Selective formation of interfacial bonding enables superior hydrogen production in organic–inorganic hybrid cocatalyzed photocatalysts

Abstract Rational design of cocatalysts on semiconductor photocatalysts holds great promise for boosting the photo-to-electron conversion efficiency. However, constructing favorable interfacial structure facilitating the charge carriers’ transportation in photocatalyst system remains challenging. Here, we demonstrate an organic–inorganic hybrid cocatalyzed photocatalyst with tunable interfacial structure for photocatalytic hydrogen (H2) production, where polyaniline (PANI) monolayer and Pt nanoparticles cocatalyzed CdS is a proof-of-concept. The selective formation of adequate interfacial bonding at both the cocatalyst/semiconductor interfaces, and the organic/inorganic cocatalyst interface is the key to promote charge carriers’ transport. The photocatalytic H2 production rate of CdS/PANI-O/Pt-OH with adequate S-C, S-Pt and Pt-N interfacial bonding is 16 times and 84 times that of CdS/PANI-R/Pt-H with much less interfacial bonding and pristine CdS, respectively. And superior apparent quantum efficiency of 92.1% at 440 nm is achieved. This finding opens up a rational approach to understanding and engineering the interfacial structure in various energy conversion systems.