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Abstract  

The complexation of technetium with humic acid is usually done by a reduction of pertechnetate by Sn2+ ions. A Tc-HA complex can be scavenged in a Sn-HA complex, if tin is present as reductant. The main aim of the study was a preparation of the Tc-HA complex without impurities of Sn ions or other metal reductant, which was performed by a ligand exchange with hexakis(thiourea-S)technetium(III) under nitrogen atmosphere at pH 5.5. The [Tc(tu)6]3+ complex was prepared from TcO4 - in acidic solution with thiourea as a reductant. Presence of the Tc-HA complex and other technetium species was determined by gel chromatography, paper chromatography and dialysis. Yield of Tc-HA complex was about 80% and reaction mixture contains about 20% of technetium dioxide, which is a side product of ligand-exchange.

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The thermal behaviour of humic acids and their sodium salts in oxygen has been studied. The sodium humates were prepared by neutralization of humic acids or by dialysis of their pseudosolutions in sodium hydroxide. Infrared and X-ray diffraction spectra of samples taken between the dissociation steps obtained from the DTA-TG-DTG curves suggest a double mechanism. Below 500°, sodium carbonate and carbon are formed. At 600°, the dissociation of carbonate starts. The residual carbon burns at once at 770°. The extent of reaction changes with the amount of sodium initially present.

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Abstract  

A landfill leachate sample was radiolyzed with γ-rays at 12.5, 25, 50, 100, 200 and 400 kGy. The radiolyzed solutions were studied by UV–VIS–NIR spectroscopy to measure the color change, by chemical oxygen demand (COD) analysis to check the degree of mineralization of the soluble organic matter present in the leachate and by FT–IR spectroscopy of the humic substance of the leachate. The results have shown that the humic substance present in the landfill leachate is extremely refractory to radiolysis: even at 400 kGy it was detected and recovered only with minor changes. It is shown that the radiolysis followed by ozonolysis is able to cause important improvements of the leachate color and important reduction on the COD. However, the results in terms of bleaching and COD abatement after radiolysis and ozonolysis of the leachate can be achieved directly by a simple exhaustive ozonolysis of the leachate. The structural changes occurring in the humic substances and in the humic acids present in the leachate after radiolysis and ozonolysis were analyzed by FT–IR spectroscopy.

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Abstract  

The sorption of radiocadmium on Ca-montmorillonite as a function of contact time, pH, ionic strength, foreign ions, humic acid (HA) and fulvic acid (FA) was studied using batch technique. The results demonstrated that the sorption of Cd(II) was dependent on ionic strength at pH < 9, and was independent of ionic strength at pH > 9. Outer-sphere surface complexation and/or ion exchange were the main mechanism of Cd(II) sorption on Ca-montmorillonite at low pH, whereas the sorption at high pH was mainly dominated via inner-sphere surface complexation. The sorption of Cd(II) on Ca-montmorillonite was dependent on foreign ions at low pH values, but was independent of foreign ions at high pH values. A positive effect of HA/FA on Cd(II) sorption was found at low pH values, whereas a negative effect was observed at high pH values. The thermodynamic parameters (i.e., ΔH 0, ΔS 0, ΔG 0) were calculated from the temperature dependent sorption isotherms, and the results indicated that the sorption process of Cd(II) on Ca-montmorillonite was spontaneous and endothermic.

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Abstract  

Herein, the sorption properties of Eu(III) on Na-attapulgite were performed by using batch sorption experiments under different experimental conditions, such as contact time, pH, ionic strength, humic acid and temperatures. The results indicated that the sorption of Eu(III) on Na-attapulgite was strongly dependent on pH and temperature. At low pH values, the sorption of Eu(III) was influenced by ionic strength, whereas the sorption was not affected by ionic strength at high pH values. The sorption of Eu(III) was mainly dominated by ion exchange or outer-sphere surface complexation at low pH values, and by inner-sphere surface complexation or surface precipitation at high pH values. The sorption of Eu(III) onto Na-attapulgite increased with increasing temperature. The Langmuir and Freundlich models were applied to simulate the sorption isotherms, and the results indicated that the Langmuir model simulated the sorption isotherms better than the Freundlich model. The thermodynamic parameters (∆G o, ∆S o, ∆H o) were calculated from the temperature dependent sorption isotherms at 293, 313 and 333 K, respectively, and the results indicated that the uptake of Eu(III) on Na-attapulgite was an endothermic and spontaneous process. The results of high Eu(III) sorption capacity on Na-attapulgite suggest that the attapulgite is a suitable material for the preconcentration and immobilization of Eu(III) ions from large volumes of aqueous solutions.

