Sequestration of radioactive nickel in fly ash by incorporating nanogoethite

Sequestration of radioactive nickel (⁶³Ni²⁺) in fly ash coming from hospital wastes incineration plant by incorporating nano-goethite as a function of pH, particle size and the ratio of solid and liquid was investigated under the batch leaching experiments. The synthetic nanogoethite was characterized by X-ray diffraction (XRD), transmission electron microscopy (TEM) and specific surface area (SSA). The admired needle nanogoethite was obtained in terms of XRD, TEM and SSA analysis. Approximate 5% of ⁶³Ni²⁺ was desorbed from the nanogoethite/fly ash composite under the circum natural pH conditions. The ratio of solid to liquid has little effect on desorption of ⁶³Ni²⁺ from nanogoethite/fly ash composite. These results indicate that the radioactive nickel in fly ash can be sequestrated by incorporating nanogoethite. The results may play significantly a role in immobilization in situ of trace radionuclides in the natural environment.     

A method for the replacement of 137Cs with 40K as a non-hazardous radioactive tracer for open-source decommissioning research applications

The potential of ⁴⁰K as a radioactive tracer analogue of ¹³⁷Cs in ion exchange experiments is reported. Solutions of varying concentrations of potassium chloride (KCl) have been monitored radiometrically in a sodium iodide well-counter to determine the activity-concentration relationship. Ion exchange reactions using an exemplar ion exchange resin, KCl and non-radioactive caesium chloride (CsCl) solutions have been studied radiometrically. The adsorbed amounts of potassium and caesium are observed, inferred from displaced K⁺ ions, to be consistent with the total exchange capacity of the resin. Adsorption isotherm models have been applied to the experimental data, with the Freundlich isotherm observed to fit the data with the highest degree of consistency. The reported results indicate that decontamination techniques involving hazardous isotopes of anthropogenic origin such as ¹³⁷Cs can be developed, evaluated and optimised by substituting a chemically and physically similar non-hazardous radioactive isotope, in this case ⁴⁰K. This represents a means by which innovative decontamination techniques and regimes might be identified without the need to use ¹³⁷Cs and thus avoids additional generation of radioactive wastes.     

Magnesium-Potassium Phosphate Matrix for Immobilization of <Superscript>14</Superscript>C

Possibility of using a low-temperature magnesium-potassium phosphate matrix to solve the problem of immobilizing the radioactive wastes containing radioactive carbon (¹⁴C) in the form of calcium carbonate was examined. The physicochemical characteristics of the compounds obtained were determined. Large values of the ultimate compression strength (22 ± 5 MPa), which satisfy the technical requirements for cemented radioactive wastes (no less than 4.9 MPa), were obtained. The minimum carryover of carbon dioxide into the atmosphere in the course of synthesis and in keeping of samples for 14 days was noted: not more than 3 wt % relative to the starting CaCO₃. The leaching rate of carbonate ions from magnesium-potassium compounds by 28th day of contact with air does not exceed 10?9 g cm^?2 day^?1, with this value for the rest of the compound components not exceeding 10^?4 g cm^?2 day^?1. Thus, it was found that the magnesium?potassium phosphate matrix is an alternative to the cementation for solidification of radioactive wastes containing ¹⁴C.     

Separation and determination of <Superscript>90</Superscript>Sr in low- and intermediate-level radioactive wastes using extraction chromatography and LSC

A methodology for the determination of ⁹⁰Sr in low- and intermediate-level radioactive wastes from nuclear power plants is presented in this work. It is a part of a methodology developed for the sequential radiochemical separation of radionuclides difficult-to-measure directly by gamma spectrometry in these radioactive wastes. The separation procedure was carried out using precipitation and extraction chromatography with Sr Resin, from Eichrom and the ⁹⁰Sr was measured by liquid scintillation counting (LSC). Optimum conditions for the pretreatment, separation and LSC measurements were determined using simulated samples, which were prepared using standard solutions and carriers. The procedure showed to be rapid and achieved a good chemical yield, in the range 60–90%, and a detection limit of 6.0 × 10⁻⁴ Bq g⁻¹. The method was also tested by participation in a national intercomparison program, with aqueous samples, with good agreement of results.     

