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<p>The development of sustainable, metal-free photocatalysts that combine homogeneous reactivity with effective recyclability remains a key challenge in photoredox catalysis. Here, we report a series of rationally designed polymers of intrinsic microporosity (PIMs) tailored for visible light-driven photoredox reactions. Using a multidisciplinary approach by integrating in silico predictions, photophysical and materials characterization, and a series of benchmarking studies, we establish these PIMs as highly effective photocatalysts with broad applicability across diverse photoredox reactions, including Minisci reactions, aryl amination, trifluoromethylation, radical sulfonylation, and dual Ni-catalyzed C–N, C–C, and C–S couplings. We further evaluate multiple recycling strategies, including precipitation, heterogeneous coating, and homogeneous recovery by nanofiltration. The PIM catalysts exhibit near-complete retention in nanofiltration, enabling the development of a continuous-flow reaction–separation system with in-line catalyst recovery and real-time process monitoring. This work establishes a platform for tunable, scalable, and recyclable photocatalysis and provides a blueprint for sustainable continuous-flow fine chemical manufacturing.</p>

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Tailoring polymers of intrinsic microporosity as photoredox catalysts for continuous-flow reaction–separation processes

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年6月2日

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  • Martin Gede,
  • Gergo Ignacz,
  • Catherine S. P. De Castro,
  • Busra Dereli,
  • Mariia Ferree,
  • Frederic Laquai,
  • Luigi Cavallo,
  • Gyorgy Szekely

摘要

The development of sustainable, metal-free photocatalysts that combine homogeneous reactivity with effective recyclability remains a key challenge in photoredox catalysis. Here, we report a series of rationally designed polymers of intrinsic microporosity (PIMs) tailored for visible light-driven photoredox reactions. Using a multidisciplinary approach by integrating in silico predictions, photophysical and materials characterization, and a series of benchmarking studies, we establish these PIMs as highly effective photocatalysts with broad applicability across diverse photoredox reactions, including Minisci reactions, aryl amination, trifluoromethylation, radical sulfonylation, and dual Ni-catalyzed C–N, C–C, and C–S couplings. We further evaluate multiple recycling strategies, including precipitation, heterogeneous coating, and homogeneous recovery by nanofiltration. The PIM catalysts exhibit near-complete retention in nanofiltration, enabling the development of a continuous-flow reaction–separation system with in-line catalyst recovery and real-time process monitoring. This work establishes a platform for tunable, scalable, and recyclable photocatalysis and provides a blueprint for sustainable continuous-flow fine chemical manufacturing.