A Study of Uranyl (VI) Chloride Complexes in Aqueous Solutions under Hydrothermal Conditions using Raman Spectroscopy

MRS Advances ◽  
2020 ◽  
Vol 5 (51) ◽  
pp. 2623-2629
Author(s):  
Diwash Dhakal ◽  
Nadib Akram ◽  
Robert A. Mayanovic ◽  
Hakim Boukhalfa ◽  
Hongwu Xu
Keyword(s):  
Raman Spectroscopy ◽  
Nuclear Waste ◽  
Nuclear Reactor ◽  
Aqueous Media ◽  
Chloride Concentration ◽  
Spent Fuel ◽  
Hydrothermal Conditions ◽  
Chloride Complexes ◽  
Complex Species ◽  
Uranyl Chloride

ABSTRACTThe transport and deposition of uranium under hydrothermal conditions in the Earth’s crust has been a subject of ongoing study but is yet to be completely understood. In addition, there is little known about the fate of nuclear waste, consisting of uranium from spent fuel and other radioactive materials, upon storage in repositories or in nuclear reactor facilities. Because the nuclear waste often comes in contact with aqueous fluids in storage environments, studies of uranyl complexation with chloride and other ligands in aqueous media, to high temperature and pressure conditions, are needed. The primary purpose of this study was to investigate the speciation of aqueous uranyl (VI) chloride complexes, in solutions having a 0.05 M uranyl concentration and [Cl] concentrations ranging from 0.2 M to 6 M, under hydrothermal conditions. The aqueous uranyl chloride complexes in the samples were studied using Raman spectroscopy and the hydrothermal diamond anvil cell (HDAC), at temperatures up to 500 °C and pressures up to ~ 0.5 GPa. The uranyl bond stretching band feature occurring in the ~810 to 870 cm-1 region was fitted using the Voigt peak shape to determine the speciation of the equilibrium uranyl chloride complexes present in the samples. As expected, the n integer value of the UO2Cln+2-n complex species increases with the increase in temperature and chloride concentration, generally trending toward charge neutrality at high temperatures.

Study of the Susceptibility of Oxygen-Free Phosphorous Doped Copper to Corrosion in Simulated Groundwater in the Presence of Chloride and Sulfide

2006 ◽  
Vol 985 ◽  
Author(s):  
Ivan Escobar ◽  
Claudia Lamas ◽  
Lars Werme ◽  
Virginia Oversby
Keyword(s):  
Electrochemical Impedance ◽  
Copper Chloride ◽  
Chloride Concentration ◽  
Copper Surface ◽  
Chloride Ions ◽  
Transport Processes ◽  
Ion Concentration ◽  
Spent Fuel ◽  
High Concentration ◽  
Chloride Complexes

AbstractCopper of the quality oxygen free and high conductivity, doped with phosphorus (Cu OFP) has been chosen as the material for the fabrication of high level nuclear waste containers in Sweden. This material will be the corrosion barrier for spent fuel in the environment of a deep geological repository. It is planned that the service life of this container will be 100,000 years. During this time water with high concentration of chloride ions might come in contact with the copper surface. If pH conditions are appropriate, this might cause pitting corrosion. This work reports a study of the susceptibility of Cu OFP to corrosion when chloride ions are present, both deionized water (DW) and in standard synthetic underground water (SUW). The techniques used were electrochemical methods such as corrosion potential evolution and Tafel curves. In addition, this system was studied with Electrochemical Impedance Spectroscopy (EIS). We also used characterization techniques such as Scanning Electronic Microscopy (SEM), Energy Disperse Spectroscopy (EDS) . The main conclusions are that copper is more susceptible to corrosion at high chloride ion concentration. Additionally, when the chloride concentration is low, it is possible to form copper chloride crystals, but at the highest concentration, copper chloride complexes are formed, leaving the copper surface without deposits. When the chloride concentration is low (<0.1 M) the corrosion process is mainly controlled by diffusion, while at higher concentrations (0.1M to 1M) corrosion is controlled by transport processes. At low concentration of sulfide ( <3*10-5M), copper corrosion in the presence of chloride is controlled by diffusional processes.

