Analysis of differential scanning calorimetry data for aged plutonium

Chiravalle, Vincent P.

doi:10.1063/5.0234018

Title: Analysis of differential scanning calorimetry data for aged plutonium

Journal Article · 23 October 2024 · Journal of Chemical Physics

DOI: https://doi.org/10.1063/5.0234018 · OSTI ID:2475581

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Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)

Differential scanning calorimetry data for samples of a 52 year old plutonium alloy with 3.3 at. % Ga that were heated beyond the melting point is analyzed using transition state theory to find activation energies for the δ to ε and ε to liquid phase transitions. A Bayesian statistical method involving a Gaussian process model is used to find mean values and confidence intervals for the activation energies. The activation energy for the δ to ε phase transition increases by 3.3 ± 3.8% per decade, relative to the case when all age related plutonium lattice point defects have been removed through annealing. The corresponding increase in activation energy for the ε to liquid transition is shown to be 7.1 ± 1.8% per decade. It is postulated that the change in activation energy with age for both phase transitions is caused, in part, by the accumulation of the same type of lattice point defects associated with the observed increase in elastic bulk modulus over time.

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Research Organization:: Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)

Sponsoring Organization:: USDOE

Grant/Contract Number:: 89233218CNA000001

OSTI ID:: 2475581

Report Number(s):: LA-UR--23-32538

Journal Information:: Journal of Chemical Physics, Journal Name: Journal of Chemical Physics Journal Issue: 16 Vol. 161; ISSN 0021-9606

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

References (28)

