Stochastic optimization of a uranium oxide reaction mechanism using plasma flow reactor measurements

Finko, Mikhail; Koroglu, Batikan; Rodriguez, Kate E.; Rose, Timothy P.; Crowhurst, Jonathan C.; Curreli, Davide; Radousky, Harry B.; Knight, Kim B.

doi:10.1038/s41598-023-35355-6

Title: Stochastic optimization of a uranium oxide reaction mechanism using plasma flow reactor measurements

Journal Article · 07 June 2023 · Scientific Reports

DOI: https://doi.org/10.1038/s41598-023-35355-6 · OSTI ID:1984174

Finko, Mikhail; Koroglu, Batikan; Rodriguez, Kate E.; Rose, Timothy P.; Crowhurst, Jonathan C.; Curreli, Davide; Radousky, Harry B.; Knight, Kim B.

Abstract In this work, a coupled Monte Carlo Genetic Algorithm (MCGA) approach is used to optimize a gas phase uranium oxide reaction mechanism based on plasma flow reactor (PFR) measurements. The PFR produces a steady Ar plasma containing U, O, H, and N species with high temperature regions (3000–5000 K) relevant to observing UO formation via optical emission spectroscopy. A global kinetic treatment is used to model the chemical evolution in the PFR and to produce synthetic emission signals for direct comparison with experiments. The parameter space of a uranium oxide reaction mechanism is then explored via Monte Carlo sampling using objective functions to quantify the model-experiment agreement. The Monte Carlo results are subsequently refined using a genetic algorithm to obtain an experimentally corroborated set of reaction pathways and rate coefficients. Out of 12 reaction channels targeted for optimization, four channels are found to be well constrained across all optimization runs while another three channels are constrained in select cases. The optimized channels highlight the importance of the OH radical in oxidizing uranium in the PFR. This study comprises a first step toward producing a comprehensive experimentally validated reaction mechanism for gas phase uranium molecular species formation.

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Research Organization:: Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)

Sponsoring Organization:: USDOE; USDOE Laboratory Directed Research and Development (LDRD) Program; USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: AC52-07NA27344

OSTI ID:: 1984174

Report Number(s):: LLNL-JRNL-840534; 9293; PII: 35355

Journal Information:: Scientific Reports, Journal Name: Scientific Reports Journal Issue: 1 Vol. 13; ISSN 2045-2322

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United Kingdom

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
analytical chemistry
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Title: Stochastic optimization of a uranium oxide reaction mechanism using plasma flow reactor measurements

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