Management of Nuclear Waste and Spent Fuel

1982 ◽  
Author(s):  
E. DRAPER ◽  
GEORGE COULBOURN
Keyword(s):  
Nuclear Waste ◽  
Spent Fuel

scholarly journals Corrosion of ternary borosilicate glass in acidic solution studied in operando by fluid-cell Raman spectroscopy

2021 ◽  
Vol 5 (1) ◽  
Author(s):  
Christoph Lenting ◽  
Thorsten Geisler
Keyword(s):  
Raman Spectroscopy ◽  
Nuclear Waste ◽  
Numerical Models ◽  
Adsorbed Water ◽  
Corrosion Mechanism ◽  
Borosilicate Glasses ◽  
Long Term Storage ◽  
In Operando ◽  
High Level ◽  
Fluid Cell

AbstractFluid-cell Raman spectroscopy is a space and time-resolving application allowing in operando studies of dynamic processes during solution–solid interactions. A currently heavily debated example is the corrosion mechanism of borosilicate glasses, which are the favoured material for the immobilization of high-level nuclear waste. With an upgraded fluid-cell lid design made entirely from the glass sample itself, we present the polymerization of the surface alteration layer over time in an initially acidic environment, including the differentiation between pore and surface-adsorbed water within it. Our results support an interface-coupled dissolution-precipitation model, which opposes traditional ion-exchange models for the corrosion mechanism. A sound description of the corrosion mechanism is essential for reliable numerical models to predict the corrosion rate of nuclear waste glasses during long-term storage in a geological repository.

scholarly journals Nuclear waste imaging and spent fuel verification by muon tomography

2013 ◽  
Vol 53 ◽  
pp. 267-273 ◽  
Author(s):  
G. Jonkmans ◽  
V.N.P. Anghel ◽  
C. Jewett ◽  
M. Thompson
Keyword(s):  
Nuclear Waste ◽  
Spent Fuel ◽  
Muon Tomography

NUCLEAR WASTE MANAGEMENT IN SPAIN: ANALYSIS OF THE CURRENT SITUATION AND ALTERNATIVE STRATEGIES

10.6036/10156 ◽  
2021 ◽  
Vol 96 (4) ◽  
pp. 355-358
Author(s):  
Pablo Fernández Arias ◽  
DIEGO VERGARA RODRIGUEZ
Keyword(s):  
Nuclear Waste ◽  
Nuclear Power ◽  
Power Plants ◽  
Nuclear Power Plants ◽  
Spent Fuel ◽  
Nuclear Waste Storage ◽  
Alternative Strategies ◽  
Temporary Storage ◽  
Long Term Storage ◽  
High Level

Centralized Temporary Storage Facility (CTS) is an industrial facility designed to store spent fuel (SF) and high level radioactive waste (HLW) generated at Spanish nuclear power plants (NPP) in a single location. At the end of 2011, the Spanish Government approved the installation of the CTS in the municipality of Villar de Cañas in Cuenca. This approval was the outcome of a long process of technical studies and political decisions that were always surrounded by great social rejection. After years of confrontations between the different political levels, with hardly any progress in its construction, this infrastructure of national importance seems to have been definitively postponed. The present research analyzes the management strategy of SF and HLW in Spain, as well as the alternative strategies proposed, taking into account the current schedule foreseen for the closure of the Spanish NPPs. In view of the results obtained, it is difficult to affirm that the CTS will be available in 2028, with the possibility that its implementation may be delayed to 2032, or even that it may never happen, making it necessary to adopt an alternative strategy for the management of GC and ARAR in Spain. Among the different alternatives, the permanence of the current Individualized Temporary Stores (ITS) as a long-term storage strategy stands out, and even the possibility of building several distributed temporary storage facilities (DTS) in which to store the SF and HLW from several Spanish NPP. Keywords: nuclear waste, storage, nuclear power plants.