Effect of container adsorption on the210Pb/210Bi secular equilibrium relationship in spiked aqueous solutions

The radioactive boric acid wastes generated from the nuclear power plants have been solidified with cement. One of the properties required for solidified radioactive wastes is resistance to leaching. The leachability of¹³⁷Cs from solidified waste specimens prepared by various formulation has been studied according to the proposed ANS 16.1 Standard Leach Test. For the evaluation of radiological safety in the solidified radioactive waste disposal, the leachability indices have been determined from the leaching test data. The results have turned out to be 5.97–7.60, depending on formulation and solidifying matrix.     

Optical Emission Spectroscopy Measurements and Simulation of Radioelement Volatility During Radioactive Waste Treatment by Plasma

An optical emission spectroscopy (OES) method has been used to measure the concentration above the melt of some radioelements, ¹³⁷Cs, ⁶⁰Co and ¹⁰⁶Ru during the vitrification of radioactive wastes by thermal plasma. This method allows the study of non homogeneous optically thin plasmas exhibiting a symmetry plane without sophisticated tomographic systems. Local plasma temperatures above the melt have been evaluated using measured relative intensities of spectral lines of the plasma-forming gas. Radioelement concentrations in the plasma are deduced from the intensity ratio of the radioelement–gas spectral lines. A computer model is used to simulate the volatility of ¹³⁷Cs, ⁶⁰Co and ¹⁰⁶Ru, during the treatment of radioactive wastes by thermal plasma. This model is based on the calculation of system composition using the free enthalpy minimization method, coupled with the equation of mass transfer at the reactional interface. In this study, the OES measurements and the computer model allowed the determination of this radioelement volatility depending on the parameters like plasma current, and the nature of atmosphere furnace. The results of the model are compared to those obtained by OES measurements.     

Sequential extraction separation for determination of technetium-99 in radwastes by ICP-MS

An approach based on sequential extraction separation and the subsequent ICP-MS measurement was introduced to determine ⁹⁹Tc in radioactive wastes. The radwastes were firstly alkaline-fused and the ⁹⁹Tc was separated by a sequential solvent extraction prior to ICP-MS measurement. NaDDC was selected as a chelation reagent in the solvent extraction processes. The influence of HCl and matrix concentration on the recovery yield and the effectiveness of removing isobar and unwanted radionuclides, such as ¹³⁷Cs, ⁵⁴Mn, ⁶⁰Co and ^110mAg, were evaluated. The designed sequential extraction procedure was optimized by an extraction experiment. The proposed technique is proven to be a simple and practical alternative for ⁹⁹Tc determination in low-level radioactive wastes; chemical separation of ⁹⁹Tc can be simplified and preconcentration such as precipitation and/or ion exchange, before the solvent extraction, can be excluded.     

Speciation and Structural Properties of Hydrothermal Solutions of Sodium and Potassium Sulfate Studied by Molecular Dynamics Simulations

Aqueous solutions of salts at elevated pressures and temperatures play a key role in geochemical processes and in applications of supercritical water in waste and biomass treatment, for which salt management is crucial for performance. A major question in predicting salt behavior in such processes is how different salts affect the phase equilibria. Herein, molecular dynamics (MD) simulations are used to investigate molecular‐scale structures of solutions of sodium and/or potassium sulfate, which show contrasting macroscopic behavior. Solutions of Na?SO₄ exhibit a tendency towards forming large ionic clusters with increasing temperature, whereas solutions of K?SO₄ show significantly less clustering under equivalent conditions. In mixed systems (Na_xK_2?xSO₄), cluster formation is dramatically reduced with decreasing Na/(K+Na) ratio; this indicates a structure‐breaking role of K. MD results allow these phenomena to be related to the characteristics of electrostatic interactions between K⁺ and SO₄^2?, compared with the analogous Na⁺?SO₄^2? interactions. The results suggest a mechanism underlying the experimentally observed increasing solubility in ternary mixtures of solutions of Na?K?SO₄. Specifically, the propensity of sodium to associate with sulfate, versus that of potassium to break up the sodium–sulfate clusters, may affect the contrasting behavior of these salts. Thus, mutual salting‐in in ternary hydrothermal solutions of Na?K?SO₄ reflects the opposing, but complementary, natures of Na?SO₄ versus K?SO₄ interactions. The results also provide clues towards the reported liquid immiscibility in this ternary system.     

