The reviewed papers presented here provide a general overview of worldwide radioactive waste-related studies conducted in 2019. The current review includes studies related to safety assessments, decommission and decontamination of nuclear facilities, fusion facilities, and transportation. Further, the review highlights radioactive wastewater decontamination, management solutions for the final disposal of low- and high-level radioactive wastes (LLRW and HLRW), interim storage and final disposal options for spent fuel (SF), and tritiated wastes, with a focus on environmental impacts due to the mobility of radionuclides in the ecosystem, water and soil along with other research progress made in the management of radioactive waste. PRACTITIONER POINTS: The release of radionuclides and their subsequent fate and transport in the environment poses public health concern and has stimulated recent research on the waste management techniques. Seeking a safe and environmental-friendly solution is the current trend for existing and projected inventories of radioactive waste. Significant progress in the field of geological disposal of radioactive waste has been made in the last two decades.

Radioactive waste: A review.

Elucidating the speciation of extracted lanthanides by diglycolamides

Two tripodal amides obtained from nitrilotriacetic acid with n-butyl and n-octyl alkyl chains (HBNTA(LI) and HONTA(LII), respectively) were studied for the extraction of Th(IV) ions from nitric acid medium. The effect of the diluent medium, i.e., n-dodecane alone and a mixture of n-dodecane and 1-decanol, onto aggregate formation were investigated using small angle neutron scattering (SANS) studies. In addition, the influence of the ligand structure, nitric acid, and Th(IV) loading onto ligand aggregation and third-phase formation tendency was discussed.The LI/LII exist as monomers (aggregarte radius for LI: 6.0 Å; LII:7.4 Å) in the presence of 1-decanol, whereas LII forms dimers (aggregarte radius for LII:9.3 Å; LI does not dissolve in n-dodecane) in the absence of 1-decanol. The aggregation number increases for both the ligands after HNO3 and Th(IV) loading. The maximum organic concentration (0.050 ± 0.004 M) of Th(IV) was reached without third-phase formation for 0.1 M LI/LII dissolved in 20% isodecanol +80% n-dodecane. The interaction of 1-decanol with LII and HNO3/Th(IV) with amidic oxygens of LI/LII results in shift of carbonyl stretching frequency, as shown by attenuated total reflectance-Fourier transform infrared (ATR-FTIR) studies. The structural and bonding information of the Th-LI/LII complex were derived from the density functional theoretical (DFT) studies. The molecular dynamics (MD) simulations suggested that the aggregation behavior of the ligand in the present system is governed by the population of hydrogen bonds by phase modifier around the ligand molecules. Although the theoretical studies suggested higher Gibbs free energy of complexation for Th4+ ions with LI than LII, the extraction was found to be higher with the latter, possibly due to the higher lipophilicity and solubility of the Th-LII aggregate in the nonpolar media.

Aggregation Behavior of Nitrilotriacetamide (NTAmide) Ligands in Thorium(IV) Extraction from Acidic Medium: Small-Angle Neutron Scattering, Fourier Transform Infrared, and Theoretical Studies.

Abstract This article studied the sorption behavior of Cs(I) ions from aqueous solutions onto molybdenum vanadate@bentonite (MoV@bentonite) composite. MoV@bentonite has been fabricated using the precipitation method and was characterized by different analytical tools including, FT-IR, XRD, and SEM attached with an EDX unit. The sorption studies applied on Cs(I) ions include the effect of contact time, pH, initial metal concentrations, ionic strength, desorption, and recycling. The experimental results revealed that in the adsorption process carried out after equilibrium time (300 min), saturation capacity has a value of 26.72 mg·g −1 and the sorption of Cs(I) ions is dependent on pH values and ionic strength. Sorption kinetic better fit with the pseudo-second-order model; sorption isotherms apply to Langmuir, Freundlich, and Dubinin-Radushkevich (D-R) isotherm models. Data of thermodynamic parameters indicate that sorption is spontaneous and endothermic. Recycling experiments show that MoV@bentonite could be used for 7 cycles and the best eluant for the recovery of Cs(I) ions is 0.1 M HCl (76.9%). All the obtained data clarify that MoV@bentonite is considered a promising sorbent for the sorption of Cs(I) ions from aqueous solutions. 

/pdf/performance-of-molybdenum-vanadate-loaded-on-bentonite-for-1hidfpem.pdf

Performance of molybdenum vanadate loaded on bentonite for retention of cesium-134 from aqueous solutions

