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Title: Surface force measurements and simulations of mussel-derived peptide adhesives on wet organic surfaces

Translating sticky biological molecules—such as mussel foot proteins (MFPs)—into synthetic, cost-effective underwater adhesives with adjustable nano- and macroscale characteristics requires an intimate understanding of the glue’s molecular interactions. In this paper, to help facilitate the next generation of aqueous adhesives, we performed a combination of surface forces apparatus (SFA) measurements and replica-exchange molecular dynamics (REMD) simulations on a synthetic, easy to prepare, Dopa-containing peptide (MFP-3s peptide), which adheres to organic surfaces just as effectively as its wild-type protein analog. Experiments and simulations both show significant differences in peptide adsorption on CH 3-terminated (hydrophobic) and OH-terminated (hydrophilic) self-assembled monolayers (SAMs), where adsorption is strongest on hydrophobic SAMs because of orientationally specific interactions with Dopa. Finally, additional umbrella-sampling simulations yield free-energy profiles that quantitatively agree with SFA measurements and are used to extract the adhesive properties of individual amino acids within the context of MFP-3s peptide adhesion, revealing a delicate balance between van der Waals, hydrophobic, and electrostatic forces.
Authors:
 [1] ;  [2] ;  [3] ;  [2] ;  [4] ;  [5] ;  [5] ;  [6] ;  [7] ;  [1]
  1. Univ. of California, Santa Barbara, CA (United States). Dept. of Physics. Dept. of Chemistry and Biochemistry
  2. Univ. of California, Santa Barbara, CA (United States). Dept. of Chemical Engineering
  3. Univ. of California, Santa Barbara, CA (United States). Materials Research Lab.
  4. Rowan Univ., Glassboro, NJ (United States). Dept. of Chemistry and Biochemistry
  5. Lehigh Univ., Bethlehem, PA (United States). Dept. of Chemical and Biomolecular Engineering
  6. Univ. of California, Santa Barbara, CA (United States). Materials Research Lab. Dept. of Molecular, Cell and Developmental Biology
  7. Univ. of California, Santa Barbara, CA (United States). Dept. of Chemical Engineering. Materials Research Lab.
Publication Date:
Grant/Contract Number:
SC0013979; MCB-1158577; DMR 1121053; CNS-0960316; ACI-1053575; R01 DE018468
Type:
Accepted Manuscript
Journal Name:
Proceedings of the National Academy of Sciences of the United States of America
Additional Journal Information:
Journal Volume: 113; Journal Issue: 16; Journal ID: ISSN 0027-8424
Publisher:
National Academy of Sciences, Washington, DC (United States)
Research Org:
Lehigh Univ., Bethlehem, PA (United States); Univ. of California, Santa Barbara, CA (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); National Science Foundation (NSF); National Inst. of Health (NIH) (United States)
Country of Publication:
United States
Language:
English
Subject:
59 BASIC BIOLOGICAL SCIENCES; mussel foot proteins; self-assembled monolayers; protein folding; molecular dynamics simulations; surface forces apparatus
OSTI Identifier:
1469313

Levine, Zachary A., Rapp, Michael V., Wei, Wei, Mullen, Ryan Gotchy, Wu, Chun, Zerze, Gül H., Mittal, Jeetain, Waite, J. Herbert, Israelachvili, Jacob N., and Shea, Joan-Emma. Surface force measurements and simulations of mussel-derived peptide adhesives on wet organic surfaces. United States: N. p., Web. doi:10.1073/pnas.1603065113.
Levine, Zachary A., Rapp, Michael V., Wei, Wei, Mullen, Ryan Gotchy, Wu, Chun, Zerze, Gül H., Mittal, Jeetain, Waite, J. Herbert, Israelachvili, Jacob N., & Shea, Joan-Emma. Surface force measurements and simulations of mussel-derived peptide adhesives on wet organic surfaces. United States. doi:10.1073/pnas.1603065113.
Levine, Zachary A., Rapp, Michael V., Wei, Wei, Mullen, Ryan Gotchy, Wu, Chun, Zerze, Gül H., Mittal, Jeetain, Waite, J. Herbert, Israelachvili, Jacob N., and Shea, Joan-Emma. 2016. "Surface force measurements and simulations of mussel-derived peptide adhesives on wet organic surfaces". United States. doi:10.1073/pnas.1603065113. https://www.osti.gov/servlets/purl/1469313.
@article{osti_1469313,
title = {Surface force measurements and simulations of mussel-derived peptide adhesives on wet organic surfaces},
author = {Levine, Zachary A. and Rapp, Michael V. and Wei, Wei and Mullen, Ryan Gotchy and Wu, Chun and Zerze, Gül H. and Mittal, Jeetain and Waite, J. Herbert and Israelachvili, Jacob N. and Shea, Joan-Emma},
abstractNote = {Translating sticky biological molecules—such as mussel foot proteins (MFPs)—into synthetic, cost-effective underwater adhesives with adjustable nano- and macroscale characteristics requires an intimate understanding of the glue’s molecular interactions. In this paper, to help facilitate the next generation of aqueous adhesives, we performed a combination of surface forces apparatus (SFA) measurements and replica-exchange molecular dynamics (REMD) simulations on a synthetic, easy to prepare, Dopa-containing peptide (MFP-3s peptide), which adheres to organic surfaces just as effectively as its wild-type protein analog. Experiments and simulations both show significant differences in peptide adsorption on CH3-terminated (hydrophobic) and OH-terminated (hydrophilic) self-assembled monolayers (SAMs), where adsorption is strongest on hydrophobic SAMs because of orientationally specific interactions with Dopa. Finally, additional umbrella-sampling simulations yield free-energy profiles that quantitatively agree with SFA measurements and are used to extract the adhesive properties of individual amino acids within the context of MFP-3s peptide adhesion, revealing a delicate balance between van der Waals, hydrophobic, and electrostatic forces.},
doi = {10.1073/pnas.1603065113},
journal = {Proceedings of the National Academy of Sciences of the United States of America},
number = 16,
volume = 113,
place = {United States},
year = {2016},
month = {3}
}