Efficient Charge Migration in Chemically-Bonded Prussian Blue Analogue/CdS with Beaded Structure for Photocatalytic H(2) Evolution

[Image: see text] The design of a powerful heterojunction structure and the study of the interfacial charge migration pathway at the atomic level are essential to mitigate the photocorrosion and recombination of electron–hole pairs of CdS in photocatalytic hydrogen evolution (PHE). A temperature-induced self-assembly strategy has been proposed for the syntheses of Prussian blue analogue (PBA)/CdS nanocomposites with beaded structure. The specially designed structure had evenly exposed CdS which can efficiently harvest visible light and inhibit photocorrosion; meanwhile, PBA with a large cavity provided channels for mass transfer and photocatalytic reaction centers. Remarkably, PB-Co/CdS-LT-3 exhibits a PHE rate of 57 228 μmol h(–1) g(–1), far exceeding that of CdS or PB-Co and comparable to those of most reported crystalline porous material-based photocatalysts. The high performances are associated with efficient charge migration from CdS to PB-Co through CN-Cd electron bridges, as revealed by the DFT calculations. This work sheds light on the exploration of heterostructure materials in efficient PHE.