Sorption of uranium on magnetite nanoparticles

Magnetite (Fe₃O₄) nanoparticle was synthesized using a solid state mechanochemical method and used for studying the sorption of uranium(VI) from aqueous solution onto the nanomaterial. The synthesized product is characterized using SEM, XRD and XPS. The particles were found to be largely agglomerated. XPS analysis showed that Fe(II)/Fe(III) ratio of the product is 0.58. Sorption of uranium on the synthesized nanomaterials was studied as a function of various operational parameters such as pH, initial metal ion concentration, ionic strength and contact time. pH studies showed that uranium sorption on magnetite is maximum in neutral solution. Uranium sorption onto magnetite showed two step kinetics, an initial fast sorption completing in 4–6 h followed by a slow uptake extending to several days. XPS analysis of the nanoparticle after sorption of uranium showed presence of the reduced species U(IV) on the nanoparticle surface. Fe(II)/Fe(III) ratio of the nanoparticle after uranium sorption was found to be 0.48, lower than the initial value indicating that some of the ferrous ion might be oxidized in the presence of uranium(VI). Uranium sorption studies were also conducted with effluent from ammonium diuranate precipitation process having a uranium concentration of about 4 ppm. 42% removal was observed during 6 h of equilibration.     

Sorption of uranium (VI) species on zircon: structural investigation of the solid/solution interface

This work is an investigation of the mechanisms of interaction between uranium (VI) ions and zirconium silicate. The speciation of uranium (VI) sorbed on zircon was studied using four complementary techniques as probes of the local structure around the uranium atom: laser spectrofluorimetry, X-ray photoelectron spectroscopy (XPS), diffuse reflectance infrared Fourier-transformed (DRIFT) spectroscopy, and EXAFS spectroscopy. The sorption of uranyl on zirconium oxide was also studied to allow structural comparisons. Spectrofluorimetry and XPS results allowed an identification of the silicate sorption sites on the solid. These methods associated with spectrofluorimetry and DRIFT led to a characterization of the sorbed surface complexes, taking into account the influence of the nature of the background salt and of the pH on the structure of the U(VI) surface species. EXAFS measurements, either on air-dried samples or in situ, were then carried out on well-characterized samples and allowed identification of the sorption mechanism on zircon as the formation of an inner-sphere polydentate surface complex.     

Kinetics of sorption of uranium(VI) compounds with zirconium-silica nanosorbents

The kinetics of sorption of uranium(VI) compounds from sulfate and carbonate solutions using four samples of mesoporous zirconium-silica nanosorbents obtained by bitemplate (solubilization) synthesis was studied. The sorption equilibrium set-in time and the kinetic characteristics of sorption were shown to depend on the sorbent (its composition, specific surface area, dispersity, and pore size), the temperature, and the composition and pH of the solution from which uranium compounds are sorbed. The sorption kinetics was described by a first-order equation. The limiting stage of the process was found to be the external diffusion of uranium-containing particles to the sorbent surface.     

Adsorption behavior of uranium on polyvinyl alcohol-g-amidoxime: Physicochemical properties, kinetic and thermodynamic aspects

Amidoxime-based adsorbents are widely studied as the main adsorbent in the recovery of uranium from seawater.However,the adsorption rate and loading capacity of such adsorbents should be further improved due to the economic viability consideration.In this paper,polyvinyl alcohol functionalized with amidoxime(PVA-g-AO)has been prepared as a new adsorbent for uranium(Ⅵ)adsorption from aqueous solution.The physicochemical properties of PVA-g-AO were investigated using infrared spectroscopy(IR),scanning electron microscope(SEM),X-ray diffraction(XRD),and X-ray photoelectron spectroscopy(XPS).Results showed that the ligand monomers were successfully grafted onto the matrixes.The XRD and XPS analysis showed that uranium was adsorbed in metal ionic form rather than in crystal form.Uranyl(U(Ⅵ))adsorption properties onto PVA-g-AO were evaluated.The adsorption of U(Ⅵ)by PVA-g-AO was fast,with an equilibrium time of less than 50 min.Additionally the maximum adsorption capacity reached 42.84 mg/g at pH 4.0.     

