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Title: Chemically specific coarse-grained models to investigate the structure of biomimetic membranes

Abstract

Biomimetic polymer/protein membranes are promising materials for DNA sequencing, sensors, drug delivery and water purification. These self-assembled structures are made from low molecular weight amphiphilic block copolymers (Nhydrophobic < 40 for a diblock copolymer), including poly(ethylene oxide)–1,2-polybutadiene (EO–1,2-BD) and poly(ethylene oxide)–poly(ethyl ethylene) (EO–EE). To examine these membranes' nanoscale structure, we developed a coarse-grained molecular dynamics (CG MD) model for EO–1,2-BD and assembled a CG MD model for EO–EE using parameters from two published force fields. We observe that the polymers' hydrophobic core blocks are slightly stretched compared to the random coil configuration seen at higher molecular weights. We also observe an increase in the interdigitation of the hydrophobic leaflets with increasing molecular weight (consistent with literature). The hydration level of the EO corona (which may influence protein incorporation) is higher for membranes with a larger area/chain, regardless of whether EE or 1,2-BD forms the hydrophobic block. Our results provide a molecular-scale view of membrane packing and hydrophobicity, two important properties for creating polymer–protein biomimetic membranes.

Authors:
 [1];  [1];  [1];  [2];  [3];  [1]; ORCiD logo [4]
  1. Department of Chemical Engineering, The Pennsylvania State University, University Park, USA
  2. Department of Chemical Engineering, The Pennsylvania State University, University Park, USA, Department of Chemistry
  3. Department of Chemical Engineering, The Pennsylvania State University, University Park, USA, Surface Conditioning Business Unit
  4. Department of Chemical Engineering, The Pennsylvania State University, University Park, USA, Department of Civil and Environmental Engineering
Publication Date:
Research Org.:
Pennsylvania State Univ., University Park, PA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Advanced Scientific Computing Research (ASCR)
OSTI Identifier:
1410586
Alternate Identifier(s):
OSTI ID: 1429295
Grant/Contract Number:  
FG02-02ER25535
Resource Type:
Published Article
Journal Name:
RSC Advances
Additional Journal Information:
Journal Name: RSC Advances Journal Volume: 7 Journal Issue: 86; Journal ID: ISSN 2046-2069
Publisher:
Royal Society of Chemistry (RSC)
Country of Publication:
United Kingdom
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 59 BASIC BIOLOGICAL SCIENCES

Citation Formats

Kowalik, Małgorzata, Schantz, Allen B., Naqi, Abdullah, Shen, Yuexiao, Sines, Ian, Maranas, Janna K., and Kumar, Manish. Chemically specific coarse-grained models to investigate the structure of biomimetic membranes. United Kingdom: N. p., 2017. Web. https://doi.org/10.1039/C7RA10573H.
Kowalik, Małgorzata, Schantz, Allen B., Naqi, Abdullah, Shen, Yuexiao, Sines, Ian, Maranas, Janna K., & Kumar, Manish. Chemically specific coarse-grained models to investigate the structure of biomimetic membranes. United Kingdom. https://doi.org/10.1039/C7RA10573H
Kowalik, Małgorzata, Schantz, Allen B., Naqi, Abdullah, Shen, Yuexiao, Sines, Ian, Maranas, Janna K., and Kumar, Manish. Sun . "Chemically specific coarse-grained models to investigate the structure of biomimetic membranes". United Kingdom. https://doi.org/10.1039/C7RA10573H.
@article{osti_1410586,
title = {Chemically specific coarse-grained models to investigate the structure of biomimetic membranes},
author = {Kowalik, Małgorzata and Schantz, Allen B. and Naqi, Abdullah and Shen, Yuexiao and Sines, Ian and Maranas, Janna K. and Kumar, Manish},
abstractNote = {Biomimetic polymer/protein membranes are promising materials for DNA sequencing, sensors, drug delivery and water purification. These self-assembled structures are made from low molecular weight amphiphilic block copolymers (Nhydrophobic < 40 for a diblock copolymer), including poly(ethylene oxide)–1,2-polybutadiene (EO–1,2-BD) and poly(ethylene oxide)–poly(ethyl ethylene) (EO–EE). To examine these membranes' nanoscale structure, we developed a coarse-grained molecular dynamics (CG MD) model for EO–1,2-BD and assembled a CG MD model for EO–EE using parameters from two published force fields. We observe that the polymers' hydrophobic core blocks are slightly stretched compared to the random coil configuration seen at higher molecular weights. We also observe an increase in the interdigitation of the hydrophobic leaflets with increasing molecular weight (consistent with literature). The hydration level of the EO corona (which may influence protein incorporation) is higher for membranes with a larger area/chain, regardless of whether EE or 1,2-BD forms the hydrophobic block. Our results provide a molecular-scale view of membrane packing and hydrophobicity, two important properties for creating polymer–protein biomimetic membranes.},
doi = {10.1039/C7RA10573H},
journal = {RSC Advances},
number = 86,
volume = 7,
place = {United Kingdom},
year = {2017},
month = {1}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1039/C7RA10573H

Citation Metrics:
Cited by: 1 work
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Figures / Tables:

Fig. 1 Fig. 1: Schematic representations and a simulation snapshot. (a) The level of coarse-graining used to represent water and polymers. From top to bottom, water, poly(ethylene oxide) (EO), 1,2-polybutadiene (1,2-BD) and poly(ethyl ethylene) (EE) are shown in atomistic detail and as coarsegrained beads. Examples of the CG block copolymers are givenmore » in (b), and in (c) a simulation snapshot is presented. Our simulations use a Cartesian coordinate system in which the z-axis is normal to the plane of the membrane.« less

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