Functional graphdiyne based on perylene diimide units facilitating boosted performance of photothermal catalytic hydrogen evolution
Graphdiyne (GDY) possesses a tunable intrinsic bandgap, high charge carrier mobility, and broad-spectrum absorption, making it a candidate for photocatalytic hydrogen evolution. However, GDY/wide-band semiconductor photocatalysts are constrained by low doping concentrations and insufficient absorption in the visible-to-near-infrared (Vis-NIR) region, which limits full-spectrum energy utilization. To address these limitations, functional graphdiyne quantum dots (PG-QDs) incorporating perylene diimide (PDI) units were designed and synthesized. The PG-QDs exhibit tailored spectral absorption, reducing competition with wide-band semiconductors for UV light while enhancing Vis-NIR absorption and photothermal conversion. The PG-QDs overcome the doping concentration limitations of conventional GDY-based photocatalysts, achieving an optimal doping ratio of 15% without suppressing hydrogen evolution activity. The pronounced photothermal effect effectively suppresses the recombination of photogenerated carriers and enhances charge carrier separation efficiency. The hydrogen evolution rate reached 12.69 mmol g−1 h−1, over thirty times higher than that of P25. This study presents a strategy for improving the full-spectrum energy utilization of GDY-based photocatalysts.