Removal of Radionuclides from Fukushima Daiichi Waste Effluents

This paper describes the processes used at the Fukushima Daiichi plant, Japan, to purify the waste effluents generated in the cooling of damaged reactors. These include primary cesium removal with the Kurion zeolite system and the SARRY system utilizing silicotitanate to remove radiocesium from water recirculated to reactors for cooling. Another process is the ALPS system to purify the retentates of the reverse osmosis plant to further purify the water from radionuclides after primary cesium separation. In ALPS, a major role is played by the transition metal hexacyanoferrate product CsTreat and sodium titanate SrTreat in the removal of radiocesium and radiostrontium, respectively. The performance of these four exchangers (zeolite, silicotitanate, hexacyanoferrate, and sodium titanate) is critically analyzed with respect to processing capacities and the decontamination factors obtained in the processes. Furthermore, general information on preparation, structure and ion exchange of these ion-exchanger categories is given with additional information on their use in nuclear waste effluent treatment processes. Finally, the importance of selectivity and associated factors are discussed.Peer reviewe

The effect of UV-C irradiation and EDTA on the uptake of Co2+ by antimony oxide in the presence and absence of competing cations Ca2+ and Ni2+

In nuclear power plants and other nuclear facilities the removal of cobalt from radioactive liquid waste is needed to reduce the radioactivity concentration in effluents. In liquid wastes containing strong organic complexing agents such as EDTA cobalt removal can be problematic due to the high stability of the CoEDTA complex. In this study, the removal of cobalt from NaNO3 solutions using antimony oxide (Sb2O3) synthesized from potassium hexahydroxoantimonate was investigated in the absence and presence of EDTA. The uptake studies on the ion exchange material were conducted both in the dark (absence of UVlight) and under UV-C irradiation. Ca2+ or Ni2+ were included in the experiments as competing cations to test the selectivity of the ion exchanger. Results show that UV-C irradiation noticeably enhances the cobalt sorption efficiency on the antimony oxide. It was shown that nickel decreased the sorption of cobalt to a higher extent than calcium. Finally, the sorption data collected for Co2+ on antimony oxide was modeled using six different isotherm models. The Sips model was found to be the most suitable model to describe the sorption process. The Dubinin-Radushkevich model was further used to calculate the adsorption energy, which was found to be 6.2 kJ mol-1. (c) 2021 Korean Nuclear Society, Published by Elsevier Korea LLC. This is an open access article under the CC BY-NC-ND license (http://creativecommons.org/licenses/by-nc-nd/4.0/).Peer reviewe

Electrospun sodium titanate fibres for fast and selective water purification

From the environmental and end-​users' viewpoints, electrospun ion exchange fibres provide highly efficient and sustainable material for separation of for example trace pollutants, such as radionuclides and heavy metals. This work aimed to reduce the amount of ion exchange material needed per unit volume of raw material subjected to an ion exchange process. We present a very simple process to electrospinning of sodium titanate fibres, but also test results of ion exchange kinetics measurements. Sodium titanate fibres are very promising material and it is possible that by exploiting electrospun inorganic sub-​micron fibres the ion exchanger mass required for a given capacity can be decreased significantly.Peer reviewe

Efficient and Selective Recovery of Trace Scandium by Inorganic Titanium Phosphate Ion-Exchangers from Leachates of Waste Bauxite Residue

The research leading to these results has received funding from the European Union (EU) Horizon 2020 Programme Marie Skłodowska-Curie actions under Grant Agreement no. 636876 (MSCA-ETN REDMUD).Bauxite residue (BR) is an inevitable industrial waste generated through the classic Bayer extraction of alumina from bauxite minerals. It contains relatively significant amount of valuable rare earth elements, including scandium, and therefore, we explored the suitability of trace scandium recovery from BR acid leachate by titanium phosphate (TiP) ion exchangers. Three kinds of TiP materials (amorphous TiP, α-TiP, and γ-TiP) were synthesized through fluorine-free precursors and characterized by chemical analysis, X-ray diffraction (XRD), field emission scanning electron microscopy (FE-SEM), Fourier transform infrared (FTIR), ultraviolet/visible (UV/vis) diffuse reflectance spectrometry, 31P magic angle spinning (MAS) nuclear magnetic resonance (NMR), thermogravimetric analysis (TGA), and potentiometric titration. The Sc3+ exchange capacities were determined as 1.74, 0.55, and 0.22 mequiv g–1 for amorphous, α-, and γ-TiP, respectively. Competition of major elements (Fe, Al, Ca) in BR leachate with Sc uptake were studied in batch experiments using binary equimolar mixtures, and the separation factors of Sc/Fe2+, Sc/Al, and Sc/Ca reached magnitudes of 10–1000 on amorphous TiP. The high Sc3+selectivity by amorphous TiP was suspected to be the matching of Ti4+ lattice radius with Sc3+ ionic radius (both 0.745 Å). Finally, the separation of trace scandium from the simulated BR leachate solution was demonstrated on an amorphous TiP column. The interference of Fe3+ has been partially resolved by on-column reduction using sodium sulphite. The optimized final eluate contained only Sc, Fe, and Al. The concentration ratio of Sc/Fe can be increased by a factor of 8.8 and Sc/Al by 265 through a single cycle of chromatographic separation with an Sc recovery rate of 91.1%.Peer reviewe

