The leakage of iodine and its radioactive isotopes poses a major threat to ecosystems and human health, emphasizing the need for effective and recyclable iodine capture materials. Covalent organic frameworks (COFs), characterized by high surface areas, tunable pore sizes, and excellent chemical stability, are ideal candidates for adsorption applications. Herein, two novel COFs (JUC-700 and JUC-701) are designed and synthesized based on benzotrithiophene (BTT). Both JUC-700 and JUC-701 exhibit high surface areas (2004.9 and 1990.5 m² g^-1, respectively), mesoporous structures (≈2.6 nm), and abundant heteroatoms, contributing to their exceptional iodine capture performance. Notably, JUC-701 demonstrates superior adsorption capacity (6.17 g g^-1) compared to JUC-700 (4.73 g g^-1), attributes to the enhanced iodine affinity near its pyridine groups. Theoretical calculations further reveal that the pyridinic nitrogen in JUC-701 significantly strengthens interactions with iodine molecules, confirming its superior capture capabilities. This study provides insights into the design of functionalized COFs for iodine capture, contributing to advanced materials for environmental remediation and nuclear waste management.

Keywords: covalent organic frameworks; high surface area; iodine adsorption; porous materials.

© 2025 Wiley‐VCH GmbH.

碘和其放射性同位素的泄漏对生态系统和人类健康构成重大威胁，强调了开发有效且可回收的碘捕获材料的需求。共价有机框架（COFs）因其高比表面积、可调孔径大小和出色的化学稳定性而成为吸附应用的理想候选者。在此，基于苯并三噻吩（BTT），设计合成了两种新型COF（JUC-700和JUC-701）。这两种材料均表现出高的比表面积（分别为2004.9 和 1990.5 m²/g）、介孔结构（≈2.6 nm）以及丰富的杂原子，这些特性有助于其优异的碘捕获性能。值得注意的是，JUC-701的吸附能力优于JUC-700（分别为6.17 g/g 和 4.73 g/g），这归因于其吡啶基团附近对碘分子增强的亲和力。理论计算进一步揭示了JUC-701中的吡啶氮显著增强了与碘分子的相互作用，证实了它的卓越捕获能力。本研究为设计用于碘捕获的功能化COF提供了见解，并为环境修复和核废料管理领域开发先进材料做出了贡献。

关键词：共价有机框架；高比表面积；碘吸附；多孔材料。