Harnessing peptide–cellulose interactions to tailor the performance of self-assembled, injectable hydrogels
Year: 2025
Type: article
Abstract: Taking inspiration from natural systems, such as spider silk and mollusk nacre, that employ hierarchical assembly to attain robust material performance, we leveraged matrix-filler interactions within reinforced polymer-peptide hybrids to create self-assembled hydrogels with enhanced properties. Specifically, cellulose nanocrystals (CNCs) were incorporated into peptide-polyurea (PPU) hybrid matrices to tailor key hydrogel features through matrix-filler interactions. Herein, we examined the impact of peptide repeat length and CNC loading on hydrogelation, morphology, mechanics, and thermal behavior of PPU/CNC composite hydrogels. The addition of CNCs into PPU hydrogels resulted in increased gel stiffness; however, the extent of reinforcement of the nanocomposite gels upon nanofiller inclusion also was driven by PPU architecture. Temperature-promoted stiffening transitions observed in nanocomposite PPU hydrogels were dictated by peptide segment length. Analysis of the peptide secondary structure confirmed shifts in the conformation of peptidic domains (α-helices or β-sheets) upon CNC loading. Finally, PPU/CNC hydrogels were probed for their injectability characteristics, demonstrating that nanofiller-matrix interactions were shown to aid rapid network reformation (∼10 s) upon cessation of high shear forces. Overall, this research showcases the potential of modulating matrix-filler interactions within PPU/CNC hydrogels through strategic system design, enabling the tuning of functional hydrogel characteristics for diverse applications.
DOI: 10.1039/d5me00009b
Institution: University of Delaware
Language: English
Subfield: Biomaterials
Field: Materials Science
Domain: Physical Sciences
Open Access status: hybrid
Funders: National Science Foundation, U.S. Department of Energy, University of Delaware, Unidel Foundation, National Institutes of Health, Office of Science, National Institute of General Medical Sciences, Division of Materials Research, Office of International Science and Engineering, Basic Energy Sciences
Awards: G1177608224, G1451002057, G1705962760, G1880822571, G3115553707, CENTER FOR PLASTICS INNOVATION (CPI), G3983532892, G4129942005, G4444685404, PIRE: Bio-Inspired Materials and Systems, CENTER FOR PLASTICS INNOVATION (CPI), Delaware INBRE, G6192324953, G6345397415, G6718912342, G6772302223, University of Delaware MRSEC - Center for Hybrid, Active, and Responsive Materials (CHARM), G9000014540, G9000019295, G9000093202, G9000125231
OpenAlex ID: W4410965640