<p>The safe and sustainable development of nuclear energy depends in part on the effective capture of volatile radioactive iodine released from reprocessing off-gas, yet existing adsorbents suffer from poor kinetics, low utilization efficiency, or inadequate stability under harsh conditions. Here, we report a rationally designed imidazole-based covalent organic framework (BI-TAPB-COF) that enables efficient iodine capture through synergistic charge-transfer interactions. The fully conjugated backbone endows the material with exceptional chemical and thermal stability, while the ordered pore channels and embedded electron-rich imidazole groups serve as Lewis basic sites to facilitate strong host-guest interactions with iodine molecules. As a result, BI-TAPB-COF achieves a high dynamic adsorption capacity of 0.402 g/g under demanding conditions (75 °C, 20 mL/min), outperforming commercial silver zeolite and silica gel. Mechanistic investigations reveal the formation of polyiodide anions (I<sub>3</sub><sup>−</sup> and I<sub>5</sub><sup>−</sup>) <i>via</i> charge-transfer interactions.</p>

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A Fully Conjugated Imidazole-based Covalent Organic Framework for Efficient Dynamic Capture of Radioactive Iodine

  • Wenqi Zhang,
  • Zhonglin Ma,
  • Songbai Tang,
  • Linwei He,
  • Long Chen,
  • Shuao Wang

摘要

The safe and sustainable development of nuclear energy depends in part on the effective capture of volatile radioactive iodine released from reprocessing off-gas, yet existing adsorbents suffer from poor kinetics, low utilization efficiency, or inadequate stability under harsh conditions. Here, we report a rationally designed imidazole-based covalent organic framework (BI-TAPB-COF) that enables efficient iodine capture through synergistic charge-transfer interactions. The fully conjugated backbone endows the material with exceptional chemical and thermal stability, while the ordered pore channels and embedded electron-rich imidazole groups serve as Lewis basic sites to facilitate strong host-guest interactions with iodine molecules. As a result, BI-TAPB-COF achieves a high dynamic adsorption capacity of 0.402 g/g under demanding conditions (75 °C, 20 mL/min), outperforming commercial silver zeolite and silica gel. Mechanistic investigations reveal the formation of polyiodide anions (I3 and I5) via charge-transfer interactions.