In this project, we designed and synthesized a series of benzothiadiazole-based electron-withdrawing compounds: DPASBT-2F, IDBSBT-2F, PXZSBT-2F, DPASBT-2CN, and IDBSBT-2CN. By tuning electron-donating and functional groups, their photophysical properties and energy levels were optimized.
Fluorinated compounds exhibited absorption from blue to green light, while cyano-substituted compounds covered the entire visible spectrum. Cyclic voltammetry and energy level calculations confirmed that replacing fluorine with the stronger electron-withdrawing cyano group lowered the LUMO level, reducing the energy gap and facilitating electron transfer for photocatalytic hydrogen evolution.
ICP-OES analysis revealed minimal palladium residue in PXZSBT-2F, which achieved a hydrogen evolution rate of 237.26 μmol h⁻¹ g⁻¹, demonstrating high HER efficiency without the requirement for a metal cocatalyst. Through new material design and optimization of photocatalytic processes, it is hoped that these organic small molecule photocatalytic materials will provide sustainable and scalable energy solutions for the future.