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<p>The topological nanopores of covalent organic frameworks (COFs) are promising platforms for constructing photocatalytic nanoreactors for CO<sub>2</sub> conversion. However, simultaneously increasing electron density, promoting electron transfer, and enhancing CO<sub>2</sub> adsorption and activation within confined nanopore spaces remain critical challenges for boosting photocatalytic performance. Herein, polyhydroxylated fullerene (C<sub>60</sub>OH) molecules were assembled within the nanopores of a two-dimensional porphyrin-based COF (pCOF) through hydrogen-bonding interactions with the hydroxyl-functionalized 2,5-dihydroxyterephthalaldehyde (DHTA) acceptor units in the pCOF, thereby constructing a C<sub>60</sub>OH@pCOF photocatalytic nanoreactor featuring DHTA–C<sub>60</sub>OH molecular heterojunctions. Under full-light irradiation, the optimized C<sub>60</sub>OH@pCOF achieves a CO production rate of 40.47&#xa0;μmol/(g·h) in pure water, approximately four times higher than that of pristine pCOF, along with a CO selectivity of 99%. This remarkable enhancement is mainly attributable to the introduction of C<sub>60</sub>OH molecules into the pCOF, which facilitates the directional transfer of photogenerated electrons from the porphyrin donor to the DHTA moieties and then to the C<sub>60</sub>OH acceptor. Moreover, the abundant surface hydroxyl groups on C<sub>60</sub>OH serve as metal-free catalytic sites that effectively activate pre-accumulated CO<sub>2</sub> within the nanopore-based reactor and promote the formation and conversion of key intermediates. This study provides new insights into the design and construction of porous crystalline framework-based photocatalytic nanoreactors.</p>

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Confined Polyhydroxylated C60 in Porphyrin COF Nanopore as Nanoreactor for CO2 Photoreduction

  • 期刊论文

  • 发表日期：

    2026年7月1日

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  • Shengzhong Hao,
  • Xudong Yan,
  • Haochun Yin,
  • Hongqi Wang,
  • Jiaxin Yu,
  • Linlu Bai

摘要

The topological nanopores of covalent organic frameworks (COFs) are promising platforms for constructing photocatalytic nanoreactors for CO2 conversion. However, simultaneously increasing electron density, promoting electron transfer, and enhancing CO2 adsorption and activation within confined nanopore spaces remain critical challenges for boosting photocatalytic performance. Herein, polyhydroxylated fullerene (C60OH) molecules were assembled within the nanopores of a two-dimensional porphyrin-based COF (pCOF) through hydrogen-bonding interactions with the hydroxyl-functionalized 2,5-dihydroxyterephthalaldehyde (DHTA) acceptor units in the pCOF, thereby constructing a C60OH@pCOF photocatalytic nanoreactor featuring DHTA–C60OH molecular heterojunctions. Under full-light irradiation, the optimized C60OH@pCOF achieves a CO production rate of 40.47 μmol/(g·h) in pure water, approximately four times higher than that of pristine pCOF, along with a CO selectivity of 99%. This remarkable enhancement is mainly attributable to the introduction of C60OH molecules into the pCOF, which facilitates the directional transfer of photogenerated electrons from the porphyrin donor to the DHTA moieties and then to the C60OH acceptor. Moreover, the abundant surface hydroxyl groups on C60OH serve as metal-free catalytic sites that effectively activate pre-accumulated CO2 within the nanopore-based reactor and promote the formation and conversion of key intermediates. This study provides new insights into the design and construction of porous crystalline framework-based photocatalytic nanoreactors.