Harnessing peptide–cellulose interactions to tailor the performance of self-assembled, injectable hydrogels

Thomas, Jessica A.; Balzer, Alex H.; Kalidindi, Subhash; Korley, LaShanda T. J.

doi:10.1039/D5ME00009B

Harnessing peptide–cellulose interactions to tailor the performance of self-assembled, injectable hydrogels

Journal Article · Mon Jun 02 00:00:00 EDT 2025 · Molecular Systems Design & Engineering

DOI:https://doi.org/10.1039/D5ME00009B· OSTI ID:2569112

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Univ. of Delaware, Newark, DE (United States)

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.

View Accepted Manuscript (DOE)

Research Organization:: Univ. of Delaware, Newark, DE (United States)

Sponsoring Organization:: National Institute of General Medical Sciences (NIGMS); National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0021166

OSTI ID:: 2569112

Journal Information:: Molecular Systems Design & Engineering, Journal Name: Molecular Systems Design & Engineering Journal Issue: 8 Vol. 10; ISSN 2058-9689

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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