Embedding Thiophene-Amide into g-C3N4 Skeleton with Induction and Delocalization Effects for High Photocatalytic H2 Evolution

Molecular skeleton modification has become a recognized method that can effectively improve the photocatalytic performance of g-C3N4because it not only effectively promotes charge separation, but also tunes the conjugated system of g-C3N4to make it more conducive to photocatalytic reaction. Herein, thiophene-amide embedded g-C3N4(TA-CN-x) was successfully prepared by simple one-step thermal polycondensation using urea as a precursor and ethyl-2-amino-4-phenylthiophene-3-carboxylate (EAPC) as an additive. After embedding with thiophene-amide, the induction and delocalization effects are formed in TA-CN-x, which significantly improves the migration efficiency of photogenerated charge carriers. Meanwhile, the conjugate structure is changed due to structural modification, resulting in significant enhancement of visible light absorption compared to the pure g-C3N4(CN). Specifically, the optimized photocatalytic H2evolution rate of TA-CN-2 reaches 245.4 μmol·h−1, which is 8.4 times that of CN (with Pt nanoparticles as a co-catalyst), and the apparent quantum efficiency (AQY) at 450 nm is 13.6%. This work opens up a new modification process for fully tapping the photocatalytic hydrogen absorption potential of g-C3N4-based materials.Keywords:photocatalysts;g-C3N4;thiophene-amide;embedding;induction effect;delocalization effect;hydrogen evolution