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All sourcesNASA NTRSDOE OSTI
DOE OSTI2019

Aluminum Clad Spent Nuclear Fuel Task 5: Oxide Layer Response to Drying Experiment Test Plan

This document presents a test plan developed to assess the fundamental effectiveness of two widely accepted processes for drying spent nuclear fuel: vacuum drying and helium forced-gas drying. The experimental activities planned for Task 5 follow from the “Aluminum Clad Spent Nuclear Fuel Long Term Dry Storage Technical Issues Action Plan.”[Connolly, INL/EXT-17-43908] The objectives are to evaluate the response of the oxide corrosion layer on aluminum clad spent nuclear fuel (ASNF), processed at temperatures above 100°C, to understand and compare the behavior of oxide corrosion layer compositions resulting from a range of credible procedural variations during the transition of ASNF from wet storage to dry storage.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2014

CORROSION OF ALUMINUM CLAD SPENT NUCLEAR FUEL IN THE 70 TON CASK DURING TRANSFER FROM L AREA TO H-CANYON

Aluminum-clad spent nuclear fuel will be transported for processing in the 70-ton nuclear fuel element cask from L Basin to H-canyon. During transport these fuels would be expected to experience high temperature aqueous corrosion from the residual L Basin water that will be present in the cask. Cladding corrosion losses during transport were calculated for material test reactor (MTR) and high flux isotope reactors (HFIR) fuels using literature and site information on aqueous corrosion at a range of time/temperature conditions. Calculations of the cladding corrosion loss were based on Arrhenius relationships developed for aluminum alloys typical of cladding material with the primary assumption that an adherent passive film does not form to retard the initial corrosion rate. For MTR fuels a cladding thickness loss of 33 % was found after 1 year in the cask with a maximum temperature of 260 {degrees}C. HFIR fuels showed a thickness loss of only 6% after 1 year at a maximum temperature of 180 {degrees}C. These losses are not expected to impact the overall confinement function of the aluminum cladding.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2015

Corrosion of Aluminum Clad Spent Nuclear Fuel in the 70 Ton Cask during Transfer from L Area to H-Canyon

Aluminum-clad spent nuclear fuel will be transported for processing in the 70-ton nuclear fuel element cask from L Basin to H-canyon. During transport these fuels would be expected to experience high temperature aqueous corrosion from the residual L Basin water that will be present in the cask. Cladding corrosion losses during transport were calculated for material test reactor (MTR) and high flux isotope reactors (HFIR) fuels using literature and site information on aqueous corrosion at a range of time/temperature conditions. Calculations of the cladding corrosion loss were based on Arrhenius relationships developed for aluminum alloys typical of cladding material with the primary assumption that an adherent passive film does not form to retard the initial corrosion rate. For MTR fuels a cladding thickness loss of 33 % was found after 1 year in the cask with a maximum temperature of 263 °C. HFIR fuels showed a thickness loss of only 6% after 1 year at a maximum temperature of 180 °C. These losses are not expected to impact the overall confinement function of the aluminum cladding.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2022

Wettability and CHF limits of Accident-Tolerant nuclear fuel cladding materials in light water reactor conditions

Here, we present the results of experimental investigations aimed at evaluating the thermal–hydraulic performance of chromium-coated zircaloy, i.e., one of the most promising accident tolerant fuel (ATF) cladding material for light water nuclear reactors. Precisely, we investigate the wettability and critical heat flux (CHF) limits of chromium-coated and conventional zircaloy surfaces in prototypical reactor conditions. For both surface types, we measure the contact angle in a vapor-saturated atmosphere from ambient pressure to the operating pressure of pressurized water reactors (PWRs), i.e., ~15 MPa. We measure the ambient-pressure steady-state flow boiling CHF with a spatially uniform heat flux. We measure the high-pressure steady-state flow boiling CHF with a cosine shape heat flux (up to 20 MPa) and with a uniform heat flux (up to 15 MPa), also exploring the effect of CRUD deposits on the chromium-coated surface. Our results reveal that the chromium surface and the bare zircaloy surface have similar wettability and both become super-hydrophilic in PWR conditions, and that there is practically no difference in the steady-state CHF limits, both at low-pressure and high-pressure conditions, also when the chromium-coated surface is covered by a CRUD deposit. However, while the chromium-coating does not improve the CHF compared to the bare zircaloy surface, it improves the post-CHF behavior. The chromium coating prevents the reaction between zircaloy and steam, which results in the formation of a brittle zirconium oxide through the surface of the cladding. We also measure the transient CHF under exponentially escalating heat flux inputs of a nano-smooth and a rough surface mimicking a chromium-coated zircaloy cladding. Interestingly, the results of the transient heat flux tests suggest that the CHF limit for very short periods (i.e., fast transients) is independent of the surface finish, being the same for a rough chromium surface or a nano-smooth surface.

