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Double dynamic cellulose nanocomposite hydrogels with environmentally adaptive self-healing and pH-tuning properties

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Abstract

Dynamic hydrogels are prepared by either dynamic covalent bonds or supramolecular chemistry. Herein, we develop a dynamic hydrogel by combining both dynamic covalent bonds and supramolecular chemistry that exhibits environmentally adaptive self-healing and pH-tuning properties. To do so, we prepared a gelatin–nanopolysaccharide mixed hydrogel containing pyrogallol/catechol groups and trivalent metal ions. The as-prepared hydrogels are able to heal damage inflicted on them under acidic (pH 3 and 6), neutral (pH 7), and basic (pH 9) environments. The mechanism of healing at acidic and neutral pHs is dominated by coordination bonds between pyrogallol/catechol groups of tannic acid and ferric ions, whilst Schiff-base reaction between amines from gelatin and dialdehyde-modified cellulose nanocrystals dominates the formation of dynamic hydrogels at basic pH. Self-healing mechanism of the hydrogel at all pHs occurred at ambient temperature without any external stimuli. The hydrogels also showed different mechanical, electrical, self-healing, and self-adhesiveness properties in different pH levels. Furthermore, the hydrogels showed printability and injectability at pH 6.

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Correspondence to Abbas Z. Kouzani.

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Heidarian, P., Kouzani, A.Z., Kaynak, A. et al. Double dynamic cellulose nanocomposite hydrogels with environmentally adaptive self-healing and pH-tuning properties. Cellulose 27, 1407–1422 (2020). https://doi.org/10.1007/s10570-019-02897-w

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  • DOI: https://doi.org/10.1007/s10570-019-02897-w

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