Analysis of differential scanning calorimetry data for aged plutonium

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 ɛ and ɛ 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 ɛ 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 ɛ 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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Publication Details

Journal
The Journal of Chemical Physics
Published
2024-10-23
DOI
https://doi.org/10.1063/5.0234018
Primary Topic
Nuclear Materials and Properties
Type
article
Field-Weighted Citation Impact
0.00

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article

Analysis of differential scanning calorimetry data for aged plutonium

Vincent Chiravalle
The Journal of Chemical Physics
Nuclear Materials and Properties
article

Analysis of differential scanning calorimetry data for aged plutonium

Vincent Chiravalle
article en

Abstract

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 ɛ and ɛ 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 ɛ 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 ɛ 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.

The Journal of Chemical PhysicsVol. 161(16)
Los Alamos National Laboratory (US)
U.S. Department of Energy, National Nuclear Security Administration, Los Alamos National Laboratory
Affordable and clean energy
Openalex Percentile: Top 88%
Nuclear Materials and Properties
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