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Adsorption Kinetics Dictate Monolayer Self-Assembly for Both Lipid-In and Lipid-Out Approaches to Droplet Interface Bilayer Formation
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    Adsorption Kinetics Dictate Monolayer Self-Assembly for Both Lipid-In and Lipid-Out Approaches to Droplet Interface Bilayer Formation
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    Department of Mechanical, Aerospace, and Biomedical Engineering, University of Tennessee, Knoxville, Tennessee 37996, United States
    Department of Mechanical Science and Engineering, University of Illinois at Urbana—Champaign, Urbana, Illinois 61801, United States
    § Center for Nanophase Materials Sciences, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States
    *E-mail: [email protected] (S.A.S.).
    Other Access OptionsSupporting Information (1)

    Langmuir

    Cite this: Langmuir 2015, 31, 47, 12883–12893
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    https://doi.org/10.1021/acs.langmuir.5b02293
    Published November 10, 2015
    Copyright © 2015 American Chemical Society

    Abstract

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    The droplet interface bilayer (DIB)—a method to assemble planar lipid bilayer membranes between lipid-coated aqueous droplets—has gained popularity among researchers in many fields. Well-packed lipid monolayer on aqueous droplet–oil interfaces is a prerequisite for successfully assembling DIBs. Such monolayers can be achieved by two different techniques: “lipid-in”, in which phospholipids in the form of liposomes are placed in water, and “lipid-out”, in which phospholipids are placed in oil as inverse micelles. While both approaches are capable of monolayer assembly needed for bilayer formation, droplet pairs assembled with these two techniques require significantly different incubation periods and exhibit different success rates for bilayer formation. In this study, we combine experimental interfacial tension measurements with molecular dynamics simulations of phospholipids (DPhPC and DOPC) assembled from water and oil origins to understand the differences in kinetics of monolayer formation. With the results from simulations and by using a simplified model to analyze dynamic interfacial tensions, we conclude that, at high lipid concentrations common to DIBs, monolayer formation is simple adsorption controlled for lipid-in technique, whereas it is predominantly adsorption-barrier controlled for the lipid-out technique due to the interaction of interface-bound lipids with lipid structures in the subsurface. The adsorption barrier established in lipid-out technique leads to a prolonged incubation time and lower bilayer formation success rate, proving a good correlation between interfacial tension measurements and bilayer formation. We also clarify that advective flow expedites monolayer formation and improves bilayer formation success rate by disrupting lipid structures, rather than enhancing diffusion, in the subsurface and at the interface for lipid-out technique. Additionally, electrical properties of DIBs formed with varying lipid placement and type are characterized.

    Copyright © 2015 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.langmuir.5b02293.

    • Lipid-in solution preparation; lipid-out solution preparation; interfacial tension measurement; Figure S1, IFT data; DIB formation and contact angle measurement; electrical characterization of lipid bilayers; Figure S2, current-voltage curves; calculation of bilayer tension and adhesion energy for DIB; specific capacitance measurements; Figure S3, specific capacitance measurement procedure; MD simulation method; Figure S4, molecular dynamics system setup; Table S1, measured physical properties of DIBs; dynamic light scattering measurements of liposomes and inverse micelles; Figure S5, DLS measurements; additional IFT data for lipid-in and lipid-out conditions; Figure S6, interfacial tension versus time; interfacial tension measurement analysis; Figure S7, DPhPC-in surface pressure data and calculated fit; validity of model; Figure S8, comparison of experimental surface pressure and back-calculated surface pressure; limitations of model; Table S2, qualitative determination of suitable minimum lipid concentration; DOPC self-assembly free energy curves; Figure S9, free energy curves; and additional references (PDF)

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    Cited By

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    This article is cited by 59 publications.

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    Langmuir

    Cite this: Langmuir 2015, 31, 47, 12883–12893
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.langmuir.5b02293
    Published November 10, 2015
    Copyright © 2015 American Chemical Society

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