Analysis of the kinetics of phase transformations Mittemeijer, E. J. Journal of Materials Science, Vol. 27, Issue 15 https://doi.org/10.1007/bf01105093	journal	January 1992
Study of the effective phase transition activation energy in K2SeO4 crystals El-Korashy, A.; Afify, N. Journal of Thermal Analysis, Vol. 37, Issue 3 https://doi.org/10.1007/bf01913101	journal	March 1991
Atomistic study of small helium bubbles in plutonium Ao, B. Y.; Wang, X. L.; Hu, W. Y. Journal of Alloys and Compounds, Vol. 444-445 https://doi.org/10.1016/j.jallcom.2006.11.077	journal	October 2007
Evaluation of the nucleation and growth of helium bubbles in aged plutonium Wheeler, D. W.; Bayer, P. D. Journal of Alloys and Compounds, Vol. 444-445 https://doi.org/10.1016/j.jallcom.2007.01.038	journal	October 2007
Probing thermodynamics of radiogenic helium and defects in δ-plutonium alloys and interactions with adsorbed environmental gases Wayne, David M.; Hernandez, Sarah C.; Abdul-Jabbar, Najeb M. Journal of Alloys and Compounds, Vol. 998 https://doi.org/10.1016/j.jallcom.2024.174903	journal	September 2024
Investigation of plutonium allotropic phase transformations through differential scanning calorimetry Zocco, T. G.; Schwartz, D. S.; Park, J. Journal of Nuclear Materials, Vol. 353, Issue 1-2 https://doi.org/10.1016/j.jnucmat.2006.02.085	journal	July 2006
Molecular dynamics simulation of helium–vacancy interaction in plutonium Ao, Bingyun; Wang, Xiaolin; Hu, Wangyu Journal of Nuclear Materials, Vol. 385, Issue 1 https://doi.org/10.1016/j.jnucmat.2008.09.034	journal	March 2009
Molecular dynamics characterization of thermodynamic and mechanical properties of Pu as dependent upon alloying additions and defects concentration. Part I Dremov, V. V.; Karavaev, A. V.; Samarin, S. I. Journal of Nuclear Materials, Vol. 385, Issue 1 https://doi.org/10.1016/j.jnucmat.2008.10.037	journal	March 2009
He migration and bubble formation in Ga stabilised δ-Pu Robinson, M.; Kenny, S. D.; Smith, R. Journal of Nuclear Materials, Vol. 444, Issue 1-3 https://doi.org/10.1016/j.jnucmat.2013.10.017	journal	January 2014
Thermodynamic re-assessment of the Pu–U system and its application to the ternary Pu–U–Ga system Perron, A.; Turchi, P. E. A.; Landa, A. Journal of Nuclear Materials, Vol. 454, Issue 1-3 https://doi.org/10.1016/j.jnucmat.2014.07.051	journal	November 2014
Phase stability of an aged Pu–0.27 wt.% Ga alloy Wheeler, D. W.; Ennaceur, S. M.; Matthews, M. B. Journal of Nuclear Materials, Vol. 456 https://doi.org/10.1016/j.jnucmat.2014.09.005	journal	January 2015
Effects of self-irradiation in plutonium alloys Chung, B. W.; Lema, K. E.; Allen, P. G. Journal of Nuclear Materials, Vol. 471 https://doi.org/10.1016/j.jnucmat.2015.09.028	journal	April 2016
Atomistic simulations of dislocation dynamics in δ -Pu-Ga alloys Karavaev, A. V.; Dremov, V. V.; Ionov, G. V. Journal of Nuclear Materials, Vol. 496 https://doi.org/10.1016/j.jnucmat.2017.09.005	journal	December 2017
Density functional theory study of defects in unalloyed δ-Pu Hernandez, S. C.; Freibert, F. J.; Wills, J. M. Scripta Materialia, Vol. 134 https://doi.org/10.1016/j.scriptamat.2017.02.025	journal	June 2017
A differential scanning calorimetry study of the kinetics of the β→γ phase transformation in plutonium Ennaceur, S. M. Thermochimica Acta, Vol. 547 https://doi.org/10.1016/j.tca.2012.08.014	journal	November 2012
Study of the γ→δ phase transformation kinetics and reaction mechanism in plutonium Ennaceur, S. M. Thermochimica Acta, Vol. 566 https://doi.org/10.1016/j.tca.2013.05.042	journal	August 2013
Reaction Kinetics in Differential Thermal Analysis Kissinger, H. E. Analytical Chemistry, Vol. 29, Issue 11 https://doi.org/10.1021/ac60131a045	journal	November 1957
Rate of Nucleation in Condensed Systems Turnbull, D.; Fisher, J. C. The Journal of Chemical Physics, Vol. 17, Issue 1 https://doi.org/10.1063/1.1747055	journal	January 1949
The Activated Complex in Chemical Reactions Eyring, Henry The Journal of Chemical Physics, Vol. 3, Issue 2 https://doi.org/10.1063/1.1749604	journal	February 1935
The Thermodynamic Properties of the f-Elements and Their Compounds. I. The Lanthanide and Actinide Metals Konings, Rudy J. M.; Beneš, Ondrej Journal of Physical and Chemical Reference Data, Vol. 39, Issue 4 https://doi.org/10.1063/1.3474238	journal	December 2010
Elastic moduli of δ-Pu ²³⁹ reveal aging in real time Maiorov, Boris; Betts, Jonathan B.; Söderlind, Per Journal of Applied Physics, Vol. 121, Issue 12 https://doi.org/10.1063/1.4978509	journal	March 2017
A Critical Review of the Experimentally Known Properties of U-Pu-Zr Alloys. Part 1: Phases and Phase Diagrams Janney, Dawn E.; Hayes, Steven L.; Adkins, Cynthia A. Nuclear Technology, Vol. 205, Issue 11 https://doi.org/10.1080/00295450.2019.1578573	journal	May 2019
Characterization and modelling of helium bubbles in self-irradiated plutonium alloys Schwartz *, A. J.; Wall, M. A.; Zocco, T. G. Philosophical Magazine, Vol. 85, Issue 4-7 https://doi.org/10.1080/02678370412331320026	journal	February 2005
Toward an understanding of aging in plutonium from direct measurements of stored energy Ennaceur, S. M.; Migliori, A. Philosophical Magazine Letters, Vol. 98, Issue 11 https://doi.org/10.1080/09500839.2019.1583392	journal	November 2018
The long-range forces between dislocation loops and dislocations Makin, M. J. The Philosophical Magazine: A Journal of Theoretical Experimental and Applied Physics, Vol. 10, Issue 106 https://doi.org/10.1080/14786436408228488	journal	October 1964
Atomistic model of helium bubbles in gallium-stabilized plutonium alloys Valone, S. M.; Baskes, M. I.; Martin, R. L. Physical Review B, Vol. 73, Issue 21 https://doi.org/10.1103/physrevb.73.214209	journal	June 2006
Combining experimental data and computer simulations, with an application to flyer plate experiments Williams, Brian; Higdon, Dave; Gattiker, Jim Bayesian Analysis, Vol. 1, Issue 4 https://doi.org/10.1214/06-ba125	journal	December 2006
Nonisothermal Crystallization Kinetics by DSC: Practical Overview Vyazovkin, Sergey; Sbirrazzuoli, Nicolas Processes, Vol. 11, Issue 5 https://doi.org/10.3390/pr11051438	journal	May 2023

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Gaussian processes
bulk modulus
chemical elements
crystallographic defects
data science
differential scanning calorimetry
mechanical stress
phase transitions
statistical analysis
transition state theory

Title: Analysis of differential scanning calorimetry data for aged plutonium

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