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. 2023 Apr 14;15(8):1876.
doi: 10.3390/polym15081876.

Dynamic Crosslinked Injectable Mussel-Inspired Hydrogels with Adhesive, Self-Healing, and Biodegradation Properties

Ruixiao Wang  1 , Liqun Liu  1 , Xiang He  1   2 , Zongmei Xia  1 , Zhenjie Zhao  1 , Zhenhao Xi  1   2 , Juan Yu  1 , Jie Wang  1
Affiliations

Dynamic Crosslinked Injectable Mussel-Inspired Hydrogels with Adhesive, Self-Healing, and Biodegradation Properties

Ruixiao Wang et al. Polymers (Basel). .

Abstract

The non-invasive tissue adhesives with strong tissue adhesion and good biocompatibility are ideal for replacing traditional wound treatment methods such as sutures and needles. The self-healing hydrogels based on dynamic reversible crosslinking can recover their structure and function after damage, which is suitable for the application scenario of tissue adhesives. Herein, inspired by mussel adhesive proteins, we propose a facile strategy to achieve an injectable hydrogel (DACS hydrogel) by grafting dopamine (DOPA) onto hyaluronic acid (HA) and mixing it with carboxymethyl chitosan (CMCS) solution. The gelation time and rheological and swelling properties of the hydrogel can be controlled conveniently by adjusting the substitution degree of the catechol group and the concentration of raw materials. More importantly, the hydrogel exhibited rapid and highly efficient self-healing ability and excellent biodegradation and biocompatibility in vitro. Meanwhile, the hydrogel exhibited ~4-fold enhanced wet tissue adhesion strength (21.41 kPa) over the commercial fibrin glue. This kind of HA-based mussel biomimetic self-healing hydrogel is expected to be used as a multifunctional tissue adhesive material.

Keywords: carboxymethyl chitosan; hyaluronic acid; in situ hydrogel; tissue adhesive.

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Conflict of interest statement

The authors declare no conflict of interest.

Figures

Figure 1
Figure 1
Schematic diagram of crosslinking within DACS hydrogels by mixing DAHA and CMCS solutions.
Figure 2
Figure 2
Effect of gelation time by DAHA and CMCS concentrations. [DAHA] = 0.5–3.5 wt%, [CMCS] = 2.5 wt% (a), [CMCS] = 1.0–3.0 wt%), [DAHA] = 3 wt% (b); Effect of swelling ratio by DAHA and CMCS concentrations. [DAHA] = 1.0–3.0 wt%, [CMCS] = 2.5 wt% (c), [CMCS] = 2.0–3.0 wt%, and [DAHA] = 3 wt% (d).
Figure 3
Figure 3
Rheometric tests of DACS hydrogels. (a) The amplitude sweep tests and (b) the time sweep tests at a frequency of 1 Hz and a strain of 1%.
Figure 4
Figure 4
(a) Evaluation of injectability of the DACS with a double barrel spiral needle; (b) Schematic diagram of DACS hydrogel used for the wound; (c) Self-healing ability of DACS hydrogels and schematic diagram of the self-healing process; and (d) Rheological properties of DACS hydrogels under variable external strain (1–700%).
Figure 5
Figure 5
(a) Surface adaptability of DACS hydrogels: ceramic, metal, and plastic; (b) Average adhesion strength on wood, metal, and glass.
Figure 6
Figure 6
The fluorescence image of L929 mouse fibroblast cells cultured with control and DACS hydrogels leaching solution on the first (D1), second (D2), and third day (D3), respectively.
Figure 7
Figure 7
(a) The schematic diagram of lap-shear test of DACS hydrogels on porcine skin; (b) The average adhesion strength of DACS hydrogels with different DA content (17.9%, 55.6%, 81.5%, and 88.5%) on porcine skin tissue surfaces.
Figure 8
Figure 8
In vitro degradation of DACS hydrogels with different concentrations of DAHA (1.0–3.0 wt%).
See this image and copyright information in PMC

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