<p>Graphdiyne (GDY), known for its tunable intrinsic bandgap, high charge carrier mobility, and broad-spectrum absorption, has garnered significant attention for photocatalytic hydrogen evolution. However, GDY/wide-band semiconductor photocatalysts suffer from limitations, including low doping concentrations and insufficient absorption in the visible-to-near-infrared (Vis-NIR) region, which restricts full-spectrum energy utilization. To address these challenges, we designed and synthesized a functional graphdiyne quantum dots (PG-QDs) incorporating perylene diimide (PDI) units. These PG-QDs exhibit tailored spectral absorption, reducing competition with wide-band semiconductors for UV light while enhancing Vis-NIR absorption and photothermal conversion performance. PG-QDs overcame 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 suppressed the recombination of photogenerated carriers and enhanced charge carrier separation efficiency. The hydrogen evolution rate reached 12.69 mmol g<sup>−1</sup> h<sup>−1</sup>, over thirty times higher than P25. This study presents a novel strategy for improving the full-spectrum energy utilization of GDY-based photocatalysts.</p>

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Functional graphdiyne based on perylene diimide units facilitating boosted performance of photothermal catalytic hydrogen evolution

  • Xinyue Jiang,
  • Huajun Xu,
  • Wentao Zou,
  • Xu Zhang,
  • Fei Jin,
  • Lingya Sun,
  • Wanzhang Ding,
  • Yuanyuan Kan,
  • Yanna Sun,
  • Ke Gao

摘要

Graphdiyne (GDY), known for its tunable intrinsic bandgap, high charge carrier mobility, and broad-spectrum absorption, has garnered significant attention for photocatalytic hydrogen evolution. However, GDY/wide-band semiconductor photocatalysts suffer from limitations, including low doping concentrations and insufficient absorption in the visible-to-near-infrared (Vis-NIR) region, which restricts full-spectrum energy utilization. To address these challenges, we designed and synthesized a functional graphdiyne quantum dots (PG-QDs) incorporating perylene diimide (PDI) units. These PG-QDs exhibit tailored spectral absorption, reducing competition with wide-band semiconductors for UV light while enhancing Vis-NIR absorption and photothermal conversion performance. PG-QDs overcame 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 suppressed the recombination of photogenerated carriers and enhanced charge carrier separation efficiency. The hydrogen evolution rate reached 12.69 mmol g−1 h−1, over thirty times higher than P25. This study presents a novel strategy for improving the full-spectrum energy utilization of GDY-based photocatalysts.