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Organized Hybrid Molecular Films from Natural Phospholipids and Synthetic Block Copolymers: A Physicochemical Investigation

Cite this: Langmuir 2020, 36, 37, 10941–10951
Publication Date (Web):August 27, 2020
Copyright © 2020 American Chemical Society

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    In the last few years, hybrid lipid-copolymer assemblies have attracted increasing attention as possible two-dimensional (2D) membrane platforms, combining the biorelevance of the lipid building blocks with the stability and chemical tunability of copolymers. The relevance of these systems varies from fundamental studies on biological membrane-related phenomena to the construction of 2D complex devices for material science and biosensor technology. Both the fundamental understanding and the application of hybrid lipid-copolymer-supported bilayers require thorough physicochemical comprehension and structural control. Herein, we report a comprehensive physicochemical and structural characterization of hybrid monolayers at the air/water interface and of solid-supported hybrid membranes constituted by 1,2-dipalmitoyl-sn-glycero-3-phosphocholine (DPPC) and the block copolymer poly(butadiene-b-ethyleneoxide) (PBD-b-PEO). Hybrid lipid-copolymer supported bilayers (HSLBs) with variable copolymer contents were prepared through spontaneous rupture and fusion of hybrid vesicles onto a hydrophilic substrate. The properties of the thin films and the parent vesicles were probed through dynamic light scattering (DLS), differential scanning calorimetry (DSC), optical ellipsometry, quartz crystal microbalance with dissipation monitoring (QCM-D), and confocal scanning laser microscopy (CSLM). Stable, hybrid lipid/copolymer systems were obtained for a copolymer content of 10–65 mol %. In particular, DSC and CSLM show lateral phase separation in these hybrid systems. These results improve our fundamental understanding of HSLBs, which is necessary for future applications of hybrid systems as biomimetic membranes or as drug delivery systems, with additional properties with respect to phospholipid liposomes.

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    • Histograms of the intensity distribution for vesicles in water; derivation of eq 4; complete Π–A isothermal cycles; surface compressive modulus for the complete isothermal cycles; refractive index increments for pure DPPC and PBD-b-PEO solutions; ellipsometric studies for all of the monolayers; QCM-D-sensed mass for the supported bilayers; ellipsometric studies for all of the supported bilayers; and CSLM images for pure DPPC and PBD-b-PEO bilayers (PDF)

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    Cited By

    This article is cited by 9 publications.

    1. Samantha Micciulla, Philipp Gutfreund, Matej Kanduč, Leonardo Chiappisi. Pressure-Induced Phase Transitions of Nonionic Polymer Brushes. Macromolecules 2023, 56 (3) , 1177-1188.
    2. Yoo Kyung Go, Cecilia Leal. Polymer–Lipid Hybrid Materials. Chemical Reviews 2021, 121 (22) , 13996-14030.
    3. Efstathia Triantafyllopoulou, Dimitrios Selianitis, Anastasia Balafouti, Nefeli Lagopati, Maria Gazouli, Georgia Valsami, Stergios Pispas, Natassa Pippa. Fabricating hybrid DSPC:DOPC:P(OEGMA-co-LMA) structures: Self-assembly as the milestone of their performance. Colloids and Surfaces A: Physicochemical and Engineering Aspects 2024, 684 , 133015.
    4. Jacopo Cardellini, Arianna Balestri, Luca Comparini, Barbara Lonetti, Marco Brucale, Francesco Valle, Debora Berti, Costanza Montis. Controlling plasmonic suprastructures through self-assembly of gold nanoparticles with hybrid copolymer-lipid vesicles. Journal of Colloid and Interface Science 2024, 654 , 848-858.
    5. Rashmi Seneviratne, Georgina Coates, Zexi Xu, Caitlin E. Cornell, Rebecca F. Thompson, Amin Sadeghpour, Daniel P. Maskell, Lars J. C. Jeuken, Michael Rappolt, Paul A. Beales. High Resolution Membrane Structures within Hybrid Lipid‐Polymer Vesicles Revealed by Combining X‐Ray Scattering and Electron Microscopy. Small 2023, 19 (22)
    6. Arianna Balestri, Barbara Lonetti, Simon Harrisson, Barbara Farias-Mancilla, Junliang Zhang, Heinz Amenitsch, Ulrich S. Schubert, Carlos Guerrero-Sanchez, Costanza Montis, Debora Berti. Thermo-responsive lipophilic NIPAM-based block copolymers as stabilizers for lipid-based cubic nanoparticles. Colloids and Surfaces B: Biointerfaces 2022, 220 , 112884.
    7. Maryame Bina, Flavien Sciortino, Agata N. Mahrir. Phase separation in polymer-based biomimetic structures containing planar membranes. Biointerphases 2022, 17 (6) , 060802.
    8. Subhadeep Koner, Joseph Tawfik, Farzin Mashali, Kristen B. Kennison, William T. McClintic, Frederick A. Heberle, Yu-Ming Tu, Manish Kumar, Stephen A. Sarles. Homogeneous hybrid droplet interface bilayers assembled from binary mixtures of DPhPC phospholipids and PB-b-PEO diblock copolymers. Biochimica et Biophysica Acta (BBA) - Biomembranes 2022, 1864 (10) , 183997.
    9. Jacopo Cardellini, Arianna Balestri, Costanza Montis, Debora Berti. Advanced Static and Dynamic Fluorescence Microscopy Techniques to Investigate Drug Delivery Systems. Pharmaceutics 2021, 13 (6) , 861.

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