吸附
金属有机骨架
碘
金属
化学
组合化学
纳米技术
材料科学
化学工程
有机化学
工程类
作者
Zi‐Jian Li,Juejing Liu,Guangtao Zhang,Chris J. Benmore,Linjuan Zhang,Xiao‐Feng Guo,Jian Lin
标识
DOI:10.1016/j.cej.2024.156586
摘要
• An unprecedented positional isomerism strategy to enhance the iodine adsorption capacity of MOFs is introduced. • Ortho -amino substitution is more effective in boosting iodine adsorption compared to meta -amino substitution. • Th-UiO-68-3,3”-(NH 2 ) 2 achieves an iodine vapor adsorption capacity of 2.042 g/g. Porous metal–organic frameworks (MOFs) have emerged as highly promising adsorbents for capturing radioiodine, a predominant fission product released during nuclear fuel reprocessing. However, systematic investigations into the correlation between MOF structure and iodine uptake capacity remain scarce. Here, we present a novel approach to enhancing the iodine adsorption capacity of MOFs by optimizing linker functionalization. Using ligand-functionalized thorium-based MOFs as a structural platform, we demonstrate that ortho -amino-substitution near the node of the dicarboxylate linker significantly increases iodine adsorption capacity compared to meta -amino-substitution, where the amino groups are directed away from the node. Specifically, ortho -substituted Th-UiO-68-3,3”-(NH 2 ) 2 exhibits higher iodine uptake capacities than the meta -substituted Th-UiO-68-2,2”-(NH 2 ) 2 via both vapor diffusion-based (2.042 vs. 1.087 g/g) and solution-based (0.841 vs. 0.784 g/g) processes. Notably, the I 2 vapor adsorption capacity (2.042 g/g) of Th-UiO-68-3,3”-(NH 2 ) 2 represents the second highest among all reported Th-MOFs. Pair distribution function (PDF) studies reveal that the superior iodine uptake performance of ortho -functionalized MOFs can be attributed to the reduced steric hindrance of the amino groups compared with the meta -substituted variants. This research highlights how positional isomerism and its subtle alterations can significantly influence host–guest interactions, extending beyond simple structural considerations.
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