A radioactive tracer dilution method to determine the mass of molten salt

A new technique for molten salt mass determination, termed radioactive tracer dilution, that uses ²²Na as a tracer was validated at bench scale. It has been a challenging problem to determine the mass of molten salt in irregularly shaped containers, where a highly radioactive, high-temperature molten salt was used to process nuclear spent/used fuel during electrochemical recycling (pyro-processing) or for coolant/fuel salt from molten salt reactors. A radioactive source with known activity is dissolved into the salt. After a complete mixture, a small amount of the salt is sampled and measured in terms of its mass and radioactivity. By finding the ratio of the mass to radioactivity, the unknown salt mass in the original container can be precisely determined.

     

Rapid and accurate determination of89/90Sr in radioactive samples by Cerenkov counting

An improved and rapid method for determination of⁹⁰Sr via its daughter nuclide,⁹⁰Y, in aqueous samples from the low-level radioactive wastes by Cerenkov counting was established. This technique is applicable to beta particles maximum energies greater than 0.263 MeV in aqueous solution. A comparison of⁹⁰Sr determination by Cerenkov counting and standard wet chemical separation techniques indicates a high degree of correlation and excellent agreement. For a 20 ml aqueous sample following the prescribed experimental conditions and a 60 min counting interval, the detection limit was 0.20 dpm/ml (0.10 pCi/ml), and the relative deviation is less then 5%.     

Retention of some radionuclides in furnace lining during incineration of radioactive wastes

The incineration is one of the widely used method for treatment of solid radioactive wastes. The high volume and weight reduction coefficient (100–150 respectively 10–15) are advantages of this method. The greater part of radionuclides from solid radioactive wastes is retained in ash. From point of view of workers external irradiation, the radionuclides accumulation in furnace lining is one of risk factors. The Kalinit O 1200 is furnace lining material on NPPRIs Experimental Incineration facility. In the first step the sorption properties of this material from¹³⁷Cs,⁶⁰Co,⁵⁴Mn,⁶⁵Zn solutions were studied. The best results had⁶⁰Co, its distribution coefficient was 7036 kg · dm^–3. Cesium-137 was not absorbed on this material. The cylinders (height 5 cm, diameter 2 cm) from lining materials were made latest and were applicated inside the furnace and technological tract to study sorption properties from combustion gases. The penetration of radionuclide into lining material was studied too. The results obtained with this experiments are described in this paper.     

Determination of the amount and retention efficiency of aerosols arising during the vitrification of medium-level activity wastes from nuclear power plants

During the vitrification of medium-activity liquid wastes simulating the wastes from nuclear power plant aerosols are formed that enter into the gas pumped off from the vitrification furnace. The dependence of solid-aerosol carryover on the parameters characterizing the glass composition and its eluability were investigated in laboratory scale experiments. The aerosol carryover was determined either gravimetrically or radiometrically using radioactive tracers.¹³⁷Cs with a carrier was added to the wastes and the aerosol carryover was determined by following the¹³⁷Cs activity. In the case of the¹³⁷Cs-labeled aerosol it was observed that a higher alkali content in the melted wastes results in a higher carryover of the¹³⁷Cs-labeled aerosol. Using a multicomponent laboratory gas cleaning system a decontamination factor of 6.7·10⁶ was achieved for the removal of the¹³⁷Cs-labeled aerosol from the gas pumped off from the vitrification furnace.     

Separation of63Ni traces from low and medium level radioactive wastes produced during the operation of nuclear power reactors

The classification of low and medium level radioactive wastes produced regularly by nuclear power plants is becoming ever more important in Mexico, after a few years of running the first of two units, 600 MeV each, in Laguna Verde nuclear power plant. This paper describes a method to separate and detect traces of the weak -emitter⁶³Ni, which is one of the activation products used to classify low and medium level radioactive wastes originating from the operation of nuclear power plants.     

A Penning trap for studying cluster ions

We propose to use a Penning trap for spectroscopy of stored cluster ions. A similar device has been built for the purpose of mass measurements of short-lived nuclei produced at the on-line isotope separator ISOLDE/CERN. A resolving power of 500,000 in a mass measurement of³⁹K and an accuracy of 2 × 10^?7 for the⁸⁵Rb/³⁹K mass ratio were obtained. An efficiency for in-flight capture as high as 70% was achieved. The method provides very high sensitivity since typically only 10 to 100 ions are stored in the trap. We intend to perform laser spectroscopy on trapped Na clusters as a first application of the trap technique.     

