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Title: Geometry-Dependent Nonequilibrium Steady-State Diffusion and Adsorption of Lipid Vesicles in Micropillar Arrays

Abstract

Micro-and nanofabricated sample environments are useful tools for characterizing diffusion in confined aqueous environments. The steady-state diffusion and adsorption of unilamellar lipid vesicles in arrays of hydrophilic micropillars is investigated. Gradients in the coverage of fluorescently labeled, pillar-supported lipid films, formed from vesicle fusion, are determined from 3D z-stack images using confocal microscopy. The gradients are the result of preferential adsorption of vesicles near the tops of the pillars, which progressively deplete them from solution as they diffuse toward the base of the array. However, the increased propensity for vesicle adsorption near the pillar tops compared to the confined spaces between pillars results in the formation of confluent supported lipid bilayers at the pillar tops that resist the adsorption of additional vesicles while leaving the pillar surfaces below available for binding. This results in a reduction in the numbers of depleted vesicles compared to what one would anticipate based on diffusive fluxes. The resulting inhomogeneous spatial profiles of lipid structures on the pillars are the result of the system being maintained in a dissipative, nonequilibrium steady state during incubation of the pillar arrays in the vesicle solution, which is ultimately quenched by rinsing away the unbound, freely diffusing vesicles.

Authors:
ORCiD logo [1];  [2]; ORCiD logo [1]; ORCiD logo [1];  [3]; ORCiD logo [1]; ORCiD logo [1]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  2. Univ. of Tennessee, Knoxville, TN (United States)
  3. Eastern Tennessee State Univ., Johnson City, TN (United States)
Publication Date:
Research Org.:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1546529
Alternate Identifier(s):
OSTI ID: 1501712
Grant/Contract Number:  
AC05-00OR22725; DE‐AC05‐00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Advanced Materials Interfaces
Additional Journal Information:
Journal Volume: 6; Journal Issue: 9; Journal ID: ISSN 2196-7350
Publisher:
Wiley-VCH
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Liu, Fangjie, Abel, Steven M., Collins, Liam F., Srijanto, Bernadeta R., Standaert, Robert, Katsaras, John, and Collier, Pat. Geometry-Dependent Nonequilibrium Steady-State Diffusion and Adsorption of Lipid Vesicles in Micropillar Arrays. United States: N. p., 2019. Web. doi:10.1002/admi.201900054.
Liu, Fangjie, Abel, Steven M., Collins, Liam F., Srijanto, Bernadeta R., Standaert, Robert, Katsaras, John, & Collier, Pat. Geometry-Dependent Nonequilibrium Steady-State Diffusion and Adsorption of Lipid Vesicles in Micropillar Arrays. United States. https://doi.org/10.1002/admi.201900054
Liu, Fangjie, Abel, Steven M., Collins, Liam F., Srijanto, Bernadeta R., Standaert, Robert, Katsaras, John, and Collier, Pat. Mon . "Geometry-Dependent Nonequilibrium Steady-State Diffusion and Adsorption of Lipid Vesicles in Micropillar Arrays". United States. https://doi.org/10.1002/admi.201900054. https://www.osti.gov/servlets/purl/1546529.
@article{osti_1546529,
title = {Geometry-Dependent Nonequilibrium Steady-State Diffusion and Adsorption of Lipid Vesicles in Micropillar Arrays},
author = {Liu, Fangjie and Abel, Steven M. and Collins, Liam F. and Srijanto, Bernadeta R. and Standaert, Robert and Katsaras, John and Collier, Pat},
abstractNote = {Micro-and nanofabricated sample environments are useful tools for characterizing diffusion in confined aqueous environments. The steady-state diffusion and adsorption of unilamellar lipid vesicles in arrays of hydrophilic micropillars is investigated. Gradients in the coverage of fluorescently labeled, pillar-supported lipid films, formed from vesicle fusion, are determined from 3D z-stack images using confocal microscopy. The gradients are the result of preferential adsorption of vesicles near the tops of the pillars, which progressively deplete them from solution as they diffuse toward the base of the array. However, the increased propensity for vesicle adsorption near the pillar tops compared to the confined spaces between pillars results in the formation of confluent supported lipid bilayers at the pillar tops that resist the adsorption of additional vesicles while leaving the pillar surfaces below available for binding. This results in a reduction in the numbers of depleted vesicles compared to what one would anticipate based on diffusive fluxes. The resulting inhomogeneous spatial profiles of lipid structures on the pillars are the result of the system being maintained in a dissipative, nonequilibrium steady state during incubation of the pillar arrays in the vesicle solution, which is ultimately quenched by rinsing away the unbound, freely diffusing vesicles.},
doi = {10.1002/admi.201900054},
journal = {Advanced Materials Interfaces},
number = 9,
volume = 6,
place = {United States},
year = {Mon Mar 18 00:00:00 EDT 2019},
month = {Mon Mar 18 00:00:00 EDT 2019}
}

