This study determined the dissolution rate of studtite, (UO)O(HO), which can be formed by reaction between HO and UO that leaks from spent nuclear fuel (SNF) in deep geological repositories. The batch dissolution experiments were conducted using synthesized studtite under different solution conditions with varying pHs and concentrations of HCO and [HO] in synthetic groundwater. The experimental results suggested that carbonate ligand and HO in groundwater accelerated the dissolution of studtite and uranium (U) release. Above 10 M of HO initial concentration, the released uranium concentration in solution decreased, possibly as a result of reprecipitation of studtite due to reaction between uranium and HO. The results will be useful to assess the comprehensive transport of uranium from both nuclear waste and SNF stored in deep geological repositories.
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http://dx.doi.org/10.1016/j.jenvrad.2018.01.010 | DOI Listing |
Inorg Chem
September 2024
Department of Chemistry and Biochemistry, University of Notre Dame, Notre Dame, Indiana 46556, United States.
Four uranyl peroxide compounds with novel structures were formed following the dissolution of studtite, [(UO)(O)(HO)](HO), in imidazolium-based ionic liquids. The compounds were characterized using single crystal X-ray diffraction (SCXRD), powder X-ray diffraction (PXRD), Raman and infrared (IR) spectroscopy, and scanning electron microscopy (SEM) with energy-dispersive X-ray spectroscopy (EDS). The ionic liquids used in the experiments were 1-ethyl-3-methylimidazolium (EMIm) diethyl phosphate, EMIm ethyl sulfate, and EMIm acetate.
View Article and Find Full Text PDFJ Hazard Mater
October 2023
ICSM, Univ Montpellier, CEA, CNRS, ENSCM, Marcoule, France.
Pseudomorphic transformations are related to chemical conversions of materials while conserving their shape and structural features. Structuring ceramic shapes this way can be used to tailor the physico-chemical properties of materials that can benefit particular applications. In the context of spent nuclear fuel storage interacting with radiolysis products, the sonochemical behavior of powdered UO was investigated in dilute aqueous solutions saturated with Ar/(20 %)O (20 °C).
View Article and Find Full Text PDFInorg Chem
July 2022
Department of Civil & Environmental Engineering & Earth Sciences, University of Notre Dame, Notre Dame, Indiana 46556, United States.
Mechanochemistry enables transformations of highly insoluble materials such as uranium dioxide or the mineral studtite [(UO)(O)(HO)]·(HO) into uranyl triperoxide compounds that can subsequently assemble into hydroxide-bridged uranyl peroxide dimers in the presence of lithium hydroxide. Dissolution of these solids in water yields uranyl peroxide nanoclusters including U, Li[(UO)(O)(OH)]. Insoluble uranium solids can transform into highly soluble uranyl peroxide phases in the solid state with miniscule quantities of water.
View Article and Find Full Text PDFInorg Chem
June 2022
Department of Chemistry, School of Engineering Sciences in Chemistry, Biotechnology and Health, KTH Royal institute of Technology, SE-10044 Stockholm, Sweden.
Hydrogen peroxide is produced upon radiolysis of water and has been shown to be the main oxidant driving oxidative dissolution of UO-based nuclear fuel under geological repository conditions. While the overall mechanism and speciation are well known for granitic groundwaters, considerably less is known for saline waters of relevance in rock salt or during emergency cooling of reactors using seawater. In this work, the ternary uranyl-peroxo-chloro and uranyl-peroxo-bromo complexes were identified using IR, Raman, and nuclear magnetic resonance (NMR) spectroscopy.
View Article and Find Full Text PDFDalton Trans
May 2021
Department of Chemistry, School of Engineering Sciences in Chemistry, Biotechnology and Health, KTH Royal institute of Technology, SE-10044 Stockholm, Sweden.
Two uranyl peroxides meta-studtite and studtite exist in nature and can form as alteration phases on the surface of spent nuclear fuel upon water intrusion in a geological repository. Meta-studtite and studtite have very low solubility and could therefore reduce the reactivity of spent nuclear fuel toward radiolytic oxidants. This would inhibit the dissolution of the fuel matrix and thereby also the spreading of radionuclides.
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