Pyrohydrolytic separation technique for fluoride and chloride from radioactive liquid wastes

A rapid method for simultaneous determination of fluorine and chlorine in radioactive liquid wastes with ion chromatography after pyrohydrolysis separation was proposed for routine analysis. The elements were separated from radioactive liquid wastes by pyrohydrolysis and were subsequently determined with ion chromatograpy. Total time taken to determine these elements is about 45 min including 30 min for the pyrohydrolysis and 15 min for ion chromatography. The results of recovery tests ranged 95% or above. The limits of detection for F and Cl are 0.5 and 0.8 mg kg⁻¹, respectively.     

Activity concentration of226Ra and238U in various soils

The distribution of²²⁶Ra and²³⁸U in various soils has been studied. Supposing that radioactive equilibrium were in existence, the average activities of²²⁶Ra and²³⁸U would show a nearly 11 correlation. As weathering affects radioactive equilibrium in surface soil, radioactive equilibrium was not in existence. Therefore, four kinds of soil were selected from different weathering conditions, viz. river bed soil, paddy field soil, field soil and uncropped soil. The²²⁶Ra/²³⁸U ratio of various soils lies in the range of 1.63 to 2.41. The activity concentrations of²²⁶Ra were greater than²³⁸U in various soils. The ratio²²⁶Ra/²³⁸U can be shown to be a quantitative index of weathering. Phosphatic manure contains²³⁸U and its daughter isotopes in concentrations far exceeding the average abundance in the earth's crust. But the cultivated soils (paddy field soil, field soil) are not affected by fertilizers in Kamisaibara.     

Reduction of oxygen in lithium-potassium carbonate melt

The oxygen reduction reaction on smooth gold electrodes on Li/K (53: 47 at.%) carbonate melt has been examined in the temperature range 700–800°C. As in previous work on the Na/K melt [2], two chemically produced species (O₂^2? O₂^?) are reduced in parallel steps. The waves for the reduction of these species are close together in this melt, as distinct from those in the Na/K eutectic [2]. Exchange currents are somewhat higher than in the Na/K melt. Again, neutralization of the O^2? ion by CO₂ in rather slow, and may be rate-determining in porous electrodes.     

Preliminary results on labelling antibody Mab B72.3 with90Y

Rapid, safe and cost effective techniques for study of radiochemical wastes have been investigated by many workers. This work deals with a further study on this aspect by reverse radiometric flow injection analysis (rRFIA) technique.¹³⁷Cs and⁶⁰Co were determined in model radioactive wastewaters.     

Modified <Emphasis Type="Italic">Rhizopus arrhizus</Emphasis> biomass for sorption of <Superscript>241</Superscript>Am and other radionuclides

The improvement and the refinement of non-viable Rhizopus arrhizus biomass were investigated via immobilization. Immobilization was carried out by using sodium alginate/CaCl₂ solution and formaldehyde/HCl cross-linking with dead Rhizopus arrhizus biomass and were used for the sorption of radionuclides from low level effluent wastes. The sodium alginate/CaCl₂ immobilized biomass (ratio 1:2) showed about 86% sorption for ²⁴¹Am activity but due to its soft nature and tendency to undergo distortion in shape, is unsuitable for practical applications. The biomass cross-linked with 15% formaldehyde/0.1 M HCl solution has a relatively high mechanical strength and rigidity. It was showing a sorption of >99% for ²⁴¹Am activity and has the sorption capacity of ~65 mg/g for americium and uranium. Hence, it can be utilized for the removal of radionuclides from radioactive waste effluents.     

Estimation of 14C in irradiated graphite using CO2 gasification method

To efficiently inhibit the diffusion of radioactive nuclides in soil that were left by nuclear emergency accidents, microwave sintering technology was used in this work to vitrify the simulated strontium contaminated soil. Four kinds of simulated strontium-contaminated soil could be successfully vitrified almost completely within 30 min without any additional components. Sr²⁺ cations are immobilized into aluminosilicate glass network structure. In addition, the solubility of SrSO₄ in different soil is related to the element contents of aluminum and silicon. This work reveals a demonstration that beta-radioactive contaminated soil could be treated by microwave vitrifying.