Evaluation of sorption of uranium onto metakaolin using X-ray photoelectron and Raman spectroscopies

Metakaolin prepared from a natural clay mineral ore of aluminium kaolinite is a promising low cost and high activity aluminosilicate material that has been investigated for studying the sorption behavior of uranium. Here, metakaolin was characterized using X-ray photoelectron spectroscopy (XPS) and the effects of pH, contact time and initial metal ion concentration on its sorption behavior were studied. The sorption process was found to initially be rapid (∼60% at time 0 min) but became slower with time; equilibrium was established within 24 h (∼80% sorption). The data were applied to study the kinetics of the sorption process. The Langmuir and Dubinin-Radushkevich (D-R) sorption isotherms were used to describe partitioning behavior for the system at room temperature. The binding of metal ions was found to be pH dependent, with optimal sorption occurring at pH 5. The retained metal ions were eluted with 5 mL of 0.1 M HNO₃. Raman spectroscopy and XPS were used to evaluate the sorption mechanism of U(VI).     

Effect of various environmental factors on the adsorption of U(VI) onto biochar derived from rice straw

Herein, we used biochar pyrolyzed from rice straw to adsorb uranium (U) from aqueous solutions. The adsorption of U(VI) on biochar was strongly dependent on pH but independent on ionic strength. HA/FA enhanced the sorption at pH <6.8 while inhibited the sorption at pH >6.8. The sorption reached equilibrium within 3 h, which was not mediated by pH. The adsorption process was spontaneous and endothermic, and enhanced at higher temperature. However, the influence of temperature was negligible at low initial U(VI) concentrations. Therefore, biochar derived from rice straw may be a promising adsorbent for the removal of U(VI).

     

Adsorptive removal of U(VI) from aqueous solution by hydrothermal carbon spheres with phosphate group

The phosphorylated hydrothermal carbon spheres (HCS-PO₄) were developed by functionalizing hydrothermal carbon spheres (HCS) with o-phosphoethanolamine, and the structure and textural property were characterized by SEM and FT-IR. The parameters that affect the uranium(VI) sorption, such as solution pH, initial U(VI) concentration, contact time, and temperature, had been investigated. The HCS-PO₄ showed the highest uranium sorption capacity at initial pH 6.0 and contact time of 120 min. The adsorption kinetics was better described by the pseudo-second-order model, and the adsorption process could be well defined by the Langmuir isotherm and the maximum monolayer adsorption capacity increased from 80.00 to 434.78 mg/g after phosphorylation. The thermodynamic parameters, ?G° (298 K), ?H° and ?S°, demonstrated shown that the sorption process of U(VI) onto HCS-PO₄ was feasible, spontaneous and endothermic in nature. The spent HCS-PO₄ could be effectively regenerated by 0.1 mol/L EDTA solution for the removal and recovery of U(VI) and reused for ten cycles at least. Selective adsorption studies showed that the HCS-PO₄ could selectively remove U(VI), and the selectivity coefficients of HCS in the presence of co-existing ions, Mg(II), Na(I), Zn(II), Mn(II),Co(II), Ni(II), Sr(II), Cs(I) and Hg(II) improved after functionalization.     

Removal of uranium(VI) from aqueous solution using sponge iron

Direct reduced iron (DRI), also called sponge iron, was used for the removal of U(VI) from aqueous solution. Batch experiments were conducted to evaluate the effect of various factors including contact time, solution pH, DRI dosage and initial uranium concentration on this removal process. The result suggested that U(VI) can be rapidly removed by DRI and this removal process followed an apparent first-order reaction kinetics. The optimum pH for uranium removal was between 2.0 and 4.0. Whether U(VI) can be fully removed was influenced by the molar ratio of DRI to U(VI) in solution. The aqueous U(VI) can be removed completely when this ratio was more than ca. 1,000. The U(VI) removal capacities of DRI decreased with increasing DRI dosages at a constant concentration of U(VI), but increased almost linearly with increasing initial U(VI) concentrations at a fixed dosage of DRI. The maximum U(VI) removal capacity was 5.71 mg/g DRI. Finally, the possible mechanism of U(VI) removal by DRI was also discussed. The XPS and XRD analysis showed that U(VI) was deposited as UO₃ onto DRI surface, indicating that U(VI) can be removed without reduction.     

