Insights into uranium sequestration by coal fly-ash-derived zeolites: Understanding via wet-chemistry, and advanced spectroscopies

The operation of nuclear power plants requires a supply of nuclear fuel where uranium plays a substantial role as a primary fissile material. Its extraction from U-bearing minerals and handling may cause a leakage of heavily toxic radioactive pollution, which ends up in water bodies and soil. Therefore, tackling U-contaminated water is crucial to preserve water integrity and quality. Zeolites are known as profound ion exchangers with great affinity towards cationic species present in polluted waters. Various zeolite synthesis routes have made this group of aluminosilicates even more promising to be applied as water purification materials. Here, the synthetic gismondite, faujasite, and Linde type-A zeolites from coal fly-ash were synthesized via tailored, coupled fusion-hydrothermal method and applied to remove aqueous uranium (primarily as 238U) under varying pH, time (sorption kinetics), and initial U concentrations (sorption isotherms). The maximum U uptake was observed for Na–P1 (GIS) zeolite, which equals 48.72 mg U/g, the highest reported value on maximum U adsorption capacity for zeolitic materials. The U adsorption kinetics showed that equilibrium is reached after approximately 3 h of adsorption and that the removal process follows a Freundlich isothermal model for all zeolites, thus preferential adsorption onto heterogeneous surfaces. Advanced spectroscopic studies, including laboratory-scale X-ray Photoelectron Spectroscopy with synchrotron light X-ray Absorption Near Edge Structure in High Energy Resolution Fluorescence Detection mode, revealed that at acidic pH, predominantly an ion exchange between Na+ ions with hexavalent uranyl species takes place. In contrast, in the neutral pH region, the U is immobilized via precipitation in the form of μm-scale mineral aggregates of Na-schoepite: Na(UO2)4O2(OH)55↓. The outcomes of the research study has demonstrated that synthetic zeolites, obtained from industrial by-products such as coal fly-ash, can be successfully valorized to efficient U adsorbents while unveiling the insights to understand the zeolites/U interactions at the nanoscale level.