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Title: Hybrid gels via bulk interfacial complexation of supramolecular polymers and polyelectrolytes

Abstract

Hierarchical self-assembly leading to organized supramolecular structures across multiple length scales has been of great recent interest. Earlier work from our laboratory reported the complexation of peptide amphiphile (PA) supramolecular polymers with oppositely charged polyelectrolytes into a single solid membrane at a macroscopic interface. We report here the formation of bulk gels with many internal interfaces between the covalent and supramolecular polymer components formed by the rapid chaotic mixing of solutions, one containing negatively charged PA nanofibers and the other the positively charged biopolymer chitosan. We found that formation of a contact layer at the interface of the solutions locks the formation of hydrogels with lamellar microstructure. The nanofiber morphology of the supramolecular polymer is essential to this process since gels do not form when solutions of supramolecular assemblies form spherical micelles. Here, we found that rheological properties of the gels can be tuned by changing the relative amounts of each component. Furthermore, both positively and negatively charged proteins are easily encapsulated within the contact layer of the gel, which provides an interesting biomedical function for these systems.

Authors:
ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [2]
  1. Northwestern Univ., Evanston, IL (United States)
  2. Northwestern Univ., Evanston, IL (United States); Northwestern Univ., Chicago, IL (United States)
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Center for Bio-Inspired Energy Science (CBES)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1823105
Alternate Identifier(s):
OSTI ID: 1773523; OSTI ID: 1846602
Grant/Contract Number:  
SC0000989; AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Soft Matter
Additional Journal Information:
Journal Volume: 17; Journal Issue: 19; Journal ID: ISSN 1744-683X
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 99 GENERAL AND MISCELLANEOUS

Citation Formats

Cotey, Thomas J., Sai, Hiroaki, Perez, Cynthia, Palmer, Liam C., and Stupp, Samuel I. Hybrid gels via bulk interfacial complexation of supramolecular polymers and polyelectrolytes. United States: N. p., 2021. Web. doi:10.1039/d1sm00168j.
Cotey, Thomas J., Sai, Hiroaki, Perez, Cynthia, Palmer, Liam C., & Stupp, Samuel I. Hybrid gels via bulk interfacial complexation of supramolecular polymers and polyelectrolytes. United States. https://doi.org/10.1039/d1sm00168j
Cotey, Thomas J., Sai, Hiroaki, Perez, Cynthia, Palmer, Liam C., and Stupp, Samuel I. Wed . "Hybrid gels via bulk interfacial complexation of supramolecular polymers and polyelectrolytes". United States. https://doi.org/10.1039/d1sm00168j. https://www.osti.gov/servlets/purl/1823105.
@article{osti_1823105,
title = {Hybrid gels via bulk interfacial complexation of supramolecular polymers and polyelectrolytes},
author = {Cotey, Thomas J. and Sai, Hiroaki and Perez, Cynthia and Palmer, Liam C. and Stupp, Samuel I.},
abstractNote = {Hierarchical self-assembly leading to organized supramolecular structures across multiple length scales has been of great recent interest. Earlier work from our laboratory reported the complexation of peptide amphiphile (PA) supramolecular polymers with oppositely charged polyelectrolytes into a single solid membrane at a macroscopic interface. We report here the formation of bulk gels with many internal interfaces between the covalent and supramolecular polymer components formed by the rapid chaotic mixing of solutions, one containing negatively charged PA nanofibers and the other the positively charged biopolymer chitosan. We found that formation of a contact layer at the interface of the solutions locks the formation of hydrogels with lamellar microstructure. The nanofiber morphology of the supramolecular polymer is essential to this process since gels do not form when solutions of supramolecular assemblies form spherical micelles. Here, we found that rheological properties of the gels can be tuned by changing the relative amounts of each component. Furthermore, both positively and negatively charged proteins are easily encapsulated within the contact layer of the gel, which provides an interesting biomedical function for these systems.},
doi = {10.1039/d1sm00168j},
journal = {Soft Matter},
number = 19,
volume = 17,
place = {United States},
year = {Wed Mar 31 00:00:00 EDT 2021},
month = {Wed Mar 31 00:00:00 EDT 2021}
}

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