Adsorption of uranium from aqueous solution using HDTMA+-pillared bentonite: isotherm, kinetic and thermodynamic aspects

The ability of hexadecyltrimethylammonium cation pillared bentonite (HDTMA⁺-bentonite) has been explored for the removal and recovery of uranium from aqueous solutions. The adsorbent was characterized using small-angle X-ray diffraction, high resolution transmission electron microscopy, and Fourier transform infrared spectroscopy. The influences of different experimental parameters such as solution pH, initial uranium concentration, contact time, dosage and temperature on adsorption were investigated. The HDTMA⁺-bentonite exhibited the highest uranium sorption capacity at initial pH of 6.0 and at 80?min. Adsorption kinetics was better described by the pseudo-second-order model and adsorption process could be well defined by the Langmuir isotherm. The thermodynamic parameters, ??G° (308?K), ??H°, and ??S° were determined to be ?31.64, ?83.84?kJ/mol, and ?169.49?J/mol/K, respectively, which demonstrated the sorption process of HDTMA⁺-bentonite towards U(VI) was feasible, spontaneous, and exothermic in nature. The adsorption on HDTMA⁺-bentonite was more favor than Na-bentonite, in addition the saturated monolayer sorption capacity increased from 65.02 to 106.38?mg/g at 298?K after HDTMA⁺ pillaring. Complete removal (??100%) of U(VI) from 1.0?L simulated nuclear industry wastewater containing 10.0?mg U(VI) ions was possible with 1.5?g HDTMA⁺-bentonite.     

Enhanced adsorption of arsenate on the aminated fibers: sorption behavior and uptake mechanism

Novel aminated polyacrylonitrile fibers (APANFs) were prepared through the reaction of polyacrylonitrile fibers (PANFs) with four multinitrogen-containing aminating reagents, and the best adsorbent was obtained after the optimization of preparation experiments. The APANFs were effective for arsenate removal from aqueous solution, and the sorption behaviors including kinetics, isotherms, effect of pH, and competitive anions were investigated. Experimental results show that the equilibrium of arsenate sorption on the fibers was achieved within 1 h, and Langmuir equation described the sorption isotherms well with a high sorption capacity of 256.1 mg/g obtained. The thermodynamic parameters calculated show that the sorption was spontaneous and exothermic under the condition applied. The zero point of zeta potential of the APANFs was at about pH = 8.2, in contrast with that of the PANFs at pH = 3.6. Fourier transform infrared (FTIR) and X-ray photoelectron spectroscopy (XPS) for the APANFs before and after arsenate adsorption revealed that the amine groups on the fiber surface played an important role in the removal of arsenate from water, attributed to the electrostatic interaction between the positive protonated amine groups and negative arsenate ions.     

Synthesis of ordered mesoporous carbonaceous materials and their highly efficient capture of uranium from solutions

An extremely effortless method was applied for successful synthesis of mesoporous carbonaceous materials(MCMs) using well-ordered mesoporous silica as template. Various characterizations(scanning electron microscopy(SEM), transmission electron microscopy(TEM), X-ray diffraction(XRD), Fourier transform infrared spectroscopy(FT-IR), Raman, X-ray photoelectron spectroscopy(XPS), Brunner-Emmet-Teller(BET) and Zeta potential) confirmed that MCMs had large surface area, uniform pore size distribution, and abundant oxygen-containing functional groups. The batch techniques were employed to study U(VI) adsorption on MCMs under a wide range of experiment conditions. The adsorption kinetics of U(VI) onto MCMs were well-fitted by pseudo-second-order kinetic model, indicating a chemisorption process. The excellent adsorption capacity of MCMs calculated from the Langmuir model was 293.95 mg g~(-1) at pH 4.0. The FT-IR and XPS analyses further evidenced that the binding of U(VI) onto MCMs was ascribed to the plentiful adsorption sites(–OH and –COOH groups) in the internal mesoporous structure, which could efficiently trap guest U(VI) ions. The results presented herein revealed that MCMs were ideal adsorbents in the efficient elimination of uranium or other lanthanides/actinides from aqueous solutions, which would play an important role in environmental pollution management application.     

