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<p>A series of novel host-guest complexes were synthesized using selenoviologen-based tetracationic cyclophane <b>1</b> (green box) and various electron-rich guests (<b>G</b><sub><b>1</b></sub>, <b>G</b><sub><b>2</b></sub>, <b>G</b><sub><b>3</b></sub>, and <b>G</b><sub><b>4</b></sub>). These complexes demonstrated high binding affinity and favorable redox properties due to the unique structural characteristics of selenoviologens. Femtosecond transient absorption (fs-TA) spectroscopy revealed that the host-guest complexes exhibited efficient charge separation and enhanced electron transfer. These complexes were subsequently assembled onto the surface of graphitic carbon nitride (g-C<sub>3</sub>N<sub>4</sub>) through hydrogen bonding interactions between the hydroxyl groups of the guests and the amino groups of g-C<sub>3</sub>N<sub>4</sub>, forming a series of functionalized composite materials. This assembly strategy facilitated the incorporation of the green box onto the g-C<sub>3</sub>N<sub>4</sub> surface, leading to rapid photo-induced electron transfer (PET) and a significant delay in charge recombination. As a result, the photocatalytic hydrogen production efficiency was markedly improved. Notably, the g-C<sub>3</sub>N<sub>4</sub>/<b>1</b>⊃<b>G</b><sub><b>4</b></sub>/Pt composites achieved the highest efficiency for visible-light-driven hydrogen evolution, exhibiting a higher H<sub>2</sub> evolution rate (2765 µmol g<sup>−1</sup> h<sup>−1</sup>), an apparent quantum yield (AQY) of 1.08 × 10<sup>−2</sup>, turnover number (TON) of 216 and turnover frequency (TOF) of 1.5 × 10<sup>−2</sup> s<sup>−1</sup>, with a production rate six times greater than that of unmodified g-C<sub>3</sub>N<sub>4</sub>/Pt composites.</p>

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Hydrogen-bonded green box-based host-guest complexes on g-C3N4 composites for enhanced visible-light photocatalysis

  • 期刊论文

  • 发表日期：

    2025年3月31日

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  • Yawen Li,
  • Naiyao Li,
  • Tianle Cao,
  • Yujing Gao,
  • Chenjing Liu,
  • Zengrong Wang,
  • Ni Yan,
  • Guoping Li,
  • Qing-Hui Guo,
  • Gang He

摘要

A series of novel host-guest complexes were synthesized using selenoviologen-based tetracationic cyclophane 1 (green box) and various electron-rich guests (G1, G2, G3, and G4). These complexes demonstrated high binding affinity and favorable redox properties due to the unique structural characteristics of selenoviologens. Femtosecond transient absorption (fs-TA) spectroscopy revealed that the host-guest complexes exhibited efficient charge separation and enhanced electron transfer. These complexes were subsequently assembled onto the surface of graphitic carbon nitride (g-C3N4) through hydrogen bonding interactions between the hydroxyl groups of the guests and the amino groups of g-C3N4, forming a series of functionalized composite materials. This assembly strategy facilitated the incorporation of the green box onto the g-C3N4 surface, leading to rapid photo-induced electron transfer (PET) and a significant delay in charge recombination. As a result, the photocatalytic hydrogen production efficiency was markedly improved. Notably, the g-C3N4/1⊃G4/Pt composites achieved the highest efficiency for visible-light-driven hydrogen evolution, exhibiting a higher H2 evolution rate (2765 µmol g−1 h−1), an apparent quantum yield (AQY) of 1.08 × 10−2, turnover number (TON) of 216 and turnover frequency (TOF) of 1.5 × 10−2 s−1, with a production rate six times greater than that of unmodified g-C3N4/Pt composites.