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<p>Rational molecular design of covalent organic frameworks (COFs) integrating site-specific capture capability and efficient charge transfer dynamics is pivotal for maximizing photocatalytic performance. However, there is a lack of systematic studies on the influence of the delicate balance between adsorption energy and photocatalytic activity. Herein, we designed a series of ternary COFs (TB-C, TTB-C, and TP-C) with precisely engineered site-specific chelating mechanical arm motifs to systematically explore how the coupling of adsorption energy and photocatalytic activity dictates uranium removal performance. Compared with TB-C and TP-C, extended benzene ring moieties in TTB-C fine-tune electron cloud distribution and elongate charge transport pathways simultaneously, endowing TTB-C with moderate uranyl adsorption energy yet achieving the optimal uranium removal performance. Consequently, TTB-C achieves an optimal U(VI) removal efficiency of 99% within 3 h, which is consistent with volcano plot predictions. Theoretical calculations and mechanisms analysis reveal a counterintuitive phenomenon that moderate and well-matched adsorption energy for uranyl ions favors efficient U(VI) desorption, in turn elevating the collision probability with <i>in-situ</i> generated H<sub>2</sub>O<sub>2</sub> to form insoluble (UO<sub>2</sub>)O<sub>2</sub>·2H<sub>2</sub>O precipitates. This is the first case to elucidate the delicate balance between U(VI) adsorption energy and photocatalytic activity in governing uranium removal efficiency, providing a rational molecular design paradigm for advanced photocatalytic COFs in radionuclide remediation.</p>

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Insight into balancing adsorption and photocatalysis in ternary covalent organic frameworks with site-specific capture for maximized photocatalytic uranium extraction

  • 期刊论文

  • 发表日期：

    2026年6月22日

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  • Jinghan Hao,
  • Yayu Dong,
  • Yanan Cheng,
  • Yunxuan Wu,
  • Chang Liu,
  • Zhimin Dong,
  • Xishi Tai,
  • Zhibin Zhang,
  • Yunhai Liu,
  • Xiaohong Cao,
  • Xiangke Wang

摘要

Rational molecular design of covalent organic frameworks (COFs) integrating site-specific capture capability and efficient charge transfer dynamics is pivotal for maximizing photocatalytic performance. However, there is a lack of systematic studies on the influence of the delicate balance between adsorption energy and photocatalytic activity. Herein, we designed a series of ternary COFs (TB-C, TTB-C, and TP-C) with precisely engineered site-specific chelating mechanical arm motifs to systematically explore how the coupling of adsorption energy and photocatalytic activity dictates uranium removal performance. Compared with TB-C and TP-C, extended benzene ring moieties in TTB-C fine-tune electron cloud distribution and elongate charge transport pathways simultaneously, endowing TTB-C with moderate uranyl adsorption energy yet achieving the optimal uranium removal performance. Consequently, TTB-C achieves an optimal U(VI) removal efficiency of 99% within 3 h, which is consistent with volcano plot predictions. Theoretical calculations and mechanisms analysis reveal a counterintuitive phenomenon that moderate and well-matched adsorption energy for uranyl ions favors efficient U(VI) desorption, in turn elevating the collision probability with in-situ generated H2O2 to form insoluble (UO2)O2·2H2O precipitates. This is the first case to elucidate the delicate balance between U(VI) adsorption energy and photocatalytic activity in governing uranium removal efficiency, providing a rational molecular design paradigm for advanced photocatalytic COFs in radionuclide remediation.