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Impact of Molecular Partitioning and Partial Equilibration on the Estimation of Diffusion Coefficients from Release Experiments

  • Reza Ghanbari
    Reza Ghanbari
    Food and Soft Materials Science, Department of Health Science & Technology, Institute of Food, Nutrition & Health, ETH Zurich, Schmelzbergstrasse 9, CH-8092 Zurich, Switzerland
  • Salvatore Assenza
    Salvatore Assenza
    Food and Soft Materials Science, Department of Health Science & Technology, Institute of Food, Nutrition & Health, ETH Zurich, Schmelzbergstrasse 9, CH-8092 Zurich, Switzerland
  • Patrick Zueblin
    Patrick Zueblin
    Food and Soft Materials Science, Department of Health Science & Technology, Institute of Food, Nutrition & Health, ETH Zurich, Schmelzbergstrasse 9, CH-8092 Zurich, Switzerland
  • , and 
  • Raffaele Mezzenga*
    Raffaele Mezzenga
    Food and Soft Materials Science, Department of Health Science & Technology, Institute of Food, Nutrition & Health, ETH Zurich, Schmelzbergstrasse 9, CH-8092 Zurich, Switzerland
    Department of Materials, ETH Zurich, Wolfgang-Pauli-Strasse 10, 8093 Zurich, Switzerland
    *E-mail: [email protected]
Cite this: Langmuir 2019, 35, 16, 5663–5671
Publication Date (Web):March 31, 2019
https://doi.org/10.1021/acs.langmuir.9b00510
Copyright © 2019 American Chemical Society

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    Abstract

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    The present work addresses the effect of partial equilibration and molecular partitioning on the interpretation of release experiments. In this regard, it is shown how release profiles and the values of extracted transport parameters are affected by the time protocol chosen for sample collection by considering a series of experiments where the latter is systematically varied. Caffeine is investigated as a main model drug because of its similar affinity for water and lipids, while monolinolein-based lipid cubic phases are chosen as host matrices because of their wide employment in release studies. Our findings point to a progressive decline in diffusion rate upon increasing the time step, that is, the gap in time between two consecutive pickups, which is a signature of increasing equilibration of caffeine concentration between the lipidic mesophase and the water phase. Furthermore, the amount of released molecules at the first pickup displays negligible changes for large time steps, indicating complete equilibration in such cases. A model is introduced based on Fick’s diffusion which goes beyond the assumption of perfect-sink conditions, a common feature of the typical theoretical approaches hitherto developed. The model is shown to account quantitatively for the experimental data and is subsequently employed to clarify the interplay of the adopted release protocol with the various transport parameters in determining the final outcome of the release process. Particularly, two additional molecular drugs are considered, namely glucose and proflavine, which are, respectively, more hydrophilic and hydrophobic than caffeine, thus allowing elucidating the role of molecular partitioning.

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.langmuir.9b00510.

    • SAXS data on bicontinuous cubic phases composed of caffeine solution with Ci = 1.0 mg/mL and Dimodan upon the equilibration step and SAXS data on bicontinuous cubic phases composed of caffeine solution and Dimodan before and after the Release experiment (PDF)

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    Cited By

    This article is cited by 5 publications.

    1. Yan Shan Loo, N. Idayu Zahid, Thiagarajan Madheswaran, Shinya Ikeno, Armania Nurdin, Intan Diana Mat Azmi. Coencapsulation of Gemcitabine and Thymoquinone in Citrem–Phosphatidylcholine Hexosome Nanocarriers Improves In Vitro Cellular Uptake in Breast Cancer Cells. Molecular Pharmaceutics 2023, 20 (9) , 4611-4628. https://doi.org/10.1021/acs.molpharmaceut.3c00333
    2. Antonio M. Bosch, Salvatore Assenza. Interplay of Hydropathy and Heterogeneous Diffusion in the Molecular Transport within Lamellar Lipid Mesophases. Pharmaceutics 2023, 15 (2) , 573. https://doi.org/10.3390/pharmaceutics15020573
    3. Thomas G Meikle, David W Keizer, Frances Separovic, Shenggen Yao. A solution NMR view of lipidic cubic phases: Structure, dynamics, and beyond. BBA Advances 2022, 2 , 100062. https://doi.org/10.1016/j.bbadva.2022.100062
    4. Thomas G. Meikle, David W. Keizer, Frances Separovic, Shenggen Yao. A Solution Nmr View of Lipidic Cubic Phases: Structure, Dynamics, And Beyond. SSRN Electronic Journal 2022, 220 https://doi.org/10.2139/ssrn.4169004
    5. S. Khorasani, A.P. Ghandehari Yazdi, E. Taghavi, M. Alipoor Amro Abadi, H. Ghobadi, B. Zihayat, B. Rasti, M.R. Mozafari. Recent Trends in the Nanoencapsulation Processes for Food and Nutraceutical Applications. 2021, 532-545. https://doi.org/10.1016/B978-0-08-100596-5.22940-5

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