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Title: Morphology-induced defects enhance lipid transfer rates

Abstract

Molecular transfer between nanoparticles has been considered to have important implications regarding nanoparticle stability. Recently, the interparticle spontaneous lipid transfer rate constant for discoidal bicelles was found to be very different from spherical, unilamellar vesicles (ULVs). Here, we investigate the mechanism responsible for this discrepancy. Analysis of the data indicates that lipid transfer is entropically favorable, but enthalpically unfavorable with an activation energy that is independent of bicelle size and long- to short-chain lipid molar ratio. Moreover, molecular dynamics simulations reveal a lower lipid dissociation energy cost in the vicinity of interfaces (“defects”) induced by the segregation of the long- and short-chain lipids in bicelles; these defects are not present in ULVs. Taken together, these results suggest that the enhanced lipid transfer observed in bicelles arises from interfacial defects as a result of the hydrophobic mismatch between the long- and short-chain lipid species. In conclusion, the observed lipid transfer rate is found to be independent of nanoparticle stability.

Authors:
 [1];  [1];  [2];  [3];  [3];  [3];  [3];  [1];  [1]
+ Show Author Affiliations
  1. Univ. of Connecticut, Storrs, CT (United States)
  2. Univ. of Graz, Graz (Austria); Brock Univ., St. Catharines, ON (Canada)
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Publication Date:
Research Org.:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Spallation Neutron Source (SNS)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1327689
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Langmuir
Additional Journal Information:
Journal Volume: 32; Journal Issue: 38; Journal ID: ISSN 0743-7463
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Xia, Yan, Charubin, Kamil, Marquardt, Drew, Heberle, Frederick A., Katsaras, John, Tian, Jianhui, Cheng, Xiaolin, Liu, Ying, and Nieh, Mu -Ping. Morphology-induced defects enhance lipid transfer rates. United States: N. p., 2016. Web. doi:10.1021/acs.langmuir.6b02099.
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Xia, Yan, Charubin, Kamil, Marquardt, Drew, Heberle, Frederick A., Katsaras, John, Tian, Jianhui, Cheng, Xiaolin, Liu, Ying, & Nieh, Mu -Ping. Morphology-induced defects enhance lipid transfer rates. United States. https://doi.org/10.1021/acs.langmuir.6b02099
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Xia, Yan, Charubin, Kamil, Marquardt, Drew, Heberle, Frederick A., Katsaras, John, Tian, Jianhui, Cheng, Xiaolin, Liu, Ying, and Nieh, Mu -Ping. Thu . "Morphology-induced defects enhance lipid transfer rates". United States. https://doi.org/10.1021/acs.langmuir.6b02099. https://www.osti.gov/servlets/purl/1327689.
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@article{osti_1327689,
title = {Morphology-induced defects enhance lipid transfer rates},
author = {Xia, Yan and Charubin, Kamil and Marquardt, Drew and Heberle, Frederick A. and Katsaras, John and Tian, Jianhui and Cheng, Xiaolin and Liu, Ying and Nieh, Mu -Ping},
abstractNote = {Molecular transfer between nanoparticles has been considered to have important implications regarding nanoparticle stability. Recently, the interparticle spontaneous lipid transfer rate constant for discoidal bicelles was found to be very different from spherical, unilamellar vesicles (ULVs). Here, we investigate the mechanism responsible for this discrepancy. Analysis of the data indicates that lipid transfer is entropically favorable, but enthalpically unfavorable with an activation energy that is independent of bicelle size and long- to short-chain lipid molar ratio. Moreover, molecular dynamics simulations reveal a lower lipid dissociation energy cost in the vicinity of interfaces (“defects”) induced by the segregation of the long- and short-chain lipids in bicelles; these defects are not present in ULVs. Taken together, these results suggest that the enhanced lipid transfer observed in bicelles arises from interfacial defects as a result of the hydrophobic mismatch between the long- and short-chain lipid species. In conclusion, the observed lipid transfer rate is found to be independent of nanoparticle stability.},
doi = {10.1021/acs.langmuir.6b02099},
journal = {Langmuir},
number = 38,
volume = 32,
place = {United States},
year = {Thu Aug 25 00:00:00 EDT 2016},
month = {Thu Aug 25 00:00:00 EDT 2016}
}
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https://doi.org/10.1021/acs.langmuir.6b02099
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