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Abstract  

The ammonium citrate tribasic was successfully modified to attapulgite clay and the effect of modifying was characterized by FTIR and XRD techniques. Experimental results showed that the ammonium citrate tribasic modified attapulgite clay had a strong sorption ability to remove Th(IV) from aqueous solutions. The sorption of Th(IV) from aqueous solutions has been systematically investigated as a function of several variables including contact time, solid content, pH, ionic strength, Fulvic acid (FA)/humic acid (HA) and temperature under ambient conditions. The results indicate that the sorption of Th(IV) onto ammonium citrate tribasic modified attapulgite clay is strongly dependent on pH, Th(IV) initial concentration, ionic strength, temperature and HA/FA. Surface complexation and ionic exchange are the main sorption mechanisms. Sorption of Th(IV) onto ammonium citrate tribasic modified attapulgite is quick and can be fitted by a pseudo-second-order rate model very well. Sorption of Th(IV) onto ammonium citrate tribasic modified attapulgite is promoted at higher temperature and the sorption reaction is an endothermic process. Langmuir isotherm model fits the experimental data better than Freundlich and D-R isotherm models. The results suggest that the ammonium citrate tribasic modified attapulgite sample is a suitable material in the preconcentration and solidification of radionuclide Th(IV) from large volumes of aqueous solutions.

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Abstract  

During this work highly particle reactive nature of thorium was exploited for the separation of Th from aquatic stream containing U/Th. The Kd value of Th(IV) ions is 106 which is two order of magnitude higher than uranium (IV & VI). Laboratory simulated experiments were conducted to study the preferential removal of thorium by using siliceous material having particle size of about 2,000 μm. Siliceous material was prepared by decomposing the organic layer on soil particles by giving treatment with HNO3 and H2O2. Experimental solutions were generated by spiking the surface water with Th (NO3)4 and UO2(NO3)2. Experimental results shows preferential uptake of Th compared to U by siliceous material. This association is further improved by coating the siliceous material with high and low molecular weight organic materials i.e. humic and fulvic acid, respectively. Characterization of the organic material was done by ATR–FTIR whereas determination of Th was done by ICP-OES and alpha spectrometry. Experimental results clearly showed that Th and U sorption capacity is 1 and 0.3 μg mg−1 (w/w), respectively, in case of siliceous material. Thorium sorption is increased five and eight times in the case of coating with fulvic acid and humic acid, respectively. Whereas the same does not shows any pronounced impact on sorption of uranium.

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Abstract  

The migration of radionuclides with groundwater into the environment of a radioactive waste repository is an important aspect in evaluating the safety assessment of such repositories. The potential transport and fate of these radioactive species are dependent upon their speciation and the geochemical behavior of the predominant ones. The speciation of different valence states of neptunium [Np(IV, V and VI)] and their migration behavior are investigated. The data revealed that the uptake is highly dependent upon pH and the distribution coefficient (K d) is depressed by the presence of organic ligands. The relative migration velocities (V n) of the valence states relative to that of groundwater, in the concerned area, clarified that Np(V) is the most mobile species and their transport rates are highly accelerated by the presence of humic acid. Also, a radionuclide dispersion model was applied to elucidate the migration behavior of these radioactive species in the selected site and to quantitatively predict their concentrations at different distances in both x and z directions over long time scales.

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Abstract  

The aim of this study is to compare different resins regarding their separation and pre-concentration efficiency for uranium from aqueous solutions and its subsequent radiometric determination by liquid scintillation counting (LSC). The different types of the investigated resins include: (a) a pure cation-exchange resin (Dowex Marathon C), (b) a complex forming resin (Chelex 100) and (c) an impregnated resin (5% diethylene glycol succinate on Chromosorb W-H). The radiometric measurements were performed after mixing of the pre-concentrated aqueous phase with the liquid scintillation cocktail. The effect of experimental conditions such as pH, salinity (e.g. [NaCl]) and the presence of other chemical species (e.g. Ca2+ and Fe3+ ions or humic acid and silica colloids) on the separation recovery have been investigated at constant uranium/radioactivity concentration. According to the experimental results the maximum chemical recovery differs significantly from one resin to another as a function of either, pH or the other chemical parameters. The optimum pH is found to be 8, 4 and 8 for Marathon C, Chelex-100 and diethylene glycol succinate, respectively. On the other hand, generally Ca2+ and Fe3+ ions as well as the presence of colloidal species in solution (even at low concentrations) result in a significant decrease of the chemical recovery of uranium, particularly for Marathon C and the diethylene glycol succinate impregnated resins. Generally, among the studied resins Chelex 100 was superior regarding chemical recovery, selectivity, regeneration and reuse.

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Abstract  

The sorption of Co(II) on Na-montmorillonite was conducted under various conditions, i.e., contact time, adsorbent dosage, pH, ionic strength, foreign ions, fulvic acid (FA), humic acid (HA) and temperature. Results of sorption data analysis indicated the sorption of cobalt on Na-montmorillonite was strongly dependent on pH and ionic strength. At low pH, the sorption of Co(II) was dominated by outer-sphere surface complexation and ion exchange with Na+/H+ on Na-montmorillonite, whereas inner-sphere surface complexation was the main sorption mechanism at high pH. The presence of different cations influenced Co(II) sorption, while the presence of different anions had no differentiable influences on Co(II) sorption. The presence of HA and FA decreased the sorption of Co(II) on montmorillonite. The sorption isotherms are simulated well with the Langmuir model. The thermodynamic parameters (ΔH°, ΔS° and ΔG°) calculated from the temperature dependent isotherms indicated that the sorption reaction of Co(II) on montmorillonite was an endothermic and spontaneous process. The sorption test revealed that the low cost material was a suitable material in the preconcentration of Co(II) from large volumes of aqueous solutions.

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