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Phase transformation and growth kinetics in reaction zone between uranium alloy and zirconium diffusion barrier

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Date Issued:
2016
Abstract/Description:
U-10wt.%Mo (U10Mo) alloy as a part of monolithic fuel system is being developed under Material Management and Minimization Reactor Conversion (MMMRC) program, tasked with replacing high-enriched uranium (HEU) fuel with low-enriched uranium (LEU) fuel in civilian research and test reactors. Use of U10Mo fuel alloy entails a Zr diffusion barrier to avoid the undesirable interdiffusion and reactions between the U10Mo and Al-alloy cladding. To better understand the interaction between these fuel system constituents, microstructural development and diffusion kinetics in U-Mo-Zr, U-Zr and fuel plate assembly processed by co-rolling and hot isostatic pressing (HIP) were investigated using a variety of analytical techniques accompanying scanning electron microscopy and transmission electron microscopy.Phase constituents, microstructure and diffusion kinetics between U10Mo and Zr were examined using solid-to-solid diffusion couples annealed at 650 (&)deg;C for 240, 480 and 720 hours. Concentration profiles were mapped as diffusion paths on the isothermal ternary phase diagram. Within the diffusion zone, single-phase layers of (?U,?Zr) were observed along with a discontinuous layer of Mo2Zr between the ?Zr and ?U layers. In the vicinity of Mo2Zr phase, islands of ?Zr phase were also found. In addition, acicular ?Zr and U6Zr3Mo phases were observed within the ?U(Mo). Growth rate of the interdiffusion-reaction zone was determined to be 1.81 (&)#215; 10-15 m2/sec at 650 (&)deg;C, however with an assumption of a certain incubation period.Investigation for interdiffusion and reaction between U and Zr were carried out using solid-to-solid diffusion couples annealed at 580, 650, 680 and 710 (&)deg;C. The interdiffusion and reaction layer consisted of ?U containing Zr acicular precipitate, ?' (oC4-variant) and (?U,?Zr) solid solution at 650, 680 and 710 (&)deg;C. The ?-UZr2 phase, instead of (?U,?Zr) solid solution phase, was observed in the couple annealed at 580 (&)deg;C. The interdiffusion fluxes and coefficients were determined for the ?U, (?U,?Zr) and ?-UZr2 (580 ?C only) phases using both Sauer-Freise and Boltzmann-Matano analyses. For the ?'-phase with negligible concentration gradient, integrated interdiffusion coefficients were determined via Wagner method. Marker plane was found in (?U,?Zr) (cI2) solid solution from the couples annealed at 650, 680 and 710 (&)deg;C and ?-UZr2 from the couple at 580 (&)deg;C. Intrinsic diffusion coefficients at the compositions corresponding to the marker plane were determined based on Heumann analysis: U intrinsically diffused an order magnitude faster than Zr. Arrhenius temperature-dependence, Darken relation, and comparison to existing literature data demonstrated consistency in results.Monolithic fuel plate assembly was fabricated by sequential process of (1) co-rolling to laminate the Zr barrier onto the U10Mo fuel alloy and (2) HIP to encase the fuel laminated with Zr, within the Al-alloy 6061 (AA6061). In this study, HIP process was carried out as functions of temperature (520, 540, 560 and 580 (&)deg;C for 90 minutes), time (45, 60, 90, 180 and 345 minutes at 560 (&)deg;C) with ramp-cool rate (35, 70 and 280 (&)deg;C/hour). At the interface between the U10Mo and Zr, following the co-rolling, the UZr2 phase was observed to develop adjacent to Zr, and the ?U phase was found between the UZr2 and U10Mo. Mo2Zr was found as precipitates mostly within the ?U phase. 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 kJ/mol. Decomposition of ?U into ?U and ?' was observed in the U10Mo alloy. The volume fraction of ? and ?' increased as the HIP temperature and ramp-cool rate decreased. The UC-UO2 inclusions within the U10Mo fuel alloy were observed, but the volume percent of the UC-UO2 inclusions within the U10Mo alloy, ranging from approximately 0.5 to 1.8, did not change as functions of HIP temperature and holding time. However, the inclusions located near the surface of the U10Mo alloy, were frequently observed to interfere the uniformity of interdiffusion and reaction between the U10Mo alloy and Zr diffusion barrier. The regions of limited interaction between the U10Mo and Zr barrier associated with UC-UO2 inclusions decreased with an increase in HIP temperature, however no significant trend was observed with an increase in HIP duration at 560 (&)deg;C.
Title: Phase transformation and growth kinetics in reaction zone between uranium alloy and zirconium diffusion barrier.
