Chemical signal regulated injectable coacervate hydrogels

In the quest for stimuli-responsive materials with specific, controllable functions, coacervate hydrogels have become a promising candidate, featuring sensitive responsiveness to environmental signals enabling control over sol-gel transitions. However, conventional coacervation-based materials are r...

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Bibliographic Details
Published in:Chemical science (Cambridge) 2023-02, Vol.14 (6), p.1512-1523
Main Authors: Wu, Bohang, Lewis, Reece W, Li, Guotai, Gao, Yifan, Fan, Bowen, Klemm, Benjamin, Huang, Jianan, Wang, Junyou, Cohen Stuart, Martien A, Eelkema, Rienk
Format: Article
Language:English
Subjects:
Block copolymers
Chemical reactions
Chemistry
Controllability
Hydrogels
Injectability
Nucleophiles
Polyelectrolytes
Sol-gel processes
Stiffness
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Summary:In the quest for stimuli-responsive materials with specific, controllable functions, coacervate hydrogels have become a promising candidate, featuring sensitive responsiveness to environmental signals enabling control over sol-gel transitions. However, conventional coacervation-based materials are regulated by relatively non-specific signals, such as temperature, pH or salt concentration, which limits their possible applications. In this work, we constructed a coacervate hydrogel with a Michael addition-based chemical reaction network (CRN) as a platform, where the state of coacervate materials can be easily tuned by specific chemical signals. We designed a pyridine-based ABA triblock copolymer, whose quaternization can be regulated by an allyl acetate electrophile and an amine nucleophile, leading to gel construction and collapse in the presence of polyanions. Our coacervate gels showed not only highly tunable stiffness and gelation times, but excellent self-healing ability and injectability with different sized needles, and accelerated degradation resulting from chemical signal-induced coacervation disruption. This work is expected to be a first step in the realization of a new class of signal-responsive injectable materials. Incorporation of reversible Michael addition controlled coacervate crosslinks in a polymer hydrogel led to injectable gels that are responsive to nucleophilic chemical signals, enabling accelerated degradation in culture media after injection.
ISSN:2041-6520
2041-6539
DOI:10.1039/d2sc06935k