skip to main content
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: The role of membrane fluidization in the gel-assisted formation of giant polymersomes

Abstract

Polymersomes are being widely explored as synthetic analogs of lipid vesicles based on their enhanced stability and potential uses in a wide variety of applications in (e.g., drug delivery, cell analogs, etc.). Controlled formation of giant polymersomes for use in membrane studies and cell mimetic systems, however, is currently limited by low-yield production methodologies. Here, we describe for the first time, how the size distribution of giant poly(ethylene glycol)-poly(butadiene) (PEO-PBD) polymersomes formed by gel-assisted rehydration may be controlled based on membrane fluidization. We first show that the average diameter and size distribution of PEO-PBD polymersomes may be readily increased by increasing the temperature of the rehydration solution. Further, we describe a correlative relationship between polymersome size and membrane fluidization through the addition of sucrose during rehydration, enabling the formation of PEO-PBD polymersomes with a range of diameters, including giant-sized vesicles (>100 μm). This correlative relationship suggests that sucrose may function as a small molecule fluidizer during rehydration, enhancing polymer diffusivity during formation and increasing polymersome size. Altogether the ability to easily regulate the size of PEO-PBD polymersomes based on membrane fluidity, either through temperature or fluidizers, has broadly applicability in areas including targeted therapeutic delivery and synthetic biology.

Authors:
ORCiD logo [1];  [1];  [1];  [1];  [1];  [1];  [2]
  1. Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
  2. Martin-Luther-Univ., Halle-Wittenberg (Germany)
Publication Date:
Research Org.:
Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1291338
Report Number(s):
SAND-2016-7533J
Journal ID: ISSN 1932-6203; 646370
Grant/Contract Number:  
AC04-94AL85000
Resource Type:
Accepted Manuscript
Journal Name:
PLoS ONE
Additional Journal Information:
Journal Volume: 11; Journal Issue: 7; Journal ID: ISSN 1932-6203
Publisher:
Public Library of Science
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; polymers; vesicles; fluorescence recovery after photobleaching; sucrose; lipids; gel electrophoresis; mass diffusivity; membrane potential

Citation Formats

Greene, Adrienne C., Henderson, Ian M., Gomez, Andrew, Paxton, Walter F., VanDelinder, Virginia, Bachand, George D., and Hinderberger, Dariush. The role of membrane fluidization in the gel-assisted formation of giant polymersomes. United States: N. p., 2016. Web. https://doi.org/10.1371/journal.pone.0158729.
Greene, Adrienne C., Henderson, Ian M., Gomez, Andrew, Paxton, Walter F., VanDelinder, Virginia, Bachand, George D., & Hinderberger, Dariush. The role of membrane fluidization in the gel-assisted formation of giant polymersomes. United States. https://doi.org/10.1371/journal.pone.0158729
Greene, Adrienne C., Henderson, Ian M., Gomez, Andrew, Paxton, Walter F., VanDelinder, Virginia, Bachand, George D., and Hinderberger, Dariush. Wed . "The role of membrane fluidization in the gel-assisted formation of giant polymersomes". United States. https://doi.org/10.1371/journal.pone.0158729. https://www.osti.gov/servlets/purl/1291338.
@article{osti_1291338,
title = {The role of membrane fluidization in the gel-assisted formation of giant polymersomes},
author = {Greene, Adrienne C. and Henderson, Ian M. and Gomez, Andrew and Paxton, Walter F. and VanDelinder, Virginia and Bachand, George D. and Hinderberger, Dariush},
abstractNote = {Polymersomes are being widely explored as synthetic analogs of lipid vesicles based on their enhanced stability and potential uses in a wide variety of applications in (e.g., drug delivery, cell analogs, etc.). Controlled formation of giant polymersomes for use in membrane studies and cell mimetic systems, however, is currently limited by low-yield production methodologies. Here, we describe for the first time, how the size distribution of giant poly(ethylene glycol)-poly(butadiene) (PEO-PBD) polymersomes formed by gel-assisted rehydration may be controlled based on membrane fluidization. We first show that the average diameter and size distribution of PEO-PBD polymersomes may be readily increased by increasing the temperature of the rehydration solution. Further, we describe a correlative relationship between polymersome size and membrane fluidization through the addition of sucrose during rehydration, enabling the formation of PEO-PBD polymersomes with a range of diameters, including giant-sized vesicles (>100 μm). This correlative relationship suggests that sucrose may function as a small molecule fluidizer during rehydration, enhancing polymer diffusivity during formation and increasing polymersome size. Altogether the ability to easily regulate the size of PEO-PBD polymersomes based on membrane fluidity, either through temperature or fluidizers, has broadly applicability in areas including targeted therapeutic delivery and synthetic biology.},
doi = {10.1371/journal.pone.0158729},
journal = {PLoS ONE},
number = 7,
volume = 11,
place = {United States},
year = {2016},
month = {7}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 2 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

Giant unilamellar vesicles - a perfect tool to visualize phase separation and lipid rafts in model systems.
journal, March 2009

