Uranium (iv) Dioxide and Simfuel as Chemical Analogues of Nuclear Spent Fuel Matrix Dissolution. A Comparison of Dissolution Results in a Standard Naci/NaHCO3 Solution

1994 ◽  
Vol 353 ◽  
Author(s):  
Jordi Bruno ◽  
I. Casas ◽  
E. Cera ◽  
J. de Pablo ◽  
J. GimÉnez ◽  
...  
Keyword(s):  
Dissolution Rate ◽  
Nuclear Fuel ◽  
Spent Nuclear Fuel ◽  
Dissolution Process ◽  
Experimental Comparison ◽  
Comparison Study ◽  
Spent Fuel ◽  
Dissolution Rates ◽  
Surface Sites ◽  
Radiolytic Oxidation

AbstractWe have carried out an experimental comparison study of the dissolution rates of unirradiated UO2 and SIMFUEL pellets and particles (100–300 μm) in a standard NaCI/NaHC03 solution, under oxidizing conditions. We have performed the experiments using batch and flow methodologies. Both methodologies gave similar results, indicating that the overall oxidation/dissolution process is the same in both cases. The results from the experiments indicate that under these conditions the dissolution process is both oxygen and bicarbonate promoted. The dissolution rates we obtained are: R=2.4 ± 0.8 mg U/m2 d for U02 and R= 0.17 ± 0.05 mg U/m2 d for SIMFUEL. The results of the experiments indicate that the dissolution rate under oxic conditions is clearly dependent on the number of U(VI) surface sites which for spent nuclear fuel is a function of the extent of radiolytic oxidation.

The effects of alpha-radiolysis on UO2 dissolution determined from electrochemical experiments with 238Pu-doped UO2

2002 ◽  
Vol 90 (9-11) ◽  
Author(s):  
S. Stroes-Gascoyne ◽  
F. King ◽  
J. S. Betteridge ◽  
F. Garisto
Keyword(s):  
Dose Rate ◽  
Nuclear Fuel ◽  
Spent Nuclear Fuel ◽  
Spent Fuel ◽  
Geologic Repository ◽  
Dissolution Rates ◽  
Term Stability ◽  
Long Term Stability ◽  
Alpha Radiolysis

SummaryThe long-term stability of spent nuclear fuel under deep geologic repository conditions will be determined mostly by the influence of α-radiolysis, since the dose-rate for α-radiolysis will exceed that for γ/β-radiolysis beyond a fuel age of ∼100 years and will persist for more than 10000 years. Dissolution rates derived from studies with currently available spent fuel include radiolysis effects from γ/β- as well as α-radiolysis. The use of external α-sources and chemically added H

Corrosion Study of SIMFUEL in Aerated Carbonate Solution Containing Calcium and Silicate

2013 ◽  
Vol 1518 ◽  
pp. 139-144
Author(s):  
Hundal Jung ◽  
Tae Ahn ◽  
Roberto Pabalan ◽  
David Pickett
Keyword(s):  
Fission Product ◽  
Dissolution Rate ◽  
Nuclear Fuel ◽  
Polarization Resistance ◽  
Spent Nuclear Fuel ◽  
Electrochemical Impedance ◽  
Major Effect ◽  
Solution Chemistry ◽  
High Rate ◽  
Dissolution Rates

ABSTRACTThe corrosion behavior of simulated spent nuclear fuel (SIMFUEL) was investigated using electrochemical impedance spectroscopy and solution chemistry analyses. The SIMFUEL was exposed to aerated solutions of NaCl+NaHCO3 with and without calcium (Ca) and silicate. Two SIMFUEL compositions were studied, representing spent nuclear fuel (SNF) corresponding to 3 or 6 at % burnup in terms of fission product equivalents of surrogate elements. For all tested cases, the polarization resistance increased with increased immersion time, indicating possible blocking effects due to accumulation of corrosion products on the SIMFUEL surface. The potential-pH diagram suggests formation of schoepite that may cause the increase in the polarization resistance. The addition of Ca and silicate produced no measureable change in the polarization resistance measured at the corrosion potential. The dissolution rate ranged from 1 to 3 mg/m2-day, which is similar to the range of dissolution rates for SIMFUEL and SNF reported in the literature for comparable conditions. SIMFUEL burnup did not have a major effect on the dissolution rate. Analysis of the solution chemistry shows that uranium is the dominant element dissolved in the posttest solutions, and the dissolution rates calculated from uranium (U) concentrations are consistent with the dissolution rates obtained from impedance measurements. Simulated-fission product elements (i.e., barium, molybdenum, strontium, and zirconium) dissolved from the SIMFUEL electrode at a relatively high rate. Sorption test results indicated significant sorption of U onto the oxide formed on stainless steel. Electrochemical methods were found to be effective for measuring the uranium dissolution rate in real time.

