Zhiwei Li, Dan Zhou, Linwei He, Yingtong Fan, Sen Mei, Zhonglin Ma, S. H. Tang, Zhiyong Peng, Long Chen, Long Chen, Lin Zhu, Jinghang Wang, Baoyu Li, Lixi Chen, Lixi Chen, Chao Zhao, Hailong Zhang, Yanlong Wang, Shuao Wang
Immobilizing radioactive organic iodides (ROIs) is essential for radioactive-pollution remediation. However, conventional ROI sorbents often suffer from I – leakage, and the atomic-level mechanisms underlying ROI immobilization remain unclear. Herein, a reaction-induced postactivated nanotrap strategy is proposed for the leakage-resistant immobilization of trace-level methyl iodide. The nanotrap in a stable metal–organic framework ( SCU-365 ) undergoes in situ activation by methylation during chemisorption and then precisely confines the generated I –, which enables the crystallographic visualization of chemisorbed ROI for the first time. Structural and computational analyses reveal that the synergy of multiple weak interactions for I – complexation rivals the strength of a covalent bond, endowing SCU-365 with exceptional leakage resistance superior to that of state-of-the-art ROI sorbents. This work proposes a novel strategy for antileakage material design for nuclide sequestration and fills the gap of understanding how materials interact with ROI.