Structural amine-induced interfacial electrical double layers for efficient photocatalytic H₂ evolution

The efficiency of photocatalytic hydrogen evolution is fundamentally constrained by limited charge carrier separation. Herein, we deliberately engineered an electric double layer (EDL) <i>via</i> surface modification with positively charged molecules, which optimizes the charge carrier dynamics. The anchoring of both diethylenetriamine (DETA) molecules and Pt species on CdS (denoted as Pt/CdS-D) achieves remarkable H₂ evolution performance, delivering an exceptional rate of 6295 μmol g^-1 h^-1 and an apparent quantum efficiency of 14.9%, which is 26.7-fold enhanced compared to that of CdS. The synergistic modification strategy concurrently lowers the activation energy barrier for water reduction and establishes EDL-driven directional charge transport channels that boost carrier separation efficiency. This work provides a paradigm for designing high-performance photocatalysts through the rational integration of functional organic groups and cocatalysts, opening new avenues for advanced solar-to-hydrogen energy conversion systems.