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Name(s): Park, Young Joo, Author
Sohn, Yongho, Committee Chair
Coffey, Kevin, Committee Member
Fang, Jiyu, Committee Member
University of Central Florida, Degree Grantor
Type of Resource: text
Date Issued: 2016
Publisher: University of Central Florida
Language(s): English
Abstract/Description: U-10wt.%Mo (U10Mo) alloy as a part of monolithic fuel system is being developed under Material Management and Minimization Reactor Conversion (MMMRC) program, tasked with replacing high-enriched uranium (HEU) fuel with low-enriched uranium (LEU) fuel in civilian research and test reactors. Use of U10Mo fuel alloy entails a Zr diffusion barrier to avoid the undesirable interdiffusion and reactions between the U10Mo and Al-alloy cladding. To better understand the interaction between these fuel system constituents, microstructural development and diffusion kinetics in U-Mo-Zr, U-Zr and fuel plate assembly processed by co-rolling and hot isostatic pressing (HIP) were investigated using a variety of analytical techniques accompanying scanning electron microscopy and transmission electron microscopy.Phase constituents, microstructure and diffusion kinetics between U10Mo and Zr were examined using solid-to-solid diffusion couples annealed at 650 (&)deg;C for 240, 480 and 720 hours. Concentration profiles were mapped as diffusion paths on the isothermal ternary phase diagram. Within the diffusion zone, single-phase layers of (?U,?Zr) were observed along with a discontinuous layer of Mo2Zr between the ?Zr and ?U layers. In the vicinity of Mo2Zr phase, islands of ?Zr phase were also found. In addition, acicular ?Zr and U6Zr3Mo phases were observed within the ?U(Mo). Growth rate of the interdiffusion-reaction zone was determined to be 1.81 (&)#215; 10-15 m2/sec at 650 (&)deg;C, however with an assumption of a certain incubation period.Investigation for interdiffusion and reaction between U and Zr were carried out using solid-to-solid diffusion couples annealed at 580, 650, 680 and 710 (&)deg;C. The interdiffusion and reaction layer consisted of ?U containing Zr acicular precipitate, ?' (oC4-variant) and (?U,?Zr) solid solution at 650, 680 and 710 (&)deg;C. The ?-UZr2 phase, instead of (?U,?Zr) solid solution phase, was observed in the couple annealed at 580 (&)deg;C. The interdiffusion fluxes and coefficients were determined for the ?U, (?U,?Zr) and ?-UZr2 (580 ?C only) phases using both Sauer-Freise and Boltzmann-Matano analyses. For the ?'-phase with negligible concentration gradient, integrated interdiffusion coefficients were determined via Wagner method. Marker plane was found in (?U,?Zr) (cI2) solid solution from the couples annealed at 650, 680 and 710 (&)deg;C and ?-UZr2 from the couple at 580 (&)deg;C. Intrinsic diffusion coefficients at the compositions corresponding to the marker plane were determined based on Heumann analysis: U intrinsically diffused an order magnitude faster than Zr. Arrhenius temperature-dependence, Darken relation, and comparison to existing literature data demonstrated consistency in results.Monolithic fuel plate assembly was fabricated by sequential process of (1) co-rolling to laminate the Zr barrier onto the U10Mo fuel alloy and (2) HIP to encase the fuel laminated with Zr, within the Al-alloy 6061 (AA6061). In this study, HIP process was carried out as functions of temperature (520, 540, 560 and 580 (&)deg;C for 90 minutes), time (45, 60, 90, 180 and 345 minutes at 560 (&)deg;C) with ramp-cool rate (35, 70 and 280 (&)deg;C/hour). At the interface between the U10Mo and Zr, following the co-rolling, the UZr2 phase was observed to develop adjacent to Zr, and the ?U phase was found between the UZr2 and U10Mo. Mo2Zr was found as precipitates mostly within the ?U phase. 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 kJ/mol. Decomposition of ?U into ?U and ?' was observed in the U10Mo alloy. The volume fraction of ? and ?' increased as the HIP temperature and ramp-cool rate decreased. The UC-UO2 inclusions within the U10Mo fuel alloy were observed, but the volume percent of the UC-UO2 inclusions within the U10Mo alloy, ranging from approximately 0.5 to 1.8, did not change as functions of HIP temperature and holding time. However, the inclusions located near the surface of the U10Mo alloy, were frequently observed to interfere the uniformity of interdiffusion and reaction between the U10Mo alloy and Zr diffusion barrier. The regions of limited interaction between the U10Mo and Zr barrier associated with UC-UO2 inclusions decreased with an increase in HIP temperature, however no significant trend was observed with an increase in HIP duration at 560 (&)deg;C.
Identifier: CFE0006371 (IID), ucf:51499 (fedora)
Note(s): 2016-08-01
Ph.D.
Engineering and Computer Science, Materials Science Engineering
Doctoral
This record was generated from author submitted information.
Subject(s): Phase transformation -- interdiffusion -- diffusion -- kinetics -- uranium -- zirconium
Persistent Link to This Record: http://purl.flvc.org/ucf/fd/CFE0006371
Restrictions on Access: public 2016-08-15
Host Institution: UCF

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