36 MATERIALS SCIENCE↗
DOE OSTI2015

Corrosion of Aluminum Clad Spent Nuclear Fuel in the 70 Ton Cask during Transfer from L Area to H-Canyon (Rev.1)

Aluminum-clad spent nuclear fuel will be transported for processing in the 70-ton nuclear fuel element cask from L Basin to H-canyon. During transport these fuels would be expected to experience high temperature aqueous corrosion from the residual L Basin water that will be present in the cask. Cladding corrosion losses during transport were calculated for material test reactor (MTR) and high flux isotope reactors (HFIR) fuels using literature and site information on aqueous corrosion at a range of time/temperature conditions. Calculations of the cladding corrosion loss were based on Arrhenius relationships developed for aluminum alloys typical of cladding material with the primary assumption that an adherent passive film does not form to retard the initial corrosion rate. For MTR fuels a cladding thickness loss of 33% was found after 1 year in the cask with a maximum temperature of 263 °C. HFIR fuels showed a thickness loss of only 6% after 1 year at a maximum temperature of 180 °C. These losses are not expected to impact the overall confinement function of the aluminum cladding.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2018

Aluminum Clad Spent Nuclear Fuel Task 4: Performance of Aluminum SNF in Dry Storage Experiment Test Plan

This document presents the activities to be performed in support of understanding the performance of aluminum spent nuclear fuel (ASNF) in dry storage. These activities will visually examine and acquire baseline samples of as-irradiated ATR fuel assembly components to determine fuel condition and the morphology of the aluminum oxyhydroxides present on the fuel external surfaces. Because the boehmite phase of oxyhydroxide is projected to be a significant contributor to radiolytic hydrogen production and general corrosion, being able to quantify its presence is of major importance to long term storage of aluminum spent nuclear fuel. Baseline samples will be taken from irradiated end adapters, removed from ATR SNF elements, stored in the ATR Canal. These will be transferred to Idaho National Laboratory (INL) Materials and Fuels Complex (MFC) to perform non-destructive and destructive testing to determine the degree of hydration of the wet-stored aluminum components prior to drying and air storage. Examination of the dry stored SNF at Idaho Nuclear Technology and Engineering Center (INTEC) in CPP-603 Irradiated Fuel Storage Facility (IFSF) will allow the opportunity to identify gross degradation and as conditions permit, sample the surface oxide on fueled and un-fueled portions of the stored assemblies. The information resulting from analysis of the ATR Canal samples will be used to support validation of surrogate samples prepared under Task 6, sample surrogate preparation, and used in Task 1, oxyhydroxide layer behavior and chemistry, Task 2, oxide layer radiolytic gas generation, and Task 5, oxide layer response to drying. Surface oxide samples collected from SNF in IFSF dry storage will SNF dry storage prediction modeling from Task 3, sealed and vented system episodic breathing and gas generation prediction.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2018

Aluminum Clad Spent Nuclear Fuel Task 6: Surrogate Sample Preparation and Validation Experiment Test Plan

This document presents the experimental test plan for Task 6: Surrogate Preparation and Validation. Task 6 will produce and validate surrogate oxyhydroxide materials used in other experimental tasks within the larger Aluminum Clad Spent Nuclear Fuel Long Term Dry Storage Project. Task 6 includes both the preparation and characterization of surrogate oxyhydroxide materials as well as the analysis of oxide/oxyhydroxide layers on Savannah River Site Spent Nuclear Fuel Materials. This test plan provides experimental design details and the task’s overall quality assurance approach.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2023

Review and Summary of Oxide Thickness Data for Aluminum-Clad Spent Nuclear Fuel

The U.S. Department of Energy (DOE) owns a large inventory of aluminum-clad spent nuclear fuel (ASNF) in interim storage pending ultimate disposition, with more being generated by currently operating research reactors. Dry storage in sealed DOE Standard Canisters is being investigated as an approach for long-term interim storage and/or disposition in a repository for ASNF. A primary challenge for ASNF storage is the presence of aluminum (oxy)hydroxide layers formed on the cladding surfaces during water exposure in the reactor and in wet storage, which forms a reservoir of chemisorbed water not readily removed at low (<100°C) drying temperatures. Free, physisorbed, and chemisorbed water are all susceptible to radiolytic breakdown under irradiation and can release hydrogen gas. Identifying the likely range of (oxy)hydroxide loadings on ASNF that may be placed in dry storage will help to ensure that the impact of the (oxy)hydroxide is adequately accounted for while avoiding over conservatism and enable mitigation strategies to be implemented where needed. The current report summarizes information on (oxy)hydroxide thicknesses and characteristics from the literature and from recent measurements taken in the present research campaign. In general, corrosion studies have indicated that the corrosion and oxide buildup on aluminum are affected by numerous conditions, including pH, temperature and heat flux, coolant flowrates, irradiation (in-reactor vs. unirradiated tests), duration of water exposure, and the amount of oxide already on the surface. Some of these factors are interrelated (e.g., the local temperature, heat flux, and coolant flowrate). Observations of the impact of irradiation (in-reactor versus ex-reactor measurements) on corrosion and oxide thickness are mixed, but multiple studies indicate that there is a significant difference between in-reactor and ex-reactor corrosion kinetics, even when other operating conditions such as pH, flowrate, heat flux, etc., simulate those in a reactor.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2021

Engineering Scale Drying of Aluminum-Clad Spent Nuclear Fuel: Experiment Report

Engineering-scale tests were performed to evaluate the relative effectiveness of forced gas and vacuum-drying processes on aluminum-clad spent nuclear fuel (ASNF) in preparation for extended dry storage. Drying models were developed to improve confidence in the likely range of conditions at the start of dry storage and to understand the factors most significant to each process. Testing was performed at the Holtec International Forced Helium Dehydration training facility in Camden, New Jersey, by students from the University of South Carolina in collaboration with Idaho National Laboratory. A full-size Type 1a basket, with a full-diameter vessel configuration (based on the Department of Energy standardized canister design), was used in combination with a 10 assembly surrogate ASNF arrangement to provide a proxy for geometry. A resistance heater incorporated in one assembly simulated the influence of 100 W decay heat. This instrumented chamber allowed testing of the removal of bulk water, physisorbed water, and chemisorbed water over a range of operating parameters with either drying process. Thick oxide films were grown on aluminum test plates to mimic the ASNF surface chemistry. These one-use test plates were housed within select assemblies during drying. Post-test analysis of these plates gave a measure of the moisture removed during each test, which was compared to a control. Instrumentation provided detailed thermal, humidity, and gas or pressure data relevant to each test. Model simulations generally compared favorably to instrument data for the tests. While both processes were able to remove bulk water, removal of chemisorbed water was shown to depend heavily on local temperature. To the disadvantage of vacuum drying, operations approaching or exceeding 220°C achieved consistently more dehydroxylation.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2018

Development of cone-wedge-ring-expansion test to evaluate the tensile HOOP properties of nuclear fuel cladding

Here, we report the development of a cone wedge ring expansion test method to determine the tensile hoop properties of irradiated nuclear fuel cladding in a hot cell. A closed-form solution was developed to explicitly relate the hoop stress σ θ to the axial piston loading using the scale factor χ and the shear stress correction factor α, where the χ and α factors are used to convert the applied piston load and the radial dilatation of the ring into the tensile hoop stress-strain curve. The applicability of this new test method was demonstrated by successfully evaluating ring specimens of Zr-4 alloy to failure. The ring specimens deformed uniformly in the axial and circumferential directions until onset of necking. The χ and α factors were successfully determined by using a finite-element stress analysis that benchmarked with applied test load and total work to account for frictional forces and the associated energies dissipation between the different sliding components of the testing system. The tensile hoop strength values obtained using the proposed cone-wedge-ring-expansion test method were 10% higher than values obtained from the tensile evaluation of the cladding material along the axial direction. In conclusion, the variability in results was found to be within the range reported in the literature.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2018

Aluminum Clad Spent Nuclear Fuel Task 2: Oxide Layer Radiolytic Gas Generation Resolution Experiment Test Plan

This document presents the test plan for Task 2 of the Aluminum Clad Spent Nuclear Fuel Long Term Dry Storage Technical Issues Action Plan. This task’s overarching goal is the resolution of gas generation resulting from the radiolytic degradation of the oxide layers on aluminum. The uncertainty associated with the build-up of gaseous radiolytic products inside the ASNF storage canisters is one of the dominant technical challenges associated with long term dry storage of aluminum clad fuel. The objectives of the Task 2 test plan are to: 1. Understand how radiation chemistry inside the ASNF dry storage canister impacts extended dry storage performance. 2. Understand the radiation induced mechanisms governing the production of radiolytic gases and alteration of gas composition within a canister. 3. Correlate the observed changes in material properties of ASNF with the radiolytic degradation of aluminum oxide in fill environments of variable moisture and gas composition. 4. Compile a predictive kinetic modeling tool, to provide quantitative mechanistic insight into the in-cask radiation chemistry of ASNF. 5. Interface with the canister modeling activity of Task 3 to deliver degradation rates for package performance of both sealed and vented scenarios.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2018

An advanced experimental design for modified burst testing of nuclear fuel cladding materials during transient loading

Here an advanced tube-burst test system was designed to test samples of nuclear fuel cladding under conditions relevant to a postulated design-basis reactivity insertion accident (RIA) in light-water reactors. The system is based on the “driver tube” concept and allows for high-speed testing with internal pressure impulses of 10–1000 ms. To measure strain, the system was equipped with an ultra-high-speed video camera with a telecentric lens providing high focal depth, to compensate for specimen shift. A mirror system was developed to provide 360° view of the tube specimen into a single camera. Images taken during the test allow the use of a digital image correlation approach in strain evaluation. Several experiments were conducted to assess the performance of the experimental setup, and results are reported.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2020

Modeling of SRS Aluminum-clad Spent Nuclear Fuel in Standard DOE Sealed Canisters

At the Savannah River Site (SRS), approximately 7 MTHM of aluminum-clad spent nuclear fuel is currently in wet storage at L-basin. A significant portion of this fuel is slated to be dried and sealed in DOE standard canisters for long-term storage. This report will focus on a few fuel types, which should bound all other fuel stored at SRS. These consist of the reference fuel assembly, the MURR fuel and the HFIR fuel. These bound a hypothetical maximum scenario for MTR box fuel, a maximum for decay heat in an assembly, and a maximum for the aluminum surface area, respectively. The geometry for the packages were created from DOE specifications for storage of each of the fuels. As long as the minimum time from reactor discharge to sealed storage is 3 years, then the highest temperatures which occur within the sealed canisters do not exceed 100° C for all scenarios considered here. In the geometry considered, while the HFIR fuel has a large surface area, the packaging configuration leaves large void areas, such that the aluminum surface to free volume ratio is about 30% less than an ATR or MURR packaging configuration.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2020

Independent Technical Review of INL Aluminum-Clad Spent Nuclear Fuel (ASNF) Oxide Layer Radiolytic Gas Generation Resolution: Task 2

PNNL staff performed an independent technical review (ITR) of the aluminum-clad spent nuclear fuel (ASNF) program Task 2. The objective of Task 2 is to determine G-values for the radiolytic production of gaseous molecular hydrogen (H 2 ) from the aluminum oxyhydroxide layers present on ASNF cladding. The G-values need to be defensible, bounding, but not overly conservative. As part of the ITR, the team reviewed program documents, Task 2 work plans, and results to date. In addition, the team held three separate video conferences with the program research staff to ask clarifying questions and obtain additional detail. The PNNL ITR team concludes that if the program follows the methodology and rigor outlined in the test matrices, the program will develop G-values for a defensible technical basis of extended storage of ASNF. Recommendations for improvement are given.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2017

Characterization of the Chlorination Products of Zirconium Alloys used for Nuclear Fuel Cladding

The United States produces over 2000 metric tons of used nuclear fuel material per year, of which 25% is irradiated fuel cladding, and it is expected to increase for the next 50 years. Previous simulation studies have shown that in the irradiated cladding, the major activation products found are {sup 125}Sb, {sup 60}Co, and {sup 99m}Nb, and the major fission product found is {sup 137}Cs. These radioisotopes make it impossible to treat the cladding as low level waste. A chlorination process has been proposed for zirconium reprocessing as it has been proven more efficient than previous mechanical processes, redox processes, and other chemical methods (e.g. iodination). In the chlorination process, zirconium alloy cladding reacts with Cl{sub 2} at 350- 380 deg. C to produce mainly ZrCl{sub 4}. The zirconium tetrachloride has a relatively low sublimation point (331 deg. C) that allows its separation from other products, and so it can be treated as low level waste for disposal or recycling. However, previous work has observed element impurities (iron, tin, chromium, cesium, antimony, and niobium) in the recovered ZrCl{sub 4}, meaning that additional steps are necessary in a chlorination process previous to the reduction of ZrCl, to metallic Zr. The emphasis of this research summary is on the progress that has been made to isolate and characterize the impurities produced after chlorination of three previously characterized non-irradiated zirconium alloys (Zircaloy-2, Zircaloy-4, and a commercial Zr-Nb alloy) widely used as cladding materials.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2024

Bounding Pressure and Flammability Evaluations of Aluminum-Clad Spent Nuclear Fuel Department of Energy Standard Canisters

This paper presents bounding pressure and flammability evaluations for DOE Standard Canister loaded with DOE-managed aluminum-clad spent nuclear fuel (ASNF). The objective of these evaluations is to gain confidence in the safety and feasibility of possible loading configurations for extended (>50 years) periods of dry storage, with particular focus on the dry storage canister pressures and potential for formation of a flammable atmosphere. The primary concern about the extended dry storage of ASNF is radiolytic gas generation. The aluminum cladding of these materials tends to corrode, and these corrosion products—typically aluminum oxides, such as boehmite, bayerite, or gibbsite—could carry water. This makes ASNF dry storage canisters difficult to dry. The gamma radiation field in dry storage environments could cause a radiolytic breakdown of residual water, forming chemical species such as molecular hydrogen (H2). The release of these species could increase the canister pressure and lead to the generation of a flammable canister atmosphere. The bounding evaluations presented within this study surmise conservative, but credible, conditions and processes. This includes the assumption of a full breakdown of a large quantity of free, physisorbed, and chemisorbed water (bound in a trihydrate, i.e., Al2O3 • 3H2O, layer). The considered dry storage configurations include a ~3 m (10 ft) long, ~46 cm (18 in) diameter (10 x 18) DOE Standard Canister loaded with 32 Advanced Test Reactor (ATR) ASNF elements, and a ~3 m (10 ft) long, ~61 cm (24 in) (10 x 24) diameter DOE Standard Canister loaded with 40 ATR ASNF elements. While the results of this study indicate the possibility of atmospheric hydrogen concentrations above the lower flammability limit, insufficient concentrations of oxygen will prevent the formation of flammable atmospheres. The maximum credible pressures remain well within the structural limits of the DOE Standard Canister.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