  • Wesołowska, Olga; Michalak, Krystyna; Maniewska, Jadwiga
  • Acta Biochimica Polonica, Vol. 56, Issue 1
  • DOI: 10.18388/abp.2009_2514

Polymersomes: Tough Vesicles Made from Diblock Copolymers
journal, May 1999


From Membranes to Melts, Rouse to Reptation:  Diffusion in Polymersome versus Lipid Bilayers
journal, January 2002

  • Lee, James C. -M.; Santore, Maria; Bates, Frank S.
  • Macromolecules, Vol. 35, Issue 2
  • DOI: 10.1021/ma0112063

Polymersomes
journal, August 2006


Molecular Weight Dependence of Polymersome Membrane Structure, Elasticity, and Stability
journal, October 2002

  • Bermudez, Harry; Brannan, Aaron K.; Hammer, Daniel A.
  • Macromolecules, Vol. 35, Issue 21
  • DOI: 10.1021/ma020669l

Tuning polymersome surfaces: functionalization with dendritic groups
journal, January 2012

  • Amos, Ryan C.; Nazemi, Ali; Bonduelle, Colin V.
  • Soft Matter, Vol. 8, Issue 21
  • DOI: 10.1039/c2sm25172h

Biocompatible Functionalization of Polymersome Surfaces: A New Approach to Surface Immobilization and Cell Targeting Using Polymersomes
journal, March 2011

  • Egli, Stefan; Nussbaumer, Martin G.; Balasubramanian, Vimalkumar
  • Journal of the American Chemical Society, Vol. 133, Issue 12
  • DOI: 10.1021/ja110275f

Polymersomes: smart vesicles of tunable rigidity and permeability
journal, January 2011

  • Rodríguez-García, Ruddi; Mell, Michael; López-Montero, Ivan
  • Soft Matter, Vol. 7, Issue 4
  • DOI: 10.1039/c0sm00823k

A Polymersome Nanoreactor with Controllable Permeability Induced by Stimuli-Responsive Block Copolymers
journal, March 2009

  • Kim, Kyoung Taek; Cornelissen, Jeroen J. L. M.; Nolte, Roeland J. M.
  • Advanced Materials, Vol. 21, Issue 27
  • DOI: 10.1002/adma.200900300

Hydroxide ion flux and pH-gradient driven ester hydrolysis in polymer vesicle reactors
journal, January 2013

  • Paxton, Walter F.; Price, Delisia; Richardson, Nicholas J.
  • Soft Matter, Vol. 9, Issue 47
  • DOI: 10.1039/c3sm51575c

Salt, Shake, Fuse-Giant Hybrid Polymer/Lipid Vesicles through Mechanically Activated Fusion
journal, February 2014

  • Henderson, Ian M.; Paxton, Walter F.
  • Angewandte Chemie International Edition, Vol. 53, Issue 13
  • DOI: 10.1002/anie.201309433

Thermo- and pH-responsive polymers in drug delivery☆
journal, December 2006


Giant Vesicles: Preparations and Applications
journal, March 2010


Dynamic assembly of polymer nanotube networks via kinesin powered microtubule filaments
journal, January 2015

  • Paxton, Walter F.; Bouxsein, Nathan F.; Henderson, Ian M.
  • Nanoscale, Vol. 7, Issue 25
  • DOI: 10.1039/C5NR00826C

The Effect of Chain Length on Protein Solubilization in Polymer-Based Vesicles (Polymersomes)
journal, October 2003


A review of stimuli-responsive nanocarriers for drug and gene delivery
journal, March 2008

  • Ganta, Srinivas; Devalapally, Harikrishna; Shahiwala, Aliasgar
  • Journal of Controlled Release, Vol. 126, Issue 3
  • DOI: 10.1016/j.jconrel.2007.12.017

Biocompatible and biodegradable polymersomes as delivery vehicles in biomedical applications
journal, January 2012

  • Liu, Gong-Yan; Chen, Chao-Jian; Ji, Jian
  • Soft Matter, Vol. 8, Issue 34
  • DOI: 10.1039/c2sm25721a

Oral Drug Delivery Systems Comprising Altered Geometric Configurations for Controlled Drug Delivery
journal, December 2011

  • Moodley, Kovanya; Pillay, Viness; Choonara, Yahya E.
  • International Journal of Molecular Sciences, Vol. 13, Issue 1
  • DOI: 10.3390/ijms13010018

Formation and material properties of giant liquid crystal polymersomes
journal, January 2009

  • Mabrouk, Elyes; Cuvelier, Damien; Pontani, Lea-Laetitia
  • Soft Matter, Vol. 5, Issue 9
  • DOI: 10.1039/b815817g

Templated formation of giant polymer vesicles with controlled size distributions
journal, May 2009

  • Howse, Jonathan R.; Jones, Richard A. L.; Battaglia, Giuseppe
  • Nature Materials, Vol. 8, Issue 6
  • DOI: 10.1038/nmat2446

Enzymatically triggered rupture of polymersomes
journal, January 2016

  • Jang, Woo-Sik; Park, Seung Chul; Reed, Ellen H.
  • Soft Matter, Vol. 12, Issue 4
  • DOI: 10.1039/C5SM01881A