Sorption study of uranium on carbon spheres hydrothermal synthesized with glucose from aqueous solution

The ability of oxygen-rich carbon spheres (CSs) produced by hydrothermal carbonization with the glucose has been explored for the removal and recovery of uranium from aqueous solutions. The micro-morphology and structure of CSs were characterized by FT-IR and SEM. The influences of different experimental parameters such as solution pH, initial concentration, contact time, ionic strength and temperature on adsorption were investigated. The CSs showed the highest uranium sorption capacity at initial pH of 6.0 and contact time of 25 min. Adsorption kinetics was better described by the pseudo-second-order model and adsorption process could be well defined by the Langmuir isotherm. The thermodynamic parameters, △G°(298 K), △H° and △S° were determined to be ?16.88, 12.09 kJ mol^?1 and 197.87 J mol^?1 K^?1, respectively, which demonstrated the sorption process of CSs towards U(VI) was feasible, spontaneous and endothermic in nature. The adsorbed CSs could be effectively regenerated by 0.05 mol/L HCl solution for the removal and recovery of U(VI). Complete removal (99.9 %) of U(VI) from 1.0 L industry wastewater containing 15.0 mg U(VI) ions was possible with 3.0 g CSs.     

Adsorption of uranium from aqueous solution using biochar produced by hydrothermal carbonization

The ability of biochar produced by hydrothermal carbonization (HTC) has been explored for the removal and recovery of uranium from aqueous solutions. The micro-morphology and structure of HTC were characterized by Fourier transform infrared spectroscopy and scanning electron microscopy. The influences of different experimental parameters such as solution pH, initial concentration, contact time, ionic strength and temperature on adsorption were investigated. The HTC showed the highest uranium sorption capacity at initial pH of 6.0 and contact time of 50 min. Adsorption kinetics was better described by the pseudo-second-order model and adsorption process could be well defined by the Langmuir isotherm. The thermodynamic parameters, △G°(298 K), △H° and △S° were determined to be ?14.4, 36.1 kJ mol^?1 and 169.7 J mol^?1 K^?1, respectively, which demonstrated the sorption process of HTC towards U(VI) was feasible, spontaneous and endothermic in nature. The adsorbed HTC could be effectively regenerated by 0.05 mol/L HCl solution for the removal and recovery of U(VI). Complete removal (99.9 %) of U(VI) from 1.0 L industry wastewater containing 15.0 mg U(VI) ions was possible with 2.0 g HTC.     

Effects of sulfate ligand on uranyl carbonato surface species on ferrihydrite surfaces

Understanding uranium (U) sorption processes in permeable reactive barriers (PRB) are critical in modeling reactive transport for evaluating PRB performance at the Fry Canyon demonstration site in Utah, USA. To gain insight into the U sequestration mechanism in the amorphous ferric oxyhydroxide (AFO)-coated gravel PRB, U(VI) sorption processes on ferrihydrite surfaces were studied in 0.01 M Na(2)SO(4) solutions to simulate the major chemical composition of U-contaminated groundwater (i.e., [SO(4)(2-)] ~13 mM L(-1)) at the site. Uranyl sorption was greater at pH 7.5 than that at pH 4 in both air- and 2% pCO(2)-equilibrated systems. While there were negligible effects of sulfate ligands on the pH-dependent U(VI) sorption (<24 h) in both systems, X-ray absorption spectroscopy (XAS) analysis showed sulfate ligand associated U(VI) surface species at the ferrihydrite-water interface. In air-equilibrated systems, binary and mono-sulfate U(VI) ternary surface species co-existed at pH 5.43. At pH 6.55-7.83, a mixture of mono-sulfate and bis-carbonato U(VI) ternary surface species became more important. At 2% pCO(2), there was no contribution of sulfate ligands on the U(VI) ternary surface species. Instead, a mixture of bis-carbonato inner-sphere (38%) and tris-carbonato outer-sphere U(VI) ternary surface species (62%) was found at pH 7.62. The study suggests that the competitive ligand (bicarbonate and sulfate) coordination on U(VI) surface species might be important in evaluating the U solid-state speciation in the AFO PRB at the study site where pCO(2) fluctuates between 1 and 2 pCO(2)%.     

