interfaces of heterogeneous metal oxide systems is an effective approach to modulate the interfacial adsorption behavior and carrier transfer pathways for the photocatalytic process. In this work, the amorphous‐crystalline interface is constructed by covalently linking a flexible crosslinked polymer (FCP) layer to a Pt 0.25% /TO(B) substrate. Adsorption‐photodegradation experiments show that Pt 0.25% /TO(B)‐FCP can ultimately enrich bisphenol A molecules to the interface within 5 min and in situ‐photodegrade >97.0% of bisphenol A within 10 min (50 ppm), which is 6.21 times than pure TO(B). In addition to the efficient accumulation of BPA molecules, the rapid hole transfer pathway at the amorphous‐crystalline interface is revealed by theoretical calculations, Kelvin probe force microscopy, and photoelectrochemical characterization. The coexistence of Pt single atoms (SAs) and nanoclusters (NCs) optimizes the transfer kinetics and reduces the energy barrier of photogenerated holes of TO(B). Meanwhile, the covalent hole transfer channels between the FCP layer and Pt 0.25% /TO(B) significantly accelerate the separation and transfer of photogenerated carrier, promoting the photodegradation of adsorbed BPA molecules.