Abstract
In this study, we investigated uranium dioxide () dissolution under geological repository conditions by applying a three-dimensional (3D) thermal-chemical reactive transport model. The transport of chemical species and thermal conduction in fuel pellets and chemical dissolutions of were considered. The mathematical and numerical formulations of the model are described in the paper. reactions were modeled to demonstrate the validity of modeling reaction processes. dissolution under low (25°C) and high temperatures (250°C) was simulated, taking into account the changes in aqueous uranium species with temperature. The predicted lifetime of one pellet is greatly dependent on the temperature. To illustrate the effect of uranium species on reaction rates, numerical studies were conducted at the same temperatures but with different reaction types and chemical species. It was found that reactions that produce enhance the dissolution rates of by consuming the in solutions. dissolution with varying pH values was also modeled. When pH increased to 6, the average dissolution rate of a fuel pellet was eight times slower than it was at . Dissolution simulations were carried out on the images of fractured pellets. The impact of microfractures on dissolution was illustrated. The developed model is able to quantify dissolution behaviors and identify key parameters controlling the physiochemical processes involved. The model can be used as a predictive tool for applications such as spent fuel sequestration, contaminant transport, and geothermal resources development.
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Data Availability Statement
All the data within this article is available from the corresponding author upon reasonable request.
Acknowledgments
Research presented in this article was supported by the Laboratory Directed Research and Development (LDRD) program of Los Alamos National Laboratory (LANL) under Project No. 20180007 DR. LANL, an affirmative action/equal opportunity employer, is managed by Triad National Security, LLC, for the National Nuclear Security Administration of the US Department of Energy under Contract No. 89233218CNA000001.
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Published In
Journal of Energy Engineering
Volume 149 • Issue 2 • April 2023
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© 2022 American Society of Civil Engineers.
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Received: May 19, 2022
Accepted: Sep 22, 2022
Published online: Dec 23, 2022
Published in print: Apr 1, 2023
Discussion open until: May 23, 2023
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