Pore Space Multi‐Layer Functionalization Boosting Industrial Radioactive Iodine Capture with Record Capacity and Exceptional Kinetics

Abstract Capturing radioactive molecular iodine (I 2 ) from nuclear waste under industrial conditions remains a considerable challenge. Herein, we developed for the first time a pore space multiple‐layer functionalization (PSMLF) strategy, which enables directionally distribute functional sites across the multi‐layer regions of large pore space, thereby enhancing the I 2 adsorption ability by optimizing pore space utilization. Utilizing this approach, the optimized adsorbent PAF‐1‐NTM achieves a record‐high I 2 uptake of 88.58 wt% under simulated industrial conditions (150 °C and 150 ppmv I 2 ), a 108‐fold improvement over its parent material, PAF‐1. This performance significantly surpasses that of industrial Ag@MOR and all previously benchmarked adsorbents under the same conditions. Furthermore, adsorption kinetic of PAF‐1‐NTM ( k 1 = 0.025 min −1 ) are significantly higher than those of all other porous adsorbents reported to date. These results thus establish PAF‐1‐NTM as a new benchmark for high‐temperature I 2 adsorbents. Mechanism investigation reveals a new insight that the I 2 adsorption capacity is positively correlated with the pore space utilization rate. Our work not only develops a promising adsorbent for industrial radioactive I 2 capture but also establishes a general design principle for creating high‐temperature I 2 adsorbents suitable for practical applications.