Abstract
The vitrification process represents an effective method for high-level radioactive waste disposal, but CrO42- can form crystalline spinels within the glass to cause the secondary leak of radioactive waste. Porous materials are widely used for trapping CrO42-, but the unsatisfied adsorbing capacity and poor selectivity of reported materials make CrO42- enrichment to be a challenging issue. Herein, a rarely hollow single-crystalline MOF (1) with ordered macro-micropores of 13 μm and 8.6 Å was obtained, exhibiting high N2 adsorption of 339.2 cm3/g and large BET surface area of 1150 m2/g. Cooperation effect between microporous frameworks and micron-sized channels in crystals endows 1 with excellent chromate removal capacity of 609 mg/g, which is a record value known to date among the anion-exchange materials for CrO42- removal. The kinetic analysis revealed that such adsorption was a pseudo-second-order adsorption process. Framework 1 possessed high pH stability and irradiation resistance, can repeatedly absorb/desorb CrO42- to some degree. More importantly, sample 1 can maintain its high CrO42- adsorption capacity after 400 kGy β irradiation, offering the promising application for CrO42- disposal in high-level radioactive waste.
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