Giant Host Red Blood Cell Membrane Mimicking Polymersomes Bind Parasite Proteins and Malaria Parasites
journal, April 2016

  • Najer, Adrian; Thamboo, Sagana; Palivan, Cornelia G.
  • CHIMIA International Journal for Chemistry, Vol. 70, Issue 4
  • DOI: 10.2533/chimia.2016.288

Films of Agarose Enable Rapid Formation of Giant Liposomes in Solutions of Physiologic Ionic Strength
journal, February 2009

  • Horger, Kim S.; Estes, Daniel J.; Capone, Ricardo
  • Journal of the American Chemical Society, Vol. 131, Issue 5
  • DOI: 10.1021/ja805625u

Encapsulation of Active Cytoskeletal Protein Networks in Cell-Sized Liposomes
journal, August 2011

  • Tsai, Feng-Ching; Stuhrmann, Björn; Koenderink, Gijsje H.
  • Langmuir, Vol. 27, Issue 16
  • DOI: 10.1021/la201604z

Lipid Directed Intrinsic Membrane Protein Segregation
journal, November 2013

  • Hansen, Jesper S.; Thompson, James R.; Hélix-Nielsen, Claus
  • Journal of the American Chemical Society, Vol. 135, Issue 46
  • DOI: 10.1021/ja409708e

Integrin reconstituted in GUVs: A biomimetic system to study initial steps of cell spreading
journal, October 2009

  • Streicher, Pia; Nassoy, Pierre; Bärmann, Michael
  • Biochimica et Biophysica Acta (BBA) - Biomembranes, Vol. 1788, Issue 10
  • DOI: 10.1016/j.bbamem.2009.07.025

Mobility measurement by analysis of fluorescence photobleaching recovery kinetics
journal, September 1976


A Method Improving the Accuracy of Fluorescence Recovery after Photobleaching Analysis
journal, December 2008


Spotted vesicles, striped micelles and Janus assemblies induced by ligand binding
journal, September 2009

  • Christian, David A.; Tian, Aiwei; Ellenbroek, Wouter G.
  • Nature Materials, Vol. 8, Issue 10
  • DOI: 10.1038/nmat2512

Insight into the Mechanism of Antimicrobial Conjugated Polyelectrolytes: Lipid Headgroup Charge and Membrane Fluidity Effects
journal, April 2010

  • Ding, Liping; Chi, Eva Y.; Schanze, Kirk S.
  • Langmuir, Vol. 26, Issue 8
  • DOI: 10.1021/la9038045

Size-Controlled Self-Assembly of Superparamagnetic Polymersomes
journal, December 2013

  • Hickey, Robert J.; Koski, Jason; Meng, Xin
  • ACS Nano, Vol. 8, Issue 1
  • DOI: 10.1021/nn405012h

Gel-Assisted Formation of Giant Unilamellar Vesicles
journal, July 2013

  • Weinberger, Andreas; Tsai, Feng-Ching; Koenderink, Gijsje H.
  • Biophysical Journal, Vol. 105, Issue 1
  • DOI: 10.1016/j.bpj.2013.05.024

Efficient formation of giant liposomes through the gentle hydration of phosphatidylcholine films doped with sugar
journal, January 2009


Polymer Vesicles
journal, August 2002


Asymmetric Lipid Membranes: Towards More Realistic Model Systems
journal, May 2015


Fiji: an open-source platform for biological-image analysis
journal, June 2012

  • Schindelin, Johannes; Arganda-Carreras, Ignacio; Frise, Erwin
  • Nature Methods, Vol. 9, Issue 7
  • DOI: 10.1038/nmeth.2019

    Works referencing / citing this record:

    Self‐Assembly of Giant Unilamellar Vesicles by Film Hydration Methodologies
    journal, March 2019

    • Rideau, Emeline; Wurm, Frederik R.; Landfester, Katharina
    • Advanced Biosystems, Vol. 3, Issue 6
    • DOI: 10.1002/adbi.201800324

    Polymersomes: Breaking the Glass Ceiling?
    journal, October 2018


    Self-assembly/disassembly of giant double-hydrophilic polymersomes at biologically-relevant pH
    journal, January 2018

    • Shin, Sun Hae Ra; McAninch, Patrick T.; Henderson, Ian M.
    • Chemical Communications, Vol. 54, Issue 65
    • DOI: 10.1039/c8cc05155k

    Liposomes and polymersomes: a comparative review towards cell mimicking
    journal, January 2018

    • Rideau, Emeline; Dimova, Rumiana; Schwille, Petra
    • Chemical Society Reviews, Vol. 47, Issue 23
    • DOI: 10.1039/c8cs00162f

    Giant polymersomes from non-assisted film hydration of phosphate-based block copolymers
    journal, January 2018

    • Rideau, Emeline; Wurm, Frederik R.; Landfester, Katharina
    • Polymer Chemistry, Vol. 9, Issue 44
    • DOI: 10.1039/c8py00992a