University of Massachusetts Medical School Faculty Publications

Title

Independent and Synergistic Modulations of Viscoelasticity and Stiffness of Dynamically Cross-Linked Cell-Encapsulating ClickGels by Covalently Tethered Polymer Brushes

UMMS Affiliation

Department of Orthopedics and Physical Rehabilitation

Publication Date

2021-08-09

Document Type

Article

Disciplines

Biomaterials | Materials Chemistry | Molecular, Cellular, and Tissue Engineering

Abstract

We report independent and synergistic modulations of the stiffness and viscoelasticity of ClickGels, formed by a combination of the bio-orthogonal covalent and dynamic noncovalent cross-linking, by covalently incorporating nonionic, zwitterionic, or anionic polymer brushes. Tethering nonionic and zwitterionic brushes at the cost of noncovalent cross-linking increased stiffness and slowed stress relaxation, respectively, without altering the other properties. Meanwhile, tethering anionic brushes significantly increased ClickGel stiffness, while also slowing its stress relaxation. ClickGels with faster stress relaxation, not reduced stiffness, promoted short-term (24 h) viability and YAP/TAZ nuclear localization of encapsulated bone marrow-derived stromal cells (BMSCs). In contrast, ClickGel stiffness, not viscoelasticity, inversely correlated to the short-term dehydrogenase activity of encapsulated BMSCs. This work highlights the role of the ionic state of polymer brushes in modulating the hydrogel elastic modulus and viscoelasticity and establishes the brush-modified ClickGel as a facile and reproducible tool for manipulating mechanical cues of the synthetic cellular niche.

Keywords

Stress, Stiffness, Encapsulation, Nucleic acid structure, Hydrogels

DOI of Published Version

10.1021/acs.biomac.1c00477

Source

Tan Y, Song J. Independent and Synergistic Modulations of Viscoelasticity and Stiffness of Dynamically Cross-Linked Cell-Encapsulating ClickGels by Covalently Tethered Polymer Brushes. Biomacromolecules. 2021 Aug 9;22(8):3408-3415. doi: 10.1021/acs.biomac.1c00477. Epub 2021 Jul 22. PMID: 34292720. Link to article on publisher's site

Related Resources

Link to Article in PubMed

Journal/Book/Conference Title

Biomacromolecules

PubMed ID

34292720

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