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Safe confinement of fission iodine isotopes for long-term radioactive waste disposal remains a formidable challenge, as conventional sorbents provide inherently weak iodine-host interactions. We report here a novel halogen bond (X-bond) directed strategy to sequester volatile iodine in hydrogen-bonded (H-bonded) frameworks with unprecedented stability. Charge-assisted H-bonded frameworks bearing open halide sites are developed, showing distinctive iodine encapsulation behaviors without compromising the crystallinity. Direct crystallographic evidence indicates the formation of X-bonds, i.e., I–I···Cl− and I–I···Br−, within the confined pore channels. Unusual polyhalogen anions, i.e., [I2Cl2]2− and [I2Br2]2−, sustained in H-bonded frameworks are identified for the first time. The X-bond reinforced host-guest interaction affords robust iodine trapping without leaking out even at elevated temperatures up to 180 °C. By integrating the halogen-bond chemistry with H-bonded frameworks, this study offers fresh concepts for developing effective host reservoirs to secure fission iodine isotopes from spent fuel reprocessing off-gases.
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