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<p>High-performance heterogeneous photocatalysts are essential for advancing visible-light-driven chemical transformations. This study presents a stepwise surface-engineering approach to progressively enhance the photocatalytic activities of covalent organic frameworks (COFs). Starting with an enamine-based COF (<b>JNU-221</b>), a Doebner reaction was utilized to lock the enamine linkages into rigid quinoline structures, affording a carboxyl-functionalized COF (<b>JNU-222</b>) with significantly enhanced chemical stability. Subsequent substitution of the phenyl rings on the skeleton by triazine and pyridine rings led to two nitrogen-rich COFs (<b>JNU-223</b> and <b>JNU-224</b>). Optical and electrochemical studies reveal a continuously increased light-harvesting and charge-separation efficiency with carboxyl functionalization and nitrogen introduction. As a result, JNU-224 exhibits exceptional photocatalytic performance, achieving a 99% conversion rate in the sulfide oxidation reaction under visible-light irradiation in just 2 h. This study offers a simple yet practical strategy for developing highly efficient heterogeneous photocatalysts for sustainable organic transformations, highlighting the potential of metal-free COFs in environmentally related applications.</p>

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Stepwise surface-engineering of covalent organic frameworks for enhanced photocatalytic performance

  • 期刊论文

  • 发表日期：

    2025年6月26日

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  • Kun Wu,
  • Qin-Hong Wang,
  • Hao-Bo Wang,
  • Ying Wang,
  • Fei-Long Luo,
  • Weigang Lu,
  • Dan Li

摘要

High-performance heterogeneous photocatalysts are essential for advancing visible-light-driven chemical transformations. This study presents a stepwise surface-engineering approach to progressively enhance the photocatalytic activities of covalent organic frameworks (COFs). Starting with an enamine-based COF (JNU-221), a Doebner reaction was utilized to lock the enamine linkages into rigid quinoline structures, affording a carboxyl-functionalized COF (JNU-222) with significantly enhanced chemical stability. Subsequent substitution of the phenyl rings on the skeleton by triazine and pyridine rings led to two nitrogen-rich COFs (JNU-223 and JNU-224). Optical and electrochemical studies reveal a continuously increased light-harvesting and charge-separation efficiency with carboxyl functionalization and nitrogen introduction. As a result, JNU-224 exhibits exceptional photocatalytic performance, achieving a 99% conversion rate in the sulfide oxidation reaction under visible-light irradiation in just 2 h. This study offers a simple yet practical strategy for developing highly efficient heterogeneous photocatalysts for sustainable organic transformations, highlighting the potential of metal-free COFs in environmentally related applications.