Skip to main content
OSTI.GOVU.S. Department of Energy Office of Scientific and Technical Information
U.S. Department of Energy
Office of Scientific and Technical Information
 

Revisiting thermodynamics and kinetic diffusivities of uranium–niobium with Bayesian uncertainty analysis

Journal Article · · Calphad
; ; ; ; ; ; ; ; ; ; ; ; ;
In this paper, thermodynamic and kinetic diffusivities of uranium–niobium (U–Nb) are re-assessed by means of the CALPHAD (CALculation of PHAse Diagram) methodology. In order to improve the consistency and reliability of the assessments, first-principles calculations are coupled with CALPHAD. In particular, heats of formation of γ -U–Nb are estimated and verified using various density-functional theory (DFT) approaches. These thermochemistry data are then used as constraints to guide the thermodynamic optimization process in such a way that the mutual-consistency between first-principles calculations and CALPHAD assessment is satisfactory. In addition, long-term aging experiments are conducted in order to generate new phase equilibria data at the γ2/α+γ2 boundary. These data are meant to verify the thermodynamic model. Assessment results are generally in good agreement with experiments and previous calculations, without showing the artifacts that were observed in previous modeling. The mutual-consistent thermodynamic description is then used to evaluate atomic mobility and diffusivity of γ-U–Nb. Finally, Bayesian analysis is conducted to evaluate the uncertainty of the thermodynamic model and its impact on the system's phase stability.
Research Organization:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States); Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)
Sponsoring Organization:
National Science Foundation (NSF); USDOE National Nuclear Security Administration (NNSA); USDOE Office of Science (SC)
Grant/Contract Number:
AC02-05CH11231; AC52-06NA25396; AC52-07NA27344
OSTI ID:
1334151
Alternate ID(s):
OSTI ID: 1411073
OSTI ID: 1368005
OSTI ID: 1440946
Report Number(s):
LA-UR--16-22697; LLNL-JRNL--703367
Journal Information:
Calphad, Journal Name: Calphad Journal Issue: P2 Vol. 55; ISSN 0364-5916
Publisher:
ElsevierCopyright Statement
Country of Publication:
United States
Language:
English

References (48)

The effect of quench rate on the microstructure, mechanical properties, and corrosion behavior of U-6 wt pct Nb journal July 1984
The Bayesian approach to an internally consistent thermodynamic database: theory, database, and generation of phase diagrams journal October 1998
DRAM: Efficient adaptive MCMC journal December 2006
A “sub-regular” solution model and its application to some binary alloy systems journal March 1953
Phase transformations in a uranium + 14 at.% niobium alloy journal March 1980
Etude de l'autodiffusion de l'uranium en phase γ journal July 1959
Phase transformations and equilibrium structures in uranium-rich niobium alloys journal January 1964
Decomposition of gamma phase in a uranium-9.5 wt % niobium alloy journal August 1972
Investigation of thermodynamic properties of BCC solid solutions of uranium (II). The uranium-niobium system journal January 1975
Improvement of excess parameters from thermodynamic and phase diagram data by a sequential Bayes algorithm journal January 1991
SGTE data for pure elements journal October 1991
Optimization of thermodynamic data of the Ni–Si system journal October 1999
The Ringberg workshop 1997 on the application of computational thermodynamics journal March 2000
Thermo-Calc & DICTRA, computational tools for materials science journal June 2002
The Ringberg Workshop 1996 on solution modelling journal June 1997
Confidence intervals of calculated phase boundaries journal September 1997
A Bayesian approach to evaluating the uncertainty of thermodynamic data and phase diagrams journal September 2003
Atomic mobilities, diffusivities and their kinetic implications for U– (, Nb and Mo) bcc alloys journal June 2012
Efficient stochastic generation of special quasirandom structures journal September 2013
X-ray diffraction analyses of aged U–Nb alloys journal October 2007
Thermodynamic modeling of the U–Mn and U–Nb systems journal October 2008
Low temperature age hardening in U–13at.% Nb: An assessment of chemical redistribution mechanisms journal September 2009
The U–Ti system: Strengths and weaknesses of the CALPHAD method journal December 2011
Electron correlation and relativity of the 5f electrons in the U–Zr alloy system journal January 2014
Equation of State Calculations by Fast Computing Machines journal June 1953
Models for numerical treatment of multicomponent diffusion in simple phases journal August 1992
Phase-field models in materials science journal July 2009
Monte Carlo sampling methods using Markov chains and their applications journal April 1970
LII. An essay towards solving a problem in the doctrine of chances. By the late Rev. Mr. Bayes, F. R. S. communicated by Mr. Price, in a letter to John Canton, A. M. F. R. S journal January 1763
Special points for Brillouin-zone integrations journal June 1976
Ab initiomolecular dynamics for liquid metals journal January 1993
Ab initio molecular-dynamics simulation of the liquid-metal–amorphous-semiconductor transition in germanium journal May 1994
Coherent-Potential Approximation for a Nonoverlapping-Muffin-Tin-Potential Model of Random Substitutional Alloys journal March 1972
Projector augmented-wave method journal December 1994
Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set journal October 1996
From ultrasoft pseudopotentials to the projector augmented-wave method journal January 1999
Self-consistent supercell approach to alloys with local environment effects journal April 2012
Special quasirandom structures journal July 1990
Order- N Green's Function Technique for Local Environment Effects in Alloys journal May 1996
Phase-Field Models for Microstructure Evolution journal August 2002
Constitution of Binary Alloys journal January 1958
Discontinuous reactions in solids journal February 2001
DICTRA, a tool for simulation of diffusional transformations in alloys journal May 2000
The Nb-U (Niobium-Uranium) system journal June 1998
Isothermal Transformations of Uranium-- 13 Atomic Percent Niobium report January 1971
Alloys of uranium with zirconium, chromium, columbium vanadium, and molybdenum report June 1952
An Adaptive Metropolis Algorithm journal April 2001
Kinetics of Lamellar Decomposition Reactions in U-Nb Alloys journal June 2011

Cited By (3)

Sensitivity estimation for calculated phase equilibria text January 2020
Uncertainty Quantification and Propagation in Computational Materials Science and Simulation-Assisted Materials Design journal January 2020
Uncertainty quantification of the parameters and predictions of a phenomenological constitutive model for thermally induced phase transformation in Ni–Ti shape memory alloys journal February 2019

Similar Records

High-Temperature Thermodynamics of Uranium from Ab Initio Modeling
Journal Article · Mon Feb 06 19:00:00 EST 2023 · Applied Sciences · OSTI ID:1999713

Related Subjects

36 MATERIALS SCIENCE
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
71 CLASSICAL AND QUANTUM MECHANICS
GENERAL PHYSICS
75 CONDENSED MATTER PHYSICS
SUPERCONDUCTIVITY AND SUPERFLUIDITY
Bayesian
CALPHAD
DFT
Kinetic diffusivity
Metallic fuels
Thermodynamics
Uncertainty analysis
U–Nb
kinetic diffusivity
metallic fuels
thermodynamics
uncertainty analysis