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Title: Incorporation of Melittin Enhances Interfacial Fluidity of Bicontinuous Microemulsions

Abstract

The effect of an antimicrobial peptide, melittin, on the long-range collective and local undulation motions of bicontinuous microemulsions (BμEs) was evaluated using dynamic light scattering (DLS) and neutron spin echo (NSE) spectroscopy. Small-angle neutron scattering (SANS) was also used to study the effect of melittin on the structure and the correlation length of BμEs. BμEs were isolated from Winsor-III systems formed by mixing aqueous melittin solutions containing sodium dodecyl sulfate with dodecane/1-pentanol mixtures at optimal salinity. An increase of melittin concentration linearly increased the diffusivity of the microemulsions (DDLS) and decreased the bending rigidity (κNSE) up to an aqueous melittin concentration of 2 g/L, thus indicating an increase of interfacial fluidity. Further increase of melittin concentration above 2 g/L did not change DDLS and slightly increased κNSE. The changes reflect differences of interaction between melittin and BμE surfactant monolayers at different melittin concentrations. At low concentrations, melittin is highly associated with the surfactant monolayers, likely ion-paired to the sulfate surfactant head groups and perhaps partially penetrating into the surfactant tail region. Above 2 g/L, an apparent saturation concentration, added melittin is less strongly associated with the monolayers. In contrast, the bare bending constant derived from SANS data (κbare) underwent onlymore » a minor decrease. Noting that κbare reflects contributions from both the elasticity and saddle-splay moduli, this suggests that κbare is not an effective indicator of dynamics for the BμEs investigated. Our study demonstrates that amphiphilic solubilizates can have a complex impact on dynamics of surfactant monolayers in microemulsions, with implications for transmembrane diffusion and the kinetics of release from the microemulsion phase, which are important characteristics for the use of BμEs as delivery vehicles and host systems for (bio)chemical reactions.« less

Authors:
ORCiD logo [1];  [2]; ORCiD logo [3]; ORCiD logo [4]; ORCiD logo [4]; ORCiD logo [4];  [5]; ORCiD logo [4]
  1. Bhabha Atomic Research Centre, Mumbai (India)
  2. Univ. of Tennessee, Knoxville, TN (United States)
  3. Louisiana State Univ., Baton Rouge, LA (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Spallation Neutron Source (SNS) outstation Juelich Centre for Neutron Science (JCNS), Forschungszentrum Juelich GmbH
  4. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Neutron Sciences Directorate
  5. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Spallation Neutron Source (SNS) outstation Juelich Centre for Neutron Science (JCNS), Forschungszentrum Juelich GmbH
Publication Date:
Research Org.:
Louisiana State Univ., Baton Rouge, LA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1615940
Grant/Contract Number:  
SC0012432
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry. C
Additional Journal Information:
Journal Volume: 123; Journal Issue: 17; Journal ID: ISSN 1932-7447
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; Lipids; Sodium dodecyl sulfate; Dynamic light scattering; Monolayers; Surfactants; antimicrobial peptides; bicontinuous microemulsions; dynamics; collective motions; elasticity; bending modulus; neutron spin echo; small-angle neutron scattering; dynamic light scattering; sodium dodecyl sulfate; winsor-III systems; melittin

Citation Formats

Sharma, V. K., Hayes, D. G., Gupta, S., Urban, V. S., O’Neill, H. M., Pingali, S. V., Ohl, M., and Mamontov, E. Incorporation of Melittin Enhances Interfacial Fluidity of Bicontinuous Microemulsions. United States: N. p., 2019. Web. doi:10.1021/acs.jpcc.9b00103.
Sharma, V. K., Hayes, D. G., Gupta, S., Urban, V. S., O’Neill, H. M., Pingali, S. V., Ohl, M., & Mamontov, E. Incorporation of Melittin Enhances Interfacial Fluidity of Bicontinuous Microemulsions. United States. https://doi.org/10.1021/acs.jpcc.9b00103
Sharma, V. K., Hayes, D. G., Gupta, S., Urban, V. S., O’Neill, H. M., Pingali, S. V., Ohl, M., and Mamontov, E. Fri . "Incorporation of Melittin Enhances Interfacial Fluidity of Bicontinuous Microemulsions". United States. https://doi.org/10.1021/acs.jpcc.9b00103. https://www.osti.gov/servlets/purl/1615940.
@article{osti_1615940,
title = {Incorporation of Melittin Enhances Interfacial Fluidity of Bicontinuous Microemulsions},
author = {Sharma, V. K. and Hayes, D. G. and Gupta, S. and Urban, V. S. and O’Neill, H. M. and Pingali, S. V. and Ohl, M. and Mamontov, E.},
abstractNote = {The effect of an antimicrobial peptide, melittin, on the long-range collective and local undulation motions of bicontinuous microemulsions (BμEs) was evaluated using dynamic light scattering (DLS) and neutron spin echo (NSE) spectroscopy. Small-angle neutron scattering (SANS) was also used to study the effect of melittin on the structure and the correlation length of BμEs. BμEs were isolated from Winsor-III systems formed by mixing aqueous melittin solutions containing sodium dodecyl sulfate with dodecane/1-pentanol mixtures at optimal salinity. An increase of melittin concentration linearly increased the diffusivity of the microemulsions (DDLS) and decreased the bending rigidity (κNSE) up to an aqueous melittin concentration of 2 g/L, thus indicating an increase of interfacial fluidity. Further increase of melittin concentration above 2 g/L did not change DDLS and slightly increased κNSE. The changes reflect differences of interaction between melittin and BμE surfactant monolayers at different melittin concentrations. At low concentrations, melittin is highly associated with the surfactant monolayers, likely ion-paired to the sulfate surfactant head groups and perhaps partially penetrating into the surfactant tail region. Above 2 g/L, an apparent saturation concentration, added melittin is less strongly associated with the monolayers. In contrast, the bare bending constant derived from SANS data (κbare) underwent only a minor decrease. Noting that κbare reflects contributions from both the elasticity and saddle-splay moduli, this suggests that κbare is not an effective indicator of dynamics for the BμEs investigated. Our study demonstrates that amphiphilic solubilizates can have a complex impact on dynamics of surfactant monolayers in microemulsions, with implications for transmembrane diffusion and the kinetics of release from the microemulsion phase, which are important characteristics for the use of BμEs as delivery vehicles and host systems for (bio)chemical reactions.},
doi = {10.1021/acs.jpcc.9b00103},
journal = {Journal of Physical Chemistry. C},
number = 17,
volume = 123,
place = {United States},
year = {Fri Mar 22 00:00:00 EDT 2019},
month = {Fri Mar 22 00:00:00 EDT 2019}
}

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