Abstract
Nuclear power emerges as a beacon of hope in tackling the energy crisis. However, the emission of radioactive iodine originating from nuclear waste and accidents poses a serious danger to nature and human well-being. Therefore, it becomes imperative to urgently develop suitable adsorbents capable of iodine capture and long-term storage. It’s generally recognized that achieving high iodine capture efficiency necessitates the presence of electron-rich pores/cavities that facilitate charge-transfer (CT) interactions, as well as effective sorption sites capable of engaging in lone pair interactions with iodine. In this study, an unprecedented iodine capture paradigm by nonporous amorphous electron-deficient tetracationic cycloalkanes in vapor and aqueous solutions is revealed, overturning preconceived notions of iodine trapping materials. A newly reported tetracationic cyclophane, BPy-Box4+, exhibited an exceptional iodine vapor sorption capacity of 3.99 g g−1, remarkable iodine removal efficiency in aqueous media, and outstanding reusability. The iodine capture mechanism is unambiguously elucidated by theoretical calculations and the single-crystal structures of cyclophanes with a gradual increase in iodine content, underlining the vital role of host-guest (1:1 or 1:2) interactions for the enhanced iodine capture. The current study demonstrates a new paradigm for enhanced iodine capture by nonporous amorphous electron-deficient cyclophanes through host-guest complexation.
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