RESUMO
Nanoscale zerovalent iron (Fe0)-based materials have been demonstrated to be a effective method for the U(VI) removal. However, limited research has been conducted on the long-term immobilization efficiency and mechanism of Fe0-based materials for U(VI), which are essential for achieving safe handling and disposal of U(VI) on a large scale. In this study, the prepared carboxymethyl cellulose (CMC) and sulfurization dual stabilized Fe0 (CMC-Fe0/FeS) exhibited excellent long-term immobilization performances for U(VI) under both anoxic and oxic conditions, with the immobilization efficiencies were respectively reached over 98.0 % and 94.8 % after 180 days of aging. Most importantly, different from the immobilization mechanisms of the fresh CMC-Fe0/FeS for U(VI) (the adsorption effect of -COOH and -OH groups, coordination effect with sulfur species, as well as reduction effect of Fe0), the re-mobilized U(VI) were finally re-immobilized by the formed FeOOH and Fe3O4 on the aged CMC-Fe0/FeS. Under anoxic conditions, more Fe3O4 was produced, which may be the main reason for the long-term immobilization U(VI). Under oxic conditions, the production of Fe3O4 and FeOOH were relatively high, which both played significant roles in re-immobilizing U(VI) through surface complexation, reduction and incorporation effects.
Assuntos
Urânio , Carboximetilcelulose Sódica , Ferro , AdsorçãoRESUMO
As an emerging versatile technology for separating uranium from uranium-containing wastewater (UCW), microbial fuel cell (MFC) offers a novel approach to UCW treatment. Its cathode is essential for the treatment of UCW. To thoroughly investigate the efficacy of MFC in treating UCW, investigations were conducted using MFCs with five materials (containing iron sheet (IP), stainless steel mesh (SSM), carbon cloth (CC), carbon brush (CB), and nickel foam (NF)) as cathodes. The results revealed that each MFC system performed differently in terms of carbon source degradation, uranium removal, and electricity production. In terms of carbon source degradation, CB-MFC showed the best performance. The best uranium removal method was NF-MFC, and the best electricity production method was carbon-based cathode MFC. Five MFC systems demonstrated stable performance and consistent difference over five cycles, with CC-MFC outperforming the others. Furthermore, SEM and XPS characterization of the cathode materials before and after the experiment revealed that a significant amount of U(IV) was generated during the uranium removal process, indicating that uranium ions were primarily removed by electrochemical reduction precipitation. This study confirmed that abiotic cathode MFC had a high UCW removal potential and served as a good guideline for obtaining the best cathode for MFC.
Assuntos
Fontes de Energia Bioelétrica , Urânio , Águas Residuárias , Eletricidade , Carbono , Eletrodos , NíquelRESUMO
Reduction of the migratory ability of uranium via reduction, co-precipitation or immobilization is a widely used technology for remediation of uranium contaminated groundwater (UCG). However, the re-released uranium due to environmental alterations such as oxidation, acid dissolution, or microbial decomposition limits the long-term effect of UCG remediation. Here, we developed a novel solar-powered electrochemical mineralization (SPEM) system for persistent remediation of UCG under laboratory conditions. The SPEM system incorporates uranium into magnetite crystal to achieve long-term stability of uranium. The effects of photoelectric conversion, subsurface void fraction, groundwater seepage velocity, and electrode configuration on uranium removal were systematically analyzed. The results showed that the remediation system had excellent adaptability to complex water quality and geological conditions, and could remediate large-area contamination. After 12 h of persistent treatment, the system with newly hexagonal two-dimensional electrode configuration (1A6C) reduced uranium concentration by more than 85% in simulated subsurface environment. The mineralized uranium was not re-released within continuous rinsing of treated regions using an acid solution (pH = 3.0), for 370 h. The developed method solely requires metallic iron as a raw material, which has high and long-term efficiency, is eco-friendly, simple, and widely applicable, thus reliable for the remediation of deep UCG.
Assuntos
Recuperação e Remediação Ambiental , Água Subterrânea , Monitoramento de Radiação , Urânio , Poluentes Radioativos da Água , Água Subterrânea/química , Ferro/química , Urânio/análise , Poluentes Radioativos da Água/análiseRESUMO
Iron-based materials have been widely used for treating uranium-containing wastewater. However, the iron-uranium solids originating by treating radioactive water through pollutant transfer methods has become a new uncontrolled source of persistent radioactive pollution. The safe disposal of such hazardous waste is not yet well-resolved. The electrochemical mineralization method was developed to rapidly purify uranium-containing wastewater through lattice doping in magnetite and recover uranium without generating any pollutants. An unexpected isolation of U3O8 from uranium-doped magnetite was discovered through in-situ XRD with a temperature variation from 300 °C to 700 °C. Through HRTEM and DFT calculation, it was confirmed that the destruction of the inverse spinel crystal structure during the gradual transformation of magnetite into γ-Fe2O3 and α-Fe2O3 promoted the migration, aggregation, and isolation of uranium atoms. Uniquely generated U3O8 and Fe2O3 were easily separated and over 80% uranium and 99.5% iron could be recovered. These results demonstrate a new strategy for uranium utilization and the environmentally friendly treatment of uranium-containing wastewater.