Separation of cobalt, neodymium and dysprosium using amorphous zirconium phosphate

The purpose of this study was to investigate the separation of Co, Nd and Dy from a ternary Co-Nd-Dy solution using amorphous zirconium phosphate (am-ZrP). Am-ZrP was synthesized by a precipitation method at room temperature and subsequently characterized by Fourier transform-infrared spectrometry, thermogravimetry, scanning electron microscopy, X-ray diffraction, solid-state 31P magic angle spinning nuclear magnetic resonance spectrometry and sodium hydroxide titration (with and without background salt). The ion exchange kinetics of am-ZrP that were determined in ternary 1 mM equimolar solutions at equilibrium pH 2.5. The effect of pH on the adsorption was studied in ternary 1 mM equimolar solutions and the uptakes of the metals increased with increasing pH until approximately pH 3.5. The adsorption isotherms of Co, Nd and Dy were tested in a series of ternary equimolar solution, the total uptake amounted to 4.13 meq/g at pH ~ 3.0. The preference of am-ZrP for these metals occurred in decreasing order Dy > Nd ≫ Co. The separation of Co, Nd and Dy from their 1 mM equimolar ternary mixture was investigated on an am-ZrP column. Effects of loading (7.8%, 62% and 100%) on the separation were compared by measuring the corresponding HNO3 elution fractions. It was found that with a lower metal loading of 7.8%, three clear elution bands were obtained. Am-ZrP exhibited selective separation properties towards the ternary Co-Nd-Dy system, which contribute to the future scale-up studies for the recycling of NdFeB magnets.Peer reviewe

The use of columns of the zeolite clinoptilolite in the remediation of aqueous nuclear waste streams

Mud Hills clinoptilolite has been used in an effluent treatment plant (SIXEP) at the Sellafield nuclear reprocessing site. This material has been used to remove Cs-134/137 and Sr-90 successfully from effluents for 3 decades. Samples of the zeolite have been tested in column experiments to determine their ability to remove radioactive Cs+ and Sr2+ ions under increasing concentrations of competing ions, Ca2+, Mg2+, Na+ and K+. These ions caused increased elution of Cs+ and Sr2+. Ca2+, Mg2+ and K+ were more effective competitors than Na+. For Na+, it was found that if concentration was reduced, then column performance recovered rapidly.Peer reviewe

Removal of Ni-63 and Co-57 from aqueous solution using antimony doped tin dioxide-polyacrylonitrile (Sb doped SnO2-PAN) composite ion-exchangers

WOS: 000329299200119Tin dioxide and its antimony doped counterpart were synthesized using traditional sol-gel procedure. The metal oxides were then turned into composites by mixing them with polyacrylonitrile (PAN) and composite spheres ready for use in traditional column applications were obtained. The characterization of materials was investigated by X-ray diffraction, scanning electron microscopy-energy dispersive X-ray, surface area, point of zero charge and thermal analyses. Static batch experiments showed that the antimony doped tin dioxide-PAN (Sb doped SnO2-PAN) is an effective material for nickel removal and the composite maintains its good metal uptake properties in dynamic column conditions. The composite showed a high nickel uptake capacity of 9 mmol/g in 0.1 M NaNO3 solution. It was observed that the ion exchange kinetics of antimony doped tin dioxide (Sb doped SnO2) was remarkably fast for Co-57 and Ni-63 ions but turning the material into PAN composite significantly decreased the materials kinetic properties

Effects of synthesis conditions on ion exchange properties of α-zirconium phosphate for Eu and Am

Citation Information: Radiochimica Acta, ISSN (Online) 2193-3405, ISSN (Print) 0033-8230, DOI: https://doi.org/10.1515/ract-2016-2740.Peer reviewe