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<p>Covalent organic frameworks (COFs) are emerging as promising photocatalysts owing to their tailorable structures, exceptional crystallinity, and robustness. However, the photocatalytic performance of COFs is limited by fast charge recombination and inefficient charge migration. Herein, a novel post-synthetic partial protonation strategy is proposed to construct COFs with asymmetric unprotonated/protonated homojunctions, which endow them with an enlarged molecular dipole moment, thereby generating a strong built-in electric field that significantly enhances the charge separation and transport efficiencies in COFs. In addition, the protonation process extends the light absorption range and improves the hydrophilicity of COFs. The photocatalytic hydrogen evolution rate of the partially protonated TPE-COF and ETTBA-COF is enhanced by 88- and 175-fold relative to their pristine counterparts, 4.3 and 2.48 times those of fully protonated counterparts, respectively. Our results clearly demonstrate the pivotal role of the asymmetric unprotonated/protonated homojunctions within COFs in the photocatalytic hydrogen evolution. This post-synthetic partial protonation strategy provides a novel paradigm for establishing internal electric fields within COFs.</p>

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Covalent organic frameworks with asymmetric unprotonated/protonated structures for efficient photocatalytic hydrogen evolution

  • 期刊论文

  • 发表日期：

    2025年1月3日

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  • Xiangyu Zhang,
  • Chao Gao,
  • Yongxiang Zhou,
  • Rufan Chen,
  • Xuhui Guan,
  • Zhili Shen,
  • Bincheng Hu,
  • Qing-Hua Xu

摘要

Covalent organic frameworks (COFs) are emerging as promising photocatalysts owing to their tailorable structures, exceptional crystallinity, and robustness. However, the photocatalytic performance of COFs is limited by fast charge recombination and inefficient charge migration. Herein, a novel post-synthetic partial protonation strategy is proposed to construct COFs with asymmetric unprotonated/protonated homojunctions, which endow them with an enlarged molecular dipole moment, thereby generating a strong built-in electric field that significantly enhances the charge separation and transport efficiencies in COFs. In addition, the protonation process extends the light absorption range and improves the hydrophilicity of COFs. The photocatalytic hydrogen evolution rate of the partially protonated TPE-COF and ETTBA-COF is enhanced by 88- and 175-fold relative to their pristine counterparts, 4.3 and 2.48 times those of fully protonated counterparts, respectively. Our results clearly demonstrate the pivotal role of the asymmetric unprotonated/protonated homojunctions within COFs in the photocatalytic hydrogen evolution. This post-synthetic partial protonation strategy provides a novel paradigm for establishing internal electric fields within COFs.