Molecular Design and Functional Engineering of POPs and MOFs for Advanced Radioactive Iodine Sequestration

Abstract The accumulation of radioactive iodine in nuclear industry waste poses a serious threat to environmental and human health, necessitating highly efficient capture technologies. Porous organic polymers (POPs) and metal–organic frameworks (MOFs) have emerged as leading candidates due to their high surface areas, tunable pore structures, versatile chemistries, and robust thermal and chemical stabilities. This review provides a comprehensive overview of recent advances in tailoring POPs and MOFs for iodine capture. Key strategies include optimizing surface area and pore volume, incorporating heteroatom‐rich linkers and functional groups to create strong binding sites, and employing post‐synthetic modifications and composite architectures to enhance performance. The integration of computational modeling with experimental validation has accelerated the discovery of next‐generation adsorbents. Beyond uptake capacity, we discuss practical aspects critical for real‐world applications, including adsorption kinetics, recyclability, irradiation and thermal stability, and cost‐effectiveness. A comparative analysis of POPs and MOFs highlights their respective strengths and challenges, particularly regarding scalability and long‐term durability under nuclear waste conditions. Finally, we identify persisting gaps, notably limited understanding of radiolytic stability, and propose promising directions for future research. Collectively, this review summarizes current strategies and underscores the pivotal role of POPs and MOFs in advancing nuclear waste remediation.