Responsive laminarin-boronic acid self-healing hydrogels for biomedical applications

authors	Amaral, AJR; Gaspar, VM; Mano, JF
nationality	International
journal	POLYMER JOURNAL
keywords	POLYMERS; OXIDATION
abstract	The precise chemical modification of marine-derived biopolymers provides a unique opportunity for fabricating a toolbox of bioactive (bio)materials with modulated physicochemical and biological properties. Herein, the beta-glucan laminarin was functionalized with phenylboronic acid (PBA) moieties that impart chemical reactivity toward diol-containing polymers via boronate esterification. The modification, which involved a two-pot reaction, was successfully confirmed by nuclear magnetic resonance spectroscopy. The resultant biopolymer readily established boronate ester-crosslinked hydrogels with poly(vinyl alcohol) (PVA) within seconds under physiological conditions. These hydrogels exhibited improved rheological properties, which were easily tunable, and revealed a rapid self-healing behavior upon rupture. Moreover, boronate ester bonds enabled the fabrication of reactive oxygen species-responsive and shear-thinning gels that can be administered in situ and respond to the oxidation state of the surrounding microenvironment. Importantly, due to the catalyst-free and mild-crosslinking conditions, the generated laminarin-PBA/PVA hydrogels did not show toxicity upon direct contact with preosteoblasts for up to 48 h, and thus constitute a promising platform for tissue engineering and drug delivery applications.
publisher	NATURE PUBLISHING GROUP
issn	0032-3896
isbn	1349-0540
year published	2020
volume	52
issue	8
beginning page	997
ending page	1006
digital object identifier (doi)	10.1038/s41428-020-0348-3
web of science category	Polymer Science
subject category	Polymer Science
unique article identifier	WOS:000529488600001