Control of hierarchical polymer mechanics with bioinspired metal-coordination dynamics

Grindy, Scott C.; Learsch, Robert; Mozhdehi, Davoud; Cheng, Jing; Barrett, Devin G.; Guan, Zhibin; Messersmith, Phillip B.; Holten-Andersen, Niels

doi:10.1038/nmat4401

Title: Control of hierarchical polymer mechanics with bioinspired metal-coordination dynamics

Journal Article · Mon Aug 31 00:00:00 EDT 2015 · Nature Materials

DOI:https://doi.org/10.1038/nmat4401· OSTI ID:1467436

Grindy, Scott C. ^[1]; Learsch, Robert ^[1]; Mozhdehi, Davoud ^[2]; Cheng, Jing ^[3]; Barrett, Devin G. ^[3]; Guan, Zhibin ^[2]; Messersmith, Phillip B. ^[3]; Holten-Andersen, Niels ^[1]

Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Dept. of Materials Science and Engineering
Univ. of California, Irvine, CA (United States). Dept. of Chemistry
Northwestern Univ., Evanston, IL (United States). Dept. of Biomedical Engineering

In conventional polymer materials, mechanical performance is traditionally engineered via material structure, using motifs such as polymer molecular weight, polymer branching, or copolymer-block design1. Here, by means of a model system of 4-arm poly(ethylene glycol) hydrogels crosslinked with multiple, kinetically distinct dynamic metal-ligand coordinate complexes, we show that polymer materials with decoupled spatial structure and mechanical performance can be designed. By tuning the relative concentration of two types of metal-ligand crosslinks, we demonstrate control over the material’s mechanical hierarchy of energy-dissipating modes under dynamic mechanical loading, and therefore the ability to engineer a priori the viscoelastic properties of these materials by controlling the types of crosslinks rather than by modifying the polymer itself. This strategy to decouple material mechanics from structure may inform the design of soft materials for use in complex mechanical environments.

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Research Organization:: Univ. of California, Irvine, CA (United States)

Sponsoring Organization:: USDOE

Grant/Contract Number:: FG02-04ER46162

OSTI ID:: 1467436

Journal Information:: Nature Materials, Vol. 14, Issue 12; ISSN 1476-1122

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 335 works

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Hydrogen bonding and thermoplastic elastomers - a nice couple with temperature-adjustable mechanical properties Wittenberg, Elisabeth; Meyer, Andreas; Eggers, Steffen TUHH Universitätsbibliothek https://doi.org/10.15480/882.1625	text	January 2018
Controlling Spatiotemporal Mechanics of Supramolecular Hydrogel Networks with Highly Branched Cucurbit[8]uril Polyrotaxanes Tan, Csy; Liu, Ji; Groombridge, Alexander Apollo - University of Cambridge Repository https://doi.org/10.17863/cam.25417	text	January 2018
In Vivo Biocompatibility and Immunogenicity of Metal-Phenolic Gelation Björnmalm, Mattias; Wong, Lok Man; Wojciechowski, Jonathan ChemRxiv. Materials Science https://doi.org/10.26434/chemrxiv.8786048.v1	posted_content	July 2019
Shear Melting and Recovery of Crosslinkable Cellulose Nanocrystal-Polymer Gels Rao, Abhinav; Divoux, Thibaut; McKinley, Gareth H. arXiv https://doi.org/10.48550/arxiv.1901.04373	preprint	January 2019
Reversibly tuning hydrogel stiffness through photocontrolled dynamic covalent crosslinks Accardo, Joseph V.; Kalow, Julia A. Chemical Science, Vol. 9, Issue 27 https://doi.org/10.1039/c8sc02093k	journal	January 2018
Influence of Network Topology on the Viscoelastic Properties of Dynamically Crosslinked Hydrogels Grad, Emilia M.; Tunn, Isabell; Voerman, Dion Polymer Science. ChemRxiv https://doi.org/10.26434/chemrxiv.11763792.v1	journal	January 2020
Bioinspired Histidine–Zn2+ Coordination for Tuning the Mechanical Properties of Self-Healing Coiled Coil Cross-Linked Hydrogels Tunn, Isabell; Harrington, Matthew J.; Blank, Kerstin G. Biomimetics, Vol. 4, Issue 1 https://doi.org/10.3390/biomimetics4010025	journal	March 2019
Computing the linear viscoelastic properties of soft gels using an Optimally Windowed Chirp protocol Bouzid, Mehdi; Keshavarz, Bavand; Geri, Michela arXiv https://doi.org/10.48550/arxiv.1805.07987	text	January 2018

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