Analysis of Molecular Interactions between Components in Phospholipid-Immunosuppressant-Antioxidant Mixed Langmuir Films

Jurak, M. ; Szafran, K. ; Cea, P. (Universidad de Zaragoza) ; Martín, S. (Universidad de Zaragoza)

Resumen: The study of Langmuir monolayers incorporating biomimetic and bioactive substances plays an important role today in assessing the properties and quality of the molecular films for potential biomedical applications. Here, miscibility of binary and ternary monolayers of phospholipid (dioleoyl phosphatidylcholine, DOPC), immunosuppressant (cyclosporine A, CsA), and antioxidant (lauryl gallate, LG) of varying molar fractions was analyzed by means of the Langmuir technique coupled with a surface potential (?V) module at the air-water interface. The surface pressure-area per molecule (?-A) isotherms provided information on the physical state of the films at a given surface pressure, the monolayer packing and ordering, and the type and strength of intermolecular interactions. Surface potential-area (?V-A) isotherms revealed the molecular orientation changes at the interface upon compression. In addition, the apparent dipole moment of the monolayer-forming molecules was determined from the surface potential isotherms. The obtained results indicated that the film compression provoked subsequent changes of CsA conformation and/or orientation, conferring better affinity for the hydrocarbon environment. The mutual interactions between the components were analyzed here in terms of the excess and total Gibbs energy of mixing, whose values depended on the stoichiometry of the mixed films. The strongest attraction, thus the highest thermodynamic stability, was found for a DOPC-CsA-LG mixture with a 1:1:2 molar ratio. Based on these results, a molecular model for the organization of the molecules within the Langmuir film was proposed. Through this model, we elucidated the significant role of LG in improving the miscibility of CsA in the model DOPC membrane and thus in increasing the stability of self-assembled monolayers by noncovalent interactions, such as H-bonds and Lifshitz-van der Waals forces. The above 1:1:2 combination of three components is revealed as the most promising film composition for the modification of implant device surfaces to improve their biocompatibility. Further insight into mechanisms concerning drug-membrane interactions at the molecular level is provided, which results in great importance for biocoating design and development as well as for drug release at target sites. © 2021 American Chemical Society. All rights reserved.

Idioma: Inglés

DOI: 10.1021/acs.langmuir.1c00434

Año: 2021

Publicado en: Langmuir 37, 18 (2021), 5601-5616
ISSN: 0743-7463

Factor impacto JCR: 4.331 (2021)

Categ. JCR: CHEMISTRY, PHYSICAL rank: 74 / 165 = 0.448 (2021) - Q2 - T2
Categ. JCR: CHEMISTRY, MULTIDISCIPLINARY rank: 72 / 179 = 0.402 (2021) - Q2 - T2
Categ. JCR: MATERIALS SCIENCE, MULTIDISCIPLINARY rank: 138 / 344 = 0.401 (2021) - Q2 - T2

Factor impacto CITESCORE: 6.7 - Physics and Astronomy (Q1) - Materials Science (Q1)

Factor impacto SCIMAGO: 0.884 - Condensed Matter Physics (Q1) - Electrochemistry (Q1) - Surfaces and Interfaces (Q1) - Spectroscopy (Q1) - Materials Science (miscellaneous) (Q1)

Financiación: info:eu-repo/grantAgreement/ES/DGA/E21-20R
Financiación: info:eu-repo/grantAgreement/EUR/ERA-NET-COFUND/MagicCellGene Project 2016
Financiación: info:eu-repo/grantAgreement/ES/MINECO/PCIN-2017-127

Tipo y forma: Artículo (Versión definitiva)

Área (Departamento): Área Química Física (Dpto. Química Física)