Chemical Effects at the Reaction Front in Corroding Spent Nuclear Fuel

2006 ◽  
Vol 985 ◽  
Author(s):  
Jeffrey A. Fortner ◽  
A. Jeremy Kropf ◽  
James L. Jerden ◽  
James C. Cunnane
Keyword(s):  
Transition Zone ◽  
Nuclear Fuel ◽  
Spent Nuclear Fuel ◽  
Aqueous Environment ◽  
Spent Fuel ◽  
Aqueous Corrosion ◽  
Reduction Potentials ◽  
Chemical Effects ◽  
Before And After ◽  
X Ray Absorption

AbstractPerformance assessment models of the U. S. repository at Yucca Mountain, Nevada suggest that neptunium from spent nuclear fuel is a potentially important dose contributor. A scientific understanding of how the UO2 matrix of spent nuclear fuel impacts the oxidative dissolution and reductive precipitation of Np is needed to predict the behavior of Np at the fuel surface during aqueous corrosion. Neptunium would most likely be transported as aqueous Np(V) species, but for this to occur it must first be oxidized from the Np(IV) state found within the parent spent nuclear fuel. In this paper we present synchrotron x-ray absorption spectroscopy and microscopy findings that illuminate the resultant local chemistry of neptunium and plutonium within uranium oxide spent nuclear fuel before and after corrosive alteration in an air-saturated aqueous environment. We find the Pu and Np in unaltered spent fuel to have a +4 oxidation state and an environment consistent with solid-solution in the UO2 matrix. During corrosion in an air-saturated aqueous environment, the uranium matrix is converted to uranyl (UO22+) mineral assemblage that is depleted in Np and Pu relative to the parent fuel. The transition from U(IV) in the fuel to a fully U(VI) character across the corrosion front is not sharp, but occurs over a transition zone of ∼ 50 micrometers. We find evidence of a thin (∼ 20 micrometer) layer that is enriched in Pu and Np within a predominantly U(IV) environment on the fuel side of the transition zone. These experimental observations are consistent with available data for the standard reduction potentials for NpO2+/Np4+ and UO22+/U4+ couples, which indicate that Np(IV) may not be effectively oxidized to Np(V) at the corrosion potential of uranium dioxide spent nuclear fuel in air-saturated aqueous solutions.

scholarly journals The Need for Integrating the Back End of the Nuclear Fuel Cycle in the United States of America

MRS Advances ◽  
2018 ◽  
Vol 3 (19) ◽  
pp. 991-1003 ◽  
Author(s):  
Evaristo J. Bonano ◽  
Elena A. Kalinina ◽  
Peter N. Swift
Keyword(s):  
United States ◽  
Nuclear Fuel ◽  
United States Of America ◽  
Spent Nuclear Fuel ◽  
Fuel Cycle ◽  
Nuclear Fuel Cycle ◽  
The United States ◽  
Spent Fuel ◽  
Dry Storage ◽  
The Us

ABSTRACTCurrent practice for commercial spent nuclear fuel management in the United States of America (US) includes storage of spent fuel in both pools and dry storage cask systems at nuclear power plants. Most storage pools are filled to their operational capacity, and management of the approximately 2,200 metric tons of spent fuel newly discharged each year requires transferring older and cooler fuel from pools into dry storage. In the absence of a repository that can accept spent fuel for permanent disposal, projections indicate that the US will have approximately 134,000 metric tons of spent fuel in dry storage by mid-century when the last plants in the current reactor fleet are decommissioned. Current designs for storage systems rely on large dual-purpose (storage and transportation) canisters that are not optimized for disposal. Various options exist in the US for improving integration of management practices across the entire back end of the nuclear fuel cycle.

Burnup Credit in the Criticality Safety Analysis of Spent Fuel in Storage Systems

2014 ◽  
Author(s):  
Vladyslav Soloviov
Keyword(s):  
Isotopic Composition ◽  
Nuclear Fuel ◽  
Beta Decay ◽  
Spent Nuclear Fuel ◽  
Storage Systems ◽  
Multiplication Factor ◽  
Spent Fuel ◽  
Neutron Multiplication ◽  
Initial Fuel ◽  
Effective Neutron

In this paper accounting of spent nuclear fuel (SNF) burnup of RBMK-1000 with actinides and full isotopic composition has been performed. The following characteristics were analyzed: initial fuel enrichment, burnup fraction, axial burnup profile in the fuel assembly (FA) and fuel weight. As the results show, in the first 400 hours after stopping the reactor, there is an increase in the effective neutron multiplication factor (keff) due to beta decay of 239Np into 239Pu. Further, from 5 to 50 years, there is a decrease in keff due to beta decay of 241Pu into 241Am. Beyond 50 years there is a slight change in the criticality of the system. Accounting for nuclear fuel burnup in the justification of nuclear safety of SNF systems will provide an opportunity to increase the volume of loaded fuel and thus significantly reduce technology costs of handling of SNF.

