Unsteady State Performance and Stabilization Time in Square Cascades for Stable Krypton Isotope Separation

Document Type : Research Article

Authors

1 Nuclear Fuel Cycle Research School, Nuclear Science and Technology Research Institute, Tehran, Iran.

2 Reactor and Nuclear Safety Research School, Nuclear Science and Technology Research Institute, Isfahan, Iran.

Abstract

The inherently low single stage separation factor of stable krypton isotopes makes their enrichment through multistage cascades a challenging task, requiring precise optimization of cascade parameters and a thorough understanding of transient behavior. In this work, we numerically investigate the unsteady state performance of a square cascade for krypton isotope separation, using a multicomponent mass balance model discretized by the Crank–Nicolson scheme and solved iteratively via a q method. The study focuses on how two key design variables—the cascade cut (θ) and the unit separation factor (α)—affect the stabilization time of individual isotopes and of the entire system. Simulations are conducted for θ = 0.142 (targeting light isotopes in the product) and θ = 0.827 (targeting heavy isotopes in the waste), at α = 1.2 and 1.4. Results reveal that the isotope governing the overall transient response is not fixed: at low cut, intermediate isotope Kr 82 controls the stabilization (≈184 min), whereas at high cut, the heaviest isotope Kr 86 becomes the rate limiting component (≈150–884 min depending on α). Increasing α from 1.2 to 1.4 substantially prolongs the global steady state attainment—from ~190 to ~481 min at θ = 0.142, and from ~156 to ~941 min at θ = 0.827—due to sharper concentration gradients and stronger interstage coupling. These findings demonstrate that steady state analysis alone is insufficient for cascade design; transient simulation is essential to correctly identify the bottleneck isotope and to optimize start up strategies.

Keywords


[1] Bruntz, R.C., Lane, A.N., Higashi, R.M., Fan, T.W.-M., 2017. Exploring cancer metabolism using stable isotope-resolved metabolomics (SIRM), Journal of Biological Chemistry, 292 (28), 11601–11609. https://doi.org/10.1074/jbc.R117.776054
[2] Schmidt, D.R., Patel, R., Kirsch, D.G., Lewis, C.A., Vander Heiden, M.G., Locasale, J.W., 2021. Metabolomics in cancer research and emerging applications in clinical oncology, CA: A Cancer Journal for Clinicians, 71 (4), 333–358. https://doi.org/10.3322/caac.21670
[3] Hammer, H.F., Fox, M.R., Keller, J., Salvatore, S., Basilisco, G., Hammer, J., Lopetuso, L., Benninga, M., Borrelli, O., Dumitrascu, D., Hauser, B., Herszenyi, L., Nakov, R., Pohl, D., Thapar, N., Sonyi, M., European H2-CH4-breath test group, 2022. European guideline on indications, performance, and clinical impact of hydrogen and methane breath tests in adult and pediatric patients: European Association for Gastroenterology, Endoscopy and Nutrition, European Society of Neurogastroenterology and Motility, and European Society for Paediatric Gastroenterology Hepatology and Nutrition consensus, United European Gastroenterology Journal, 10 (1), 15–40. https://doi.org/10.1002/ueg2.12133
[4] Lemos, F.F.B., de Castro, C.T., Luz, M.S., Rocha, G.R., Santos, G.L.C., de Oliveira Silva, L.G., Calmon, M.S., Souza, C.L., Zarpelon-Schutz, A.C., Teixeira, K.N., Queiroz, D.M.M., de Melo, F.F., 2024. Urea breath test for Helicobacter pylori infection in adult dyspeptic patients: A meta-analysis of diagnostic test accuracy, World Journal of Gastroenterology, 30 (6), 579. https://doi.org/10.3748/wjg.v30.i6.579
[5] Speakman, J.R., Yamada, Y., Sagayama, H., Berman, E.S., Ainslie, P.N., Andersen, L.F., et al., 2021. A standard calculation methodology for human doubly labeled water studies, Cell Reports Medicine, 2 (2), 100203. https://doi.org/10.1016/j.xcrm.2021.100203
[6] Liu, H., Nie, J., Liu, Y., Wadood, S.A., Rogers, K.M., Yuan, Y., Gan, R.-Y., 2023. A review of recent compound-specific isotope analysis studies applied to food authentication, Food Chemistry, 415, 135791. https://doi.org/10.1016/j.foodchem.2023.135791
[7] Seltzer, A.M., Severinghaus, J.P., Andraski, B.J., Stonestrom, D.A., 2017. Steady state fractionation of heavy noble gas isotopes in a deep unsaturated zone, Water Resources Research, 53 (4), 2716–2732. https://doi.org/10.1002/2016WR019655
[8] Tyroller, L., Brennwald, M.S., Busemann, H., Maden, C., Baur, H., Kipfer, R., 2018. Negligible fractionation of Kr and Xe isotopes by molecular diffusion in water, Earth and Planetary Science Letters, 492, 73–78. https://doi.org/10.1016/j.epsl.2018.03.047
[9] Ng, J., Tyne, R., Seltzer, A., Noyes, C., McIntosh, J., Severinghaus, J., 2023. A new large-volume equilibration method for high-precision measurements of dissolved noble gas stable isotopes, Rapid Communications in Mass Spectrometry, 37 (7), e9471. https://doi.org/10.1002/rcm.9471
[10] Cholach, A., Yakovin, D., Latkin, N., Sidorov, I., 2023. Freezing-out of heavy isotopes of Kr, arXiv preprint, arXiv:2311.18404. https://doi.org/10.48550/arXiv.2311.18404
[11] Garza Adl, G.A., Garrett, G.A., Murphy, J.E., 1962. Multicomponent isotope separation in cascades, Chemical Engineering Science, 15 (3–4), 188–209. https://doi.org/10.1016/0009-2509(61)85023-9
[12] Khooshechin, S., Mansourzadeh, F., Imani, M., Safdari, J., Mallah, M.H., 2021. Optimization of flexible square cascade for high separation of stable isotopes using enhanced PSO algorithm, Progress in Nuclear Energy, 140, 103922. https://doi.org/10.1016/j.pnucene.2021.103922
[13] Shadman, M.M., Ghazanfari, V., Amini, Y., Mansourzadeh, F., Khamseh, A.G., Khani, M.H., Hassanvand, A., Heydari, M., 2023. Optimal time separation modeling and simulation for stable neon isotopes in a transient square cascade: A comprehensive study, SN Applied Sciences, 5 (12), 361. https://doi.org/10.1007/s42452-023-05589-0
[14] Zeng, S., Ying, C., 2000. A second-order time-accurate method for determination of concentration distribution of multicomponent mixtures in separation cascades, Separation Science and Technology, 35 (5), 729–741. https://doi.org/10.1081/SS-100100187