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Hybrid gels via bulk interfacial complexation of supramolecular polymers and polyelectrolytes

Journal Article · · Soft Matter
DOI:https://doi.org/10.1039/d1sm00168j· OSTI ID:1823105
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.
Research Organization:
Energy Frontier Research Centers (EFRC) (United States). Center for Bio-Inspired Energy Science (CBES)
Sponsoring Organization:
USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
AC02-06CH11357; SC0000989
OSTI ID:
1823105
Alternate ID(s):
OSTI ID: 1814977
OSTI ID: 1818331
OSTI ID: 1846602
OSTI ID: 1773523
Journal Information:
Soft Matter, Journal Name: Soft Matter Journal Issue: 19 Vol. 17; ISSN 1744-683X
Publisher:
Royal Society of ChemistryCopyright Statement
Country of Publication:
United States
Language:
English

References (52)

Intermolecular Forces in the Self-Assembly of Peptide Amphiphile Nanofibers journal March 2006
Electric Field Controlled Self-Assembly of Hierarchically Ordered Membranes journal October 2011
Humidity-Triggered Self-Healing of Microporous Polyelectrolyte Multilayer Coatings for Hydrophobic Drug Delivery journal November 2015
Nanoengineering Hybrid Supramolecular Multilayered Biomaterials Using Polysaccharides and Self-Assembling Peptide Amphiphiles journal February 2017
Hydrodynamically Guided Hierarchical Self-Assembly of Peptide-Protein Bioinks journal February 2018
Ultrafast Fabrication of Gradient Nanoporous All‐Polysaccharide Films as Strong, Superfast, and Multiresponsive Actuators journal March 2019
Self-assembly of Cytotoxic Peptide Amphiphiles into Supramolecular Membranes for Cancer Therapy journal July 2012
Three-Dimensional Human Tissue Chips Fabricated by Rapid and Automatic Inkjet Cell Printing journal November 2012
Gel Scaffolds of BMP-2-Binding Peptide Amphiphile Nanofibers for Spinal Arthrodesis journal April 2014
Tunable, High Modulus Hydrogels Driven by Ionic Coacervation journal April 2011
A Multimaterial Bioink Method for 3D Printing Tunable, Cell-Compatible Hydrogels journal January 2015
Electrostatic Control of Bioactivity journal May 2011
Phase separation in polyelectrolyte solutions. Theory of complex coacervation journal May 1957
The Kenics static mixer: a three-dimensional chaotic flow journal June 1997
Hydrogel blends of chitin/chitosan, fucoidan and alginate as healing-impaired wound dressings journal January 2010
A bioactive self-assembled membrane to promote angiogenesis journal February 2011
Tunable dual growth factor delivery from polyelectrolyte multilayer films journal September 2011
Biomaterials based on chitin and chitosan in wound dressing applications journal May 2011
Complex coacervate core micelles journal March 2009
Films based on chitosan polyelectrolyte complexes for skin drug delivery: Development and characterization journal July 2008
DND-CAT's new triple area detector system for simultaneous data collection at multiple length scales
  • Weigand, Steven J.; Keane, Denis T.
  • Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 649, Issue 1 https://doi.org/10.1016/j.nima.2010.12.045
journal September 2011
Supramolecular Assembly of Peptide Amphiphiles journal September 2017
Supramolecular Nanofibrous Peptide/Polymer Hydrogels for the Multiplexing of Bioactive Signals journal July 2019
Gelator Length Precisely Tunes Supramolecular Hydrogel Stiffness and Neuronal Phenotype in 3D Culture journal January 2020
Hydrogels for Protein Delivery journal February 2012
Glucose Sensing in Supramolecular Chemistry journal May 2015
Synthetic lipidation of peptides and amino acids: monolayer structure and properties. journal September 1995
pH and Amphiphilic Structure Direct Supramolecular Behavior in Biofunctional Assemblies journal October 2014
Phase Diagram for Assembly of Biologically-Active Peptide Amphiphiles journal January 2008
Tunable Mechanics of Peptide Nanofiber Gels journal March 2010
The Polyelectrolyte Complex/Coacervate Continuum journal April 2014
Designing hydrogels for controlled drug delivery journal October 2016
Co-assembly, spatiotemporal control and morphogenesis of a hybrid protein–peptide system journal September 2015
Gel phase formation in dilute triblock copolyelectrolyte complexes journal February 2017
Cell death versus cell survival instructed by supramolecular cohesion of nanostructures journal February 2014
Internal dynamics of a supramolecular nanofibre journal May 2014
Supramolecular biomaterials journal December 2015
Energy landscapes and functions of supramolecular systems journal January 2016
Sulfated glycopeptide nanostructures for multipotent protein activation journal June 2017
Polymer physics of intracellular phase transitions journal November 2015
Biomolecular condensates: organizers of cellular biochemistry journal February 2017
Self-assembling peptide scaffolds for regenerative medicine journal January 2012
Inhibition of atherosclerosis-promoting microRNAs via targeted polyelectrolyte complex micelles journal January 2014
Molecular design for growth of supramolecular membranes with hierarchical structure journal January 2016
Drug delivery by supramolecular design journal January 2017
Physical properties of hierarchically ordered self-assembled planar and spherical membranes journal January 2010
Peptide-amphiphile nanofibers: A versatile scaffold for the preparation of self-assembling materials journal April 2002
Foundations of chaotic mixing
  • Wiggins, Stephen; Ottino, Julio M.
  • Philosophical Transactions of the Royal Society of London. Series A: Mathematical, Physical and Engineering Sciences, Vol. 362, Issue 1818 https://doi.org/10.1098/rsta.2003.1356
journal May 2004
GSAS-II : the genesis of a modern open-source all purpose crystallography software package journal March 2013
Self-Assembly and Mineralization of Peptide-Amphiphile Nanofibers journal November 2001
Self-Assembly of Large and Small Molecules into Hierarchically Ordered Sacs and Membranes journal March 2008
Fuzzy Nanoassemblies: Toward Layered Polymeric Multicomposites journal August 1997

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