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Works referenced in this record:

Model membrane systems and their applications
journal, December 2007


Nanotechnology in Drug Delivery and Tissue Engineering: From Discovery to Applications
journal, September 2010

  • Shi, Jinjun; Votruba, Alexander R.; Farokhzad, Omid C.
  • Nano Letters, Vol. 10, Issue 9
  • DOI: 10.1021/nl102184c

Targeted Delivery of Protein Drugs by Nanocarriers
journal, March 2010

  • Solaro, Roberto; Chiellini, Federica; Battisti, Antonella
  • Materials, Vol. 3, Issue 3
  • DOI: 10.3390/ma3031928

Size and mobility of lipid domains tuned by geometrical constraints
journal, July 2017

  • Schütte, Ole M.; Mey, Ingo; Enderlein, Jörg
  • Proceedings of the National Academy of Sciences, Vol. 114, Issue 30
  • DOI: 10.1073/pnas.1704199114

Diffusive dynamics of nanoparticles in ultra-confined media
journal, January 2015

  • Jacob, Jack Deodato C.; He, Kai; Retterer, Scott T.
  • Soft Matter, Vol. 11, Issue 38
  • DOI: 10.1039/C5SM01437A

Studies of Bilayers and Vesicle Adsorption to Solid Substrates: Development of a Miniature Streaming Potential Apparatus (SPA)
journal, June 2010

  • Min, Younjin; Pesika, Noshir; Zasadzinski, Joe
  • Langmuir, Vol. 26, Issue 11
  • DOI: 10.1021/la904842v

Formation of Solid-Supported Lipid Bilayers:  An Integrated View
journal, April 2006

  • Richter, Ralf P.; Bérat, Rémi; Brisson, Alain R.
  • Langmuir, Vol. 22, Issue 8
  • DOI: 10.1021/la052687c

Diffusive Dynamics of Nanoparticles in Arrays of Nanoposts
journal, May 2013

  • He, Kai; Babaye Khorasani, Firoozeh; Retterer, Scott T.
  • ACS Nano, Vol. 7, Issue 6
  • DOI: 10.1021/nn4007303

Microfluidic Mixing: A Review
journal, May 2011

  • Lee, Chia-Yen; Chang, Chin-Lung; Wang, Yao-Nan
  • International Journal of Molecular Sciences, Vol. 12, Issue 5
  • DOI: 10.3390/ijms12053263

Liposome-Templated Hydrogel Nanoparticles as Vehicles for Enzyme-Based Therapies
journal, July 2015


A Monte Carlo simulation study of lipid bilayer formation on hydrophilic substrates from vesicle solutions
journal, February 2006

  • Zheng, Zheming; Stroumpoulis, Dimitrios; Parra, Alejandro
  • The Journal of Chemical Physics, Vol. 124, Issue 6
  • DOI: 10.1063/1.2166392

Core/Shell Nanofibers with Embedded Liposomes as a Drug Delivery System
journal, March 2012

  • Mickova, Andrea; Buzgo, Matej; Benada, Oldrich
  • Biomacromolecules, Vol. 13, Issue 4
  • DOI: 10.1021/bm2018118

Micro-motors: A motile bacteria based system for liposome cargo transport
journal, July 2016

  • Dogra, Navneet; Izadi, Hadi; Vanderlick, T. Kyle
  • Scientific Reports, Vol. 6, Issue 1
  • DOI: 10.1038/srep29369

Transport and Dispersion of Nanoparticles in Periodic Nanopost Arrays
journal, April 2014

  • He, Kai; Retterer, Scott T.; Srijanto, Bernadeta R.
  • ACS Nano, Vol. 8, Issue 5
  • DOI: 10.1021/nn404497z

Bilayer Thickness Mismatch Controls Domain Size in Model Membranes
journal, February 2013

  • Heberle, Frederick A.; Petruzielo, Robin S.; Pan, Jianjun
  • Journal of the American Chemical Society, Vol. 135, Issue 18
  • DOI: 10.1021/ja3113615

Molecular dynamics simulations of electrophoresis of polyelectrolytes in nano confining cylindrical geometries
journal, March 2013

  • Nedelcu, S.; Sommer, J. -U.
  • The Journal of Chemical Physics, Vol. 138, Issue 10
  • DOI: 10.1063/1.4794195

Lipid vesicles and other colloids as drug carriers on the skin
journal, March 2004


Effect of cytoskeletal geometry on intracellular diffusion
journal, November 1989


Kinetics of Langmuirian Adsorption onto Planar, Spherical, and Cylindrical Surfaces
journal, August 1999

  • Kankare, Jouko; Vinokurov, Igor A.
  • Langmuir, Vol. 15, Issue 17
  • DOI: 10.1021/la981642r

Diffusion in macromolecular crowded media: Monte Carlo simulation of obstructed diffusion vs. FRAP experiments
journal, November 2010