Developing a Concept for a National Used Fuel Interim Storage Facility in the United States

2013 ◽  
Author(s):  
Donald Wayne Lewis
Keyword(s):  
United States ◽  
Nuclear Fuel ◽  
Nuclear Waste ◽  
Spent Nuclear Fuel ◽  
The United States ◽  
Yucca Mountain ◽  
Storage Facility ◽  
Spent Fuel ◽  
Geological Repository ◽  
Interim Storage

In the United States (U.S.) the nuclear waste issue has plagued the nuclear industry for decades. Originally, spent fuel was to be reprocessed but with the threat of nuclear proliferation, spent fuel reprocessing has been eliminated, at least for now. In 1983, the Nuclear Waste Policy Act of 1982 [1] was established, authorizing development of one or more spent fuel and high-level nuclear waste geological repositories and a consolidated national storage facility, called a “Monitored Retrievable Storage” facility, that could store the spent nuclear fuel until it could be placed into the geological repository. Plans were under way to build a geological repository, Yucca Mountain, but with the decision by President Obama to terminate the development of Yucca Mountain, a consolidated national storage facility that can store spent fuel for an interim period until a new repository is established has become very important. Since reactor sites have not been able to wait for the government to come up with a storage or disposal location, spent fuel remains in wet or dry storage at each nuclear plant. The purpose of this paper is to present a concept developed to address the DOE’s goals stated above. This concept was developed over the past few months by collaboration between the DOE and industry experts that have experience in designing spent nuclear fuel facilities. The paper examines the current spent fuel storage conditions at shutdown reactor sites, operating reactor sites, and the type of storage systems (transportable versus non-transportable, welded or bolted). The concept lays out the basis for a pilot storage facility to house spent fuel from shutdown reactor sites and then how the pilot facility can be enlarged to a larger full scale consolidated interim storage facility.

Centralization of Canada’s Spent Nuclear Fuel

2013 ◽  
Author(s):  
Krista Nicholson ◽  
John McDonald ◽  
Shona Draper ◽  
Brian M. Ikeda ◽  
Igor Pioro
Keyword(s):  
Nuclear Fuel ◽  
Site Selection ◽  
Nuclear Power ◽  
Power Plants ◽  
Spent Nuclear Fuel ◽  
Selection Process ◽  
Spent Fuel ◽  
Geologic Repository ◽  
Candu Reactors ◽  
High Level

Currently in Canada, spent fuel produced from Nuclear Power Plants (NPPs) is in the interim storage all across the country. It is Canada’s long-term strategy to have a national geologic repository for the disposal of spent nuclear fuel for CANada Deuterium Uranium (CANDU) reactors. The initial problem is to identify a means to centralize Canada’s spent nuclear fuel. The objective of this paper is to present a solution for the transportation issues that surround centralizing the waste. This paper reviews three major components of managing and the transporting of high-level nuclear waste: 1) site selection, 2) containment and 3) the proposed transportation method. The site has been selected based upon several factors including proximity to railways and highways. These factors play an important role in the site-selection process since the location must be accessible and ideally to be far from communities. For the containment of the spent fuel during transportation, a copper-shell container with a steel structural infrastructure was selected based on good thermal, structural, and corrosion resistance properties has been designed. Rail has been selected as the method of transporting the container due to both the potential to accommodate several containers at once and the extensive railway system in Canada.

scholarly journals An Automated SeaFAST ICP-DRC-MS Method for the Determination of 90Sr in Spent Nuclear Fuel Leachates

Molecules ◽  
2020 ◽  
Vol 25 (6) ◽  
pp. 1429 ◽  
Author(s):  
Víctor Vicente Vilas ◽  
Sylvain Millet ◽  
Miguel Sandow ◽  
Luis Iglesias Pérez ◽  
Daniel Serrano-Purroy ◽  
...  
Keyword(s):  
Nuclear Fuel ◽  
Safety Assessment ◽  
Analytical Approach ◽  
Source Term ◽  
Spent Nuclear Fuel ◽  
Spent Fuel ◽  
Chemical Purification ◽  
Radiochemical Method ◽  
Good Agreement

To reduce uncertainties in determining the source term and evolving condition of spent nuclear fuel is fundamental to the safety assessment. ß-emitting nuclides pose a challenging task for reliable, quantitative determination because both radiometric and mass spectrometric methodologies require prior chemical purification for the removal of interfering activity and isobars, respectively. A method for the determination of 90Sr at trace levels in nuclear spent fuel leachate samples without sophisticated and time-consuming procedures has been established. The analytical approach uses a commercially available automated pre-concentration device (SeaFAST) coupled to an ICP-DRC-MS. The method shows good performances with regard to reproducibility, precision, and LOD reducing the total time of analysis for each sample to 12.5 min. The comparison between the developed method and the classical radiochemical method shows a good agreement when taking into account the associated uncertainties.

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