Ultrasound-Mediated Self-Healing Hydrogels Based on Tunable Metal-Organic Bonding

Wei Chen Huang, Jingsi Zhao, Kelsey Rhee, Christopher J. Bettinger

Research output: Contribution to journalArticle

17 Citations (Scopus)

Abstract

Stimulus-responsive hydrogels make up an important class of programmable materials for a wide range of biomedical applications. Ultrasound (US) is a stimulus that offers utility because of its ability to permeate tissue and rapidly induce chemical alterations in aqueous media. Here we report on the synthesis and US-mediated disintegration of stimulus-responsive telechelic Dopa-modified polyethylene glycol-based hydrogels. Fe3+-[PEG-Dopa]4 hydrogels are formed through Fe3+-induced cross-linking of four-arm polyethylene glycol-dopamine precursors to produce networks. The relative amounts of H-bonds, coordination bonds, and covalent bonds can be controlled by the [Fe3+]:[Dopa] molar ratio in precursor solutions. Networks formed from precursors with high [Fe3+]:[Dopa] ratios create mechanically robust networks (G′ = 6880 ± 240 Pa) that are largely impervious to US-mediated disintegration at intensities of ≤43 W/cm2. Conversely, lightly cross-linked networks formed through [Fe3+]:[Dopa] molar ratios of <0.73 are susceptible to rapid disintegration upon exposure to US. Pulsatile US exposure allows temporal control over hydrogel disintegration and programmable self-healing. Sustained US energy can also stabilize hydrogels through the formation of additional cross-links via free radical-mediated coupling of pendant catechols. Taken together, the diverse ranges of mechanical behavior, self-healing capability, and differential susceptibility to ultrasonic disintegration suggest that Fe3+-[PEG-Dopa]4 hydrogels yield a class of application-specific stimulus-responsive polymers as smart materials for applications ranging from transient medical implants to matrices for smart drug delivery.

Original languageEnglish
Pages (from-to)1162-1171
Number of pages10
JournalBiomacromolecules
Volume18
Issue number4
DOIs
Publication statusPublished - Apr 10 2017

Fingerprint

Hydrogels
Dihydroxyphenylalanine
Disintegration
Ultrasonics
Metals
Polyethylene glycols
Catechols
Covalent bonds
Intelligent materials
Hydrogel
Free radicals
Drug delivery
Free Radicals
Dopamine
Polymers
Tissue

ASJC Scopus subject areas

  • Bioengineering
  • Biomaterials
  • Polymers and Plastics
  • Materials Chemistry

Cite this

Ultrasound-Mediated Self-Healing Hydrogels Based on Tunable Metal-Organic Bonding. / Huang, Wei Chen; Zhao, Jingsi; Rhee, Kelsey; Bettinger, Christopher J.

In: Biomacromolecules, Vol. 18, No. 4, 10.04.2017, p. 1162-1171.

Research output: Contribution to journalArticle

Huang, Wei Chen ; Zhao, Jingsi ; Rhee, Kelsey ; Bettinger, Christopher J. / Ultrasound-Mediated Self-Healing Hydrogels Based on Tunable Metal-Organic Bonding. In: Biomacromolecules. 2017 ; Vol. 18, No. 4. pp. 1162-1171.
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