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<p>Perylenediimide (PDI) materials have gained considerable interest as photocatalysts owing to their exceptional photophysical properties. However, the development of PDI-based photocatalysts remains constrained by several critical limitations, such as rapid charge recombination and aggregation-induced quenching. Here, we report the design and synthesis of a crystalline porous metal-perylenediimide framework (MPF) through the self-assmebly of PDI-based tetracarboxylate ligand (<b>H</b><sub><b>4</b></sub><b>PDI</b>) with Ce<sup>3+</sup> ions. The resulting <b>Ce-PDI</b> framework features a distinctive double-walled porous structure, stabilized by robust <i>π</i>-<i>π</i> stacking interactions between PDI units. This architecture offers abundant active sites and ample space for substrate-catalyst interactions, while mitigating aggregation-induced quenching of PDI units and facilitating efficient photogenerated charge transfer. Compared to the hydrogen-bonded assembly <b>H</b><sub><b>4</b></sub><b>PDI</b> with its dense packing, our double-walled porous <b>Ce-PDI</b> framework demonstrated markedly improved photocatalytic activity and recyclability. Specifically, <b>Ce-PDI</b> achieved catalytic yields of up to 95% for the C-3 formylation of indoles and 97% for the condensation of <i>o</i>-phenylenediamine with aromatic aldehydes, significantly outperforming <b>H</b><sub><b>4</b></sub><b>PDI</b>, which only achieved yields of 16%–34%. This work provides a simple and effective approach to overcoming the inherent limitations of PDI-based photocatalysts, thereby advancing their catalytic performance.</p>

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A double-walled porous metal-perylenediimide framework for enhanced photocatalysis

  • 期刊论文

  • 发表日期：

    2025年4月14日

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  • Li-Li Ma,
  • Feinian Yang,
  • Longyi Ding,
  • Duojun Cao,
  • Yang Li,
  • Qingchun Xia,
  • Ying-Feng Han,
  • Guozan Yuan

摘要

Perylenediimide (PDI) materials have gained considerable interest as photocatalysts owing to their exceptional photophysical properties. However, the development of PDI-based photocatalysts remains constrained by several critical limitations, such as rapid charge recombination and aggregation-induced quenching. Here, we report the design and synthesis of a crystalline porous metal-perylenediimide framework (MPF) through the self-assmebly of PDI-based tetracarboxylate ligand (H4PDI) with Ce3+ ions. The resulting Ce-PDI framework features a distinctive double-walled porous structure, stabilized by robust π-π stacking interactions between PDI units. This architecture offers abundant active sites and ample space for substrate-catalyst interactions, while mitigating aggregation-induced quenching of PDI units and facilitating efficient photogenerated charge transfer. Compared to the hydrogen-bonded assembly H4PDI with its dense packing, our double-walled porous Ce-PDI framework demonstrated markedly improved photocatalytic activity and recyclability. Specifically, Ce-PDI achieved catalytic yields of up to 95% for the C-3 formylation of indoles and 97% for the condensation of o-phenylenediamine with aromatic aldehydes, significantly outperforming H4PDI, which only achieved yields of 16%–34%. This work provides a simple and effective approach to overcoming the inherent limitations of PDI-based photocatalysts, thereby advancing their catalytic performance.