Scandium is a valuable strategic resource widely dispersed in nature and frequently coexists with other minerals, some of which contain radionuclides, particularly uranium and thorium. It is of great importance to remove these radioactive elements in a green and efficient manner to manufacture superior scandium products. The present study synthesized a range of N-heterocyclic carboxamide ligands and undertook a full investigation of their efficacy in extracting and separating uranium and thorium from scandium. Of these, two demonstrated preferential extraction of radioactive elements in HNO3, while the extraction of scandium was observed in HClO4. Under optimum conditions, 95.3% of uranium and 70.7% of thorium were extracted with only a 3.6% loss of scandium after a single-stage extraction, and the other rare earth elements were scarcely extracted. In addition, almost all the uranium and thorium in a simulated solution were depleted following a five-stage extraction process when treated with the phenanthroline-derived carboxamide ligand, resulting in a scandium oxide product with a 99.99% purity. The coordination mechanism of the extraction was identified using slope analysis, NMR titration, and UV–vis titration. All the evidence indicates that U(VI) and Th(IV) complexes with the phenanthroline-derived carboxamide ligand have a stoichiometry ratio of 1:1, whereas, in the case of scandium, there are both 1:1 and 1:2 species. This work enables the preparation of high-purity scandium with an ultra-low level of radioactivity and provides a new idea for the efficient processing of rare earth minerals. 

Selective separation of radioactive thorium and uranium from scandium using N-heterocyclic carboxamide ligands

Solvent extraction of Eu3+ and Am3+ via N,N,N′,N'-tetraoctyl diglycolamide (TODGA) dissolved in different molecular diluents was studied. The diluent types used in this work were primary and secondary alcohols, secondary ketones and alkanes. Effects of concentration of extracting agent, temperature, diluent type and its carbon chain length on the extractions were determined. Distribution ratios of Eu3+ and Am3+ showed high dependence on the diluent type as well as the carbon chain length within the same type of diluent. The highest distribution ratios for both Eu3+ and Am3+ as well as the separation factors of Eu3+ over Am3+ were observed in the alkane diluents. Unexpectedly high distribution ratios for Eu3+ and Am3+ were observed in polar diluents with 5 carbon atoms in the chain, clearly standing out against the general trends. It was found that Eu3+ and Am3+ extraction via TODGA is enthalpy driven in all the studied diluents and that extraction is more exothermic in alkane diluents. Analysis of the stoichiometry of the extracted complexes shows that the average ligand number of TODGA molecules in the extracted complex is lower for Am3+ compared to Eu3+ except for with alkane diluents.

Effect of diluent on the extraction of europium( iii ) and americium( iii ) with N , N , N ′, N ′-tetraoctyl diglycolamide (TODGA)

Abstract Thirty liters of highly acidic spent nuclear fuel solutions need to be disposed at the “Hot Laboratory (hotlab)” facility in Paul Scherrer Institut (PSI), Switzerland. In order to significantly reduce the γ dose rate before proper disposal treatment, 137Cs must be removed. In the here presented sub-project, the ion-exchange method was evaluated. Two promising sorbents, CLEVASOL® and AMP (ammonium molybdophosphate), and two derived products AMP_PAN (AMP immobilized in polyacrylonitrile) and AMP/SiO2 (AMP immobilized on silica gel) were tested by the batch method using model solutions of important high-yield fission products (Cs, Eu, Zr, Ru, Pd and Ag), as well as U and Pu. The results showed that AMP, AMP/SiO2 and AMP_PAN have higher selectivity for Cs than CLEVASOL® in 0.1–8 M (mol/L) HNO3 solutions. 4 M HNO3 solution was identified as the most suitable condition for Cs-removal with AMP, AMP_PAN and AMP/SiO2 due to the still sufficiently high separation factor of Cs from other metal ions and an acceptable volume increase factor after dilution. The follow-up kinetic studies on AMP, AMP_PAN and AMP/SiO2 indicated that although Cs exchange on AMP and AMP/SiO2 is faster than on AMP_PAN in the first 5 min, they all nearly reach equilibrium after 30 min of contacting time. The isotherm curves of Cs adsorption on AMP, AMP_PAN and AMP/SiO2 in 4 M HNO3 showed that the maximum sorption capacity of Cs is reached asymptotically. The results from Langmuir isotherm modeling agree with results from other publications.

/pdf/selective-cs-removal-from-highly-acidic-spent-nuclear-fuel-2inh8c9xbo.pdf

Selective Cs-removal from highly acidic spent nuclear fuel solutions

During previous radioanalytical studies at Paul Scherrer Institute ca. 30 L of acidic waste containing spent nuclear fuel was produced, and now they need to be disposed A flow sheet for conditioning of these waste was designed and the extraction chromatography technique is evaluated. Suitable sorbents, such as AMP_PAN, TBP impregnated resin and DGA resin, were selected for the task of Cs-removal, extraction of U and Pu, and extraction of minor actinides and lanthanides, respectively. A pilot device will be built for preliminary tests with simulated solutions, and the facility will be built and evaluated with the real spent fuel solutions.

/pdf/a-concept-for-disposal-of-highly-acidic-spent-nuclear-fuel-3m64ulyb5e.pdf

A concept for disposal of highly acidic spent nuclear fuel solutions at PSI

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Effect of diluent on the extraction of europium( iii ) and americium( iii ) with N , N , N ′, N ′-tetraoctyl diglycolamide (TODGA)

Selective Cs-removal from highly acidic spent nuclear fuel solutions

A concept for disposal of highly acidic spent nuclear fuel solutions at PSI