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<p>Covalent organic frameworks (COFs) benefit photothermal conversion through their light-harvesting capability and efficient non-radiative decay channels. However, the conversion kinetics are hampered by the phonon bottleneck imposed by the structural rigidity of the frameworks, which limits vibrational relaxation. Herein, we demonstrate a kinetic-promotion strategy to overcome this limitation using locally flexible COFs. By functionalizing the rigid frameworks with mobile aliphatic substituents, we established an additional energy thermalization pathway over the intrinsic skeleton routine. The mobile substituents served as built-in thermalization centers, accelerating the dissipation of excitation energy by providing a high density of low-frequency vibrational modes.</p>

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Accelerating photothermal conversion in covalent organic frameworks via skeleton-substituent cooperation

  • 期刊论文

  • 发表日期：

    2026年7月30日

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  • Nuolan Chen,
  • Ruike Xu,
  • Ting Song,
  • Zechun Pu,
  • Jinlong Zhu,
  • Qing Liao,
  • Zaoming Wang,
  • Cheng Gu,
  • Ping Wang

摘要

Covalent organic frameworks (COFs) benefit photothermal conversion through their light-harvesting capability and efficient non-radiative decay channels. However, the conversion kinetics are hampered by the phonon bottleneck imposed by the structural rigidity of the frameworks, which limits vibrational relaxation. Herein, we demonstrate a kinetic-promotion strategy to overcome this limitation using locally flexible COFs. By functionalizing the rigid frameworks with mobile aliphatic substituents, we established an additional energy thermalization pathway over the intrinsic skeleton routine. The mobile substituents served as built-in thermalization centers, accelerating the dissipation of excitation energy by providing a high density of low-frequency vibrational modes.