Polyphosphonate-segmented macroporous organosilicon frameworks for efficient dynamic enrichment of uranium with in-situ regeneration

Efficient separation and enrichment of uranium from radioactive effluents is of strategic significance for sustainable development of nuclear energy and environmental protection. Macropore structure of adsorbent is conducive to accessibility of the pore and transport of the adsorbate during dynamic adsorption. However, the low specific surface area results in fewer ligand sites and subsequently reduces the adsorption capacity. Herein, we present a novel strategy for efficient dynamic uranium enrichment using polyphosphonate-segmented macroporous organosilicon frameworks (PMOFs). PMOFs are constructed through the copolymerization of diethyl vinylphosphonate and triethoxyvinylsilane, followed by hydrolysis and condensation of the oligomers. The introduction of polyphosphonate segments into the frameworks endows PMOFs with a macroporous structure (31 µm) and a high ligand content (up to 72 wt%). Consequently, the optimized PMOF-3 demonstrated an ultrahigh dynamic adsorption capacity of 114.8 mg/g among covalently conjugated silicon-based materials. Additionally, PMOF-3 achieves a high enrichment factor (120) in the dynamic enrichment of uranium on a fixed bed column, which can be in-situ regenerated with 1 M NaHCO3 as the eluent. This work presents a new strategy for efficient dynamic enrichment of nuclides, which can be extended to the separation of other specific pollutants, shedding new light on adsorbent design and technical innovation.