  • Vilaseca, Eudald; Pastor, Isabel; Isvoran, Adriana
  • Theoretical Chemistry Accounts, Vol. 128, Issue 4-6
  • DOI: 10.1007/s00214-010-0840-5

Diffusion in Confined Geometries
journal, January 2009

  • Burada, P. Sekhar; Hänggi, Peter; Marchesoni, Fabio
  • ChemPhysChem, Vol. 10, Issue 1
  • DOI: 10.1002/cphc.200800526

Simulation of adsorption kinetics of lipid vesicles
journal, January 2000

  • Zhdanov, V. P.; Keller, C. A.; Glasmästar, K.
  • The Journal of Chemical Physics, Vol. 112, Issue 2
  • DOI: 10.1063/1.480617

Bilayer membrane interactions with nanofabricated scaffolds
journal, November 2015


Diffusion-limited adsorption to a spherical geometry: The impact of curvature and competitive time scales
journal, July 2010


Simplified Equation to Extract Diffusion Coefficients from Confocal FRAP Data: Simplified Confocal FRAP Analysis
journal, October 2012

  • Kang, Minchul; Day, Charles A.; Kenworthy, Anne K.
  • Traffic, Vol. 13, Issue 12
  • DOI: 10.1111/tra.12008

Biosensors based on nanomechanical systems
journal, January 2013

  • Tamayo, Javier; Kosaka, Priscila M.; Ruz, José J.
  • Chem. Soc. Rev., Vol. 42, Issue 3
  • DOI: 10.1039/C2CS35293A

Modeling of diffusion controlled drug delivery
journal, July 2012


Symmetry Breaking Instabilities in Dissipative Systems. II
journal, February 1968

  • Prigogine, I.; Lefever, R.
  • The Journal of Chemical Physics, Vol. 48, Issue 4
  • DOI: 10.1063/1.1668896

Solid supported lipid bilayers: From biophysical studies to sensor design
journal, November 2006


Macromolecular diffusion in the extracellular matrix measured by fluorescence correlation spectroscopy
journal, January 2008

  • Reitan, Nina Kristine; Juthajan, Aphirak; Lindmo, Tore
  • Journal of Biomedical Optics, Vol. 13, Issue 5
  • DOI: 10.1117/1.2982530

Confined Diffusion in Periodic Porous Nanostructures
journal, May 2011

  • Raccis, Riccardo; Nikoubashman, Arash; Retsch, Markus
  • ACS Nano, Vol. 5, Issue 6
  • DOI: 10.1021/nn200767x

Liposomes and nanoparticles: nanosized vehicles for drug delivery in cancer
journal, November 2009

  • Malam, Yogeshkumar; Loizidou, Marilena; Seifalian, Alexander M.
  • Trends in Pharmacological Sciences, Vol. 30, Issue 11
  • DOI: 10.1016/j.tips.2009.08.004

Stochastic theory of nonequilibrium steady states. Part II: Applications in chemical biophysics
journal, January 2012


Liposome: classification, preparation, and applications
journal, February 2013

  • Akbarzadeh, Abolfazl; Rezaei-Sadabady, Rogaie; Davaran, Soodabeh
  • Nanoscale Research Letters, Vol. 8, Issue 1
  • DOI: 10.1186/1556-276X-8-102

Lateral Diffusion Coefficients of an Eicosanyl-Based Bisglycerophosphocholine Determined by PFG-NMR and FRAP
journal, May 2007

  • Febo-Ayala, Wilma; Holland, David P.; Bradley, Scott A.
  • Langmuir, Vol. 23, Issue 11
  • DOI: 10.1021/la063720d

Liposomal drug delivery systems: From concept to clinical applications
journal, January 2013


Liposomes in tissue engineering and regenerative medicine
journal, December 2014

  • Monteiro, Nelson; Martins, Albino; Reis, Rui L.
  • Journal of The Royal Society Interface, Vol. 11, Issue 101
  • DOI: 10.1098/rsif.2014.0459

Fast Detection of Biomolecules in Diffusion-Limited Regime Using Micromechanical Pillars
journal, September 2011

  • Melli, Mauro; Scoles, Giacinto; Lazzarino, Marco
  • ACS Nano, Vol. 5, Issue 10
  • DOI: 10.1021/nn202224g

Nanoparticle diffusion in crowded and confined media
journal, January 2016

  • Babayekhorasani, Firoozeh; Dunstan, Dave E.; Krishnamoorti, Ramanan
  • Soft Matter, Vol. 12, Issue 40
  • DOI: 10.1039/C6SM01543C

Bilayer Thickness Mismatch Controls Domain Size in Model Membranes
journal, January 2014

  • Heberle, Frederick A.; Petruzielo, Robin S.; Pan, Jianjun
  • Biophysical Journal, Vol. 106, Issue 2
  • DOI: 10.1016/j.bpj.2013.11.1686