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. 2022 Mar 7;12(12):7453-7463.
doi: 10.1039/d2ra00122e. eCollection 2022 Mar 1.

Graphene oxide based crosslinker for simultaneous enhancement of mechanical toughness and self-healing capability of conventional hydrogels

Md Mahamudul Hasan Rumon  1 , Stephen Don Sarkar  1 , Md Mosfeq Uddin  1 , Md Mahbub Alam  1 , Sadia Nazneen Karobi  2 , Aruna Ayfar  1 , Md Shafiul Azam  1 , Chanchal Kumar Roy  1
Affiliations

Graphene oxide based crosslinker for simultaneous enhancement of mechanical toughness and self-healing capability of conventional hydrogels

Md Mahamudul Hasan Rumon et al. RSC Adv. .

Abstract

Extraordinary self-healing efficiency is rarely observed in mechanically strong hydrogels, which often limits the applications of hydrogels in biomedical engineering. We have presented an approach to utilize a special type of graphene oxide-based crosslinker (GOBC) for the simultaneous improvement of toughness and self-healing properties of conventional hydrogels. The GOBC has been prepared from graphene oxide (GO) by surface oxidation and further introduction of vinyl groups. It has been designed in such a way that the crosslinker is able to form both covalent bonds and noncovalent interactions with the polymer chains of hydrogels. To demonstrate the efficacy of GOBC, it was incorporated in a conventional polyacrylamide (PAM