Adsorption of uranium(VI) from aqueous solution by diethylenetriamine-functionalized magnetic chitosan

In this paper, the modified magnetic chitosan resin containing diethylenetriamine functional groups (DETA-MCS) was used for the adsorption of uranium ions from aqueous solutions. The influence of experimental conditions such as contact time, pH value and initial uranium(VI) concentration was studied. The Langmuir, Freundlich, Sips and Dubinin–Radushkevich equations were used to check the fitting of adsorption data to the equilibrium isotherm. The best fit for U(VI) was obtained with the Sips model. Adsorption kinetics data were tested using pseudo-first-order and pseudo-second-order models. Kinetic studies showed that the adsorption followed the pseudo-second-order kinetic model, indicating that the chemical adsorption was the rate-limiting step. The present results suggest that DETA-MCS is an adsorbent for the efficient removal of uranium(VI) from aqueous solution.     

Biosorption characteristics of uranium(VI) from aqueous solution by pummelo peel

The biomass pummelo peel was chosen as a biosorbent for removal of uranium(VI) from aqueous solution. The feasibility of adsorption of U(VI) by Pummelo peel was studied with batch adsorption experiments. The effects of contact time, biosorbent dosage and pH on adsorption capacity were investigated in detail. The pummelo peel exhibited the highest U(VI) sorption capacity 270.71?mg/g at an initial pH of 5.5, concentration of 50???g/mL, temperature 303?K and contacting time 7?h. The adsorption process of U(VI) was found to follow the pseudo-second-order kinetic equation. The adsorption isotherm study indicated that it followed both the Langmuir adsorption isotherm and the Freundlich adsorption isotherm. The thermodynamic parameters values calculated clearly indicated that the adsorption process was feasible, spontaneous and endothermic in nature. These properties show that the pummelo peel has potential application in the removal of the uranium(VI) from the radioactive waste water.     

纳米四氧化三铁表面酸碱性质研究

制备了纳米Fe3O4, 并对其进行了表征和表面酸碱行为研究. 实验结果表明, Fe3O4表面在水溶液中有非常明显的酸碱性质. 随着纳米Fe3O4加入量的增多, 溶液pH缓冲能力增强, 二者之间成正比, 据此可定量地测定H+在纳米氧化铁表面的吸附量. 运用MEDUSA和WINSGW计算软件计算了表面组分在溶液中的分布， 并讨论了表面电荷对表面组分分布的影响.     

Uranium (VI) adsorption equilibrium on purolite resin SGA 600 U/3472

This paper characterizes uranium (VI) sorption from synthetic solutions using a fixed bed Purolite resin SGA 600 U/3472 system. The effect of the sulphate anion presence in the liquid phase on sorbtion dynamics and equilibrium is analysed. In the industrial processing of solutions obtained from leaching of uranium ore (alkaline/acid), in a continuous system, there are several compounds which strongly compete with uranium for ion exchange sites and consequently these substances depress the uranium adsorption. The influence of vanadate, molybdate, chloride, and nitrate is known, therefore, in this paper, the adsorption equilibrium isotherms for uranium (VI) are obtained for different sulphate ion concentrations in solution. The adsorption capacity variation of the Purolite resin SGA 600U/3472 with the number of adsorption/desorption cycles is also studied. The experimental results reveal the negative impact of high sulphate ion content in solution on the adsorption capacity of the resin Purolite SG 600 U / 3472 with uranium (VI) and therefore it is considered one of the compounds which strongly affect the uranium adsorption.

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Sorption behaviour of uranium(VI) with N,N-dibutyl-N'-benzoylthiourea Impregnated in Amberlite XAD-16

The sorption of U(VI) by N, N-dibutyl, N'-benzoylthiourea (DBBT) impregnated resin has been studied. DBBT impregnated resin was prepared by direct adsorption of chelating ligand onto macroporous support, Amberlite XAD-16. The adsorption of DBBT on the macroporous support is shown by FTIR spectroscopy to be the result of only weak chelating ligand-support interactions. Parameters such as the pH effect on the sorption of uranium, the sorption capacity of the impregnated resin, the stripping of uranium and the effect of coexisting ions were investigated by batch experiments. The results demonstrated that uranium(VI) ions, at pH 4.5-7 could be sorbed completely using 0.1 g Amberlite XAD-16 resin loaded with DBBT. The sorption capacity of the impregnated resin is 0.90 mmol uranium(VI) g(-1). Quantitative recovery of U(VI) is achieved by stripping with 0.1 M HNO(3). The method was applied to the determination of uranium in synthetic samples. The precision of the method was 2.4 RSD% in a concentration of 1.20 mug ml(-1) for ten replicate analysis.