The Effect of Waste Package Components on Radionuclides Released from Spent Fuel Under Hydrothermal Conditions

1987 ◽  
Vol 112 ◽  
Author(s):  
Shirley A. Rawson ◽  
William L. Neal ◽  
James R. Burnell
Keyword(s):  
Low Carbon Steel ◽  
Fission Products ◽  
Nuclear Waste Repository ◽  
Low Carbon ◽  
Spent Fuel ◽  
Hydrothermal Conditions ◽  
Waste Package ◽  
Dissolved Species ◽  
Radionuclide Release ◽  
Time Invariant

AbstractThe Basalt Waste Isolation Project has conducted a series of hydrothermal experiments to characterize waste/barrier/rock interactions as a part of its study of the Columbia River basalts as a potential medium for a nuclear waste repository. Hydrothermal tests of 3–15 months duration were performed with light water reactor spent fuel and simulated groundwater, in combination with candidate container materials (low-carbon steel or copper) and/or basalt, in order to evaluate the effect of waste package materials on spent fuel radionuclide release behavior. Solutions were filtered through 400 and 1.8 nm filters to distinguish colloidal from dissolved species. In all experiments, 14C, 129I, and 137Cs occurred only as dissolved species, whereas the actinides occurred in 400 nm filtrates primarily as spent fuel particles. Actinide concentrations in 1.8 nm filtrates were below detection in steel-bearing experiments. In the system spent fuel + copper, apparent time-invariant concentrations of 14C and 137Cs were obtained, but in the spent fuel + steel system, the concentrations of 14C and 137Cs increased gradually throughout the experiments. In experiments containing basalt or steel + basalt, 137Cs concentrations decreased with time. In tests with copper + basalt, 14C and 129I concentrations attained time-invariant values and 137Cs concentrations decreased. Concentrations for the actinides and fission products measured in these experiments were below those calculated from Federal regulations governing radionuclide release.

scholarly journals Remote Monitoring and Evaluation of Damage at a Decommissioned Nuclear Facility Using Acoustic Emission

2018 ◽  
Vol 8 (9) ◽  
pp. 1663 ◽  
Author(s):  
Marwa Abdelrahman ◽  
Mohamed ElBatanouny ◽  
Kenneth Dixon ◽  
Michael Serrato ◽  
Paul Ziehl
Keyword(s):  
Acoustic Emission ◽  
Remote Monitoring ◽  
Nuclear Reactor ◽  
Corrosion Damage ◽  
Monitoring And Evaluation ◽  
Structural Condition ◽  
Spent Fuel ◽  
Nuclear Facility ◽  
Nuclear Facilities ◽  
Accelerated Corrosion

Reinforced concrete systems used in the construction of nuclear reactor buildings, spent fuel pools, and related nuclear facilities are subject to degradation over time. Corrosion of steel reinforcement and thermal cracking are potential degradation mechanisms that adversely affect durability. Remote monitoring of such degradation can be used to enable informed decision making for facility maintenance operations and projecting remaining service life. Acoustic emission (AE) monitoring has been successfully employed for the detection and evaluation of damage related to cracking and material degradation in laboratory settings. This paper describes the use of AE sensing systems for remote monitoring of active corrosion regions in a decommissioned reactor facility for a period of approximately one year. In parallel, a representative block was cut from a wall at a similar nuclear facility and monitored during an accelerated corrosion test in the laboratory. Electrochemical measurements were recorded periodically during the test to correlate AE activity to quantifiable corrosion measurements. The results of both investigations demonstrate the feasibility of using AE for corrosion damage detection and classification as well as its potential as a remote monitoring technique for structural condition assessment and prognosis of aging structures.

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