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Title: The influence of cladding on fission gas release from irradiated U-Mo monolithic fuel

Abstract

The monolithic uranium-molybdenum (U-Mo) alloy has been proposed as a fuel design capable of converting the world’s highest power research reactors from use of high enriched uranium to low enriched uranium. However, a zirconium (Zr) diffusion barrier must be used to eliminate interactions that form during fabrication and are enhanced during irradiation between the U-Mo monolith and aluminum alloy 6061 (AA6061) cladding. One aspect of fuel development and qualification is to demonstrate appropriate understanding of the extent of fission product release from the fuel under anticipated service environments. An exothermic reaction has previously been observed between the AA6061 cladding and Zr diffusion layer. In this paper, two fuel segments with different irradiation history were subjected to specified thermal profiles under a controlled atmosphere using a thermogravimetric/differential thermal analyzer coupled with a mass spectrometer inside a hot cell. Samples from each segment were tested with cladding and without cladding to investigate the effect, if any, that the exothermic reaction has on fission gas release mechanisms. Measurements revealed there is an instantaneous effect of the cladding/Zr exothermic reaction, but not necessarily a cumulative effect above approximately 973 K (700 oC). The mechanisms responsible for fission gas release events are discussed.

Authors:
; ;
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1361009
Report Number(s):
PNNL-SA-121666
Journal ID: ISSN 0022-3115; DN3001010
DOE Contract Number:
AC05-76RL01830
Resource Type:
Journal Article
Resource Relation:
Journal Name: Journal of Nuclear Materials; Journal Volume: 486
Country of Publication:
United States
Language:
English
Subject:
U-Mo; fi; irradiation; cl

Citation Formats

Burkes, Douglas E., Casella, Amanda J., and Casella, Andrew M. The influence of cladding on fission gas release from irradiated U-Mo monolithic fuel. United States: N. p., 2017. Web. doi:10.1016/j.jnucmat.2017.01.016.
Burkes, Douglas E., Casella, Amanda J., & Casella, Andrew M. The influence of cladding on fission gas release from irradiated U-Mo monolithic fuel. United States. doi:10.1016/j.jnucmat.2017.01.016.
Burkes, Douglas E., Casella, Amanda J., and Casella, Andrew M. Sat . "The influence of cladding on fission gas release from irradiated U-Mo monolithic fuel". United States. doi:10.1016/j.jnucmat.2017.01.016.
@article{osti_1361009,
title = {The influence of cladding on fission gas release from irradiated U-Mo monolithic fuel},
author = {Burkes, Douglas E. and Casella, Amanda J. and Casella, Andrew M.},
abstractNote = {The monolithic uranium-molybdenum (U-Mo) alloy has been proposed as a fuel design capable of converting the world’s highest power research reactors from use of high enriched uranium to low enriched uranium. However, a zirconium (Zr) diffusion barrier must be used to eliminate interactions that form during fabrication and are enhanced during irradiation between the U-Mo monolith and aluminum alloy 6061 (AA6061) cladding. One aspect of fuel development and qualification is to demonstrate appropriate understanding of the extent of fission product release from the fuel under anticipated service environments. An exothermic reaction has previously been observed between the AA6061 cladding and Zr diffusion layer. In this paper, two fuel segments with different irradiation history were subjected to specified thermal profiles under a controlled atmosphere using a thermogravimetric/differential thermal analyzer coupled with a mass spectrometer inside a hot cell. Samples from each segment were tested with cladding and without cladding to investigate the effect, if any, that the exothermic reaction has on fission gas release mechanisms. Measurements revealed there is an instantaneous effect of the cladding/Zr exothermic reaction, but not necessarily a cumulative effect above approximately 973 K (700 oC). The mechanisms responsible for fission gas release events are discussed.},
doi = {10.1016/j.jnucmat.2017.01.016},
journal = {Journal of Nuclear Materials},
number = ,
volume = 486,
place = {United States},
year = {Sat Apr 01 00:00:00 EDT 2017},
month = {Sat Apr 01 00:00:00 EDT 2017}
}
  • The uranium–molybdenum (U-Mo) alloy in a monolithic form has been proposed as one fuel design capable of converting some of the world’s highest power research reactors from the use of high enriched uranium (HEU) to low enriched uranium (LEU). One aspect of the fuel development and qualification process is to demonstrate appropriate understanding of the extent of fission product release from the fuel under anticipated service environments. An apparatus capable of heating post-irradiated small-scale samples cut from larger fuel segments according to specified thermal profiles under a controlled atmosphere has been installed into a hot cell. Results show that optimizedmore » experimental parameters to investigate fission product release from small samples have been established. Initial measurements conducted on aluminum alloy clad uranium–molybdenum monolithic fuel samples reveal three clear fission gas release events over the temperature range of 30-1000 °C. The mechanisms responsible for these events are discussed, and the results have been compared with available information in the literature.« less
  • The uranium-molybdenum (U-Mo) alloy in a monolithic form has been proposed as one fuel design capable of converting some of the world’s highest power research reactors from the use of high enriched uranium (HEU) to low enriched uranium (LEU). One aspect of the fuel development and qualification process is to demonstrate appropriate understanding of the extent of fission product release from the fuel under anticipated service environments. An apparatus capable of annealing post-irradiated small-scale samples cut from larger fuel segments according to specified thermal profiles under a controlled atmosphere has been installed into a hot cell. Results show that optimizedmore » experimental parameters to investigate fission product release from small samples have been established. Initial measurements conducted on aluminum alloy clad uranium-molybdenum monolithic fuel samples reveal three clear fission gas release events over the temperature range of 30-1050 C. The mechanisms responsible for these events are discussed, and the results have been compared with available information in literature.« less
  • Low-enrichment (U-235 < 20%) U-Mo monolithic fuel is being developed for use in research and test reactors. The earliest design for this fuel that was investigated via reactor testing was comprised of a nominally U-10Mo fuel foil encased in AA6061 (Al-6061) cladding. For a fuel design to be deemed adequate for final use in a reactor, it must maintain dimensional stability and retain fission products throughout irradiation, which means that there must be good integrity at the fuel foil/cladding interface. To investigate the nature of the fuel/cladding interface for this fuel type after irradiation, fuel plates that were tested inmore » INL's Advanced Test Reactor (ATR) were subsequently characterized using optical metallography, scanning electron microscopy, and transmission electron microscopy. Results of this characterization showed that the fuel/cladding interaction layers present at the U-Mo fuel/AA6061 cladding interface after fabrication became amorphous during irradiation. Up to two main interaction layers, based on composition, could be found at the fuel/cladding interface, depending on location. After irradiation, an Al-rich layer contained very few fission gas bubbles, but did exhibit Xe enrichment near the AA6061 cladding interface. Another layer, which contained more Si, had more observable fission gas bubbles. Adjacent to the AA6061 cladding were Mg-rich precipitates, which was in close proximity to the region where Xe is observed to be enriched. In samples produced using a focused ion beam at the interaction zone/AA6061 cladding interface were possible indications of porosity/debonding, which suggested that the interface in this location is relatively weak.« less
  • Phase constituents and microstructure changes in RERTR fuel plate assemblies as functions of temperature and duration of hot-isostatic pressing (HIP) during fabrication were examined. The HIP process was carried out as functions of temperature (520, 540, 560 and 580 °C for 90 min) and time (45–345 min at 560 °C) to bond 6061 Al-alloy to the Zr diffusion barrier that had been co-rolled with U-10 wt.% Mo (U10Mo) fuel monolith prior to the HIP process. Scanning and transmission electron microscopies were employed to examine the phase constituents, microstructure and layer thickness of interaction products from interdiffusion. At the interface betweenmore » the U10Mo and Zr, following the co-rolling, the UZr2 phase was observed to develop adjacent to Zr, and the a-U phase was found between the UZr2 and U10Mo, while the Mo2Zr was found as precipitates mostly within the a-U phase. The phase constituents and thickness of the interaction layer at the U10Mo-Zr interface remained unchanged regardless of HIP processing variation. Observable growth due to HIP was only observed for the (Al,Si)3Zr phase found at the Zr/AA6061 interface, however, with a large activation energy of 457 ± 28 kJ/mole. Thus, HIP can be carried to improve the adhesion quality of fuel plate without concern for the excessive growth of the interaction layer, particularly at the U10Mo-Zr interface with the a-U, Mo2Zr, and UZr2 phases.« less