A novel carboxyl-functionalized metal-organic framework for highly efficient uranium sorption was prepared through a generic postsynthetic strategy, and this MOF's saturation sorption capacity is found to be as high as 314 mg·g-1. The preliminary application illustrated that the grafted free-standing carboxyl groups have notably enhanced the sorption of uranyl ions on MIL-101. In addition, we have performed molecular dynamics simulation combined with density functional theory calculations to investigate the molecular insights of uranyl ions binding on MOFs. The high selectivity and easy separation of the as-prepared material have shown tremendous potential for practical applications in the nuclear industry or radioactive water treatment, and the functionalized MOF can be extended readily upon the versatility of click chemistry. This work provides a facile and purposeful approach for developing MOFs toward a highly efficient and selective extraction of uranium(VI) in aqueous solution, and it further facilitates the structure-based design of nanomaterials for radionuclide-containing-medium pretreatment.
Keywords: DFT calculation; metal−organic frameworks; molecular dynamics simulation; postsynthetic strategy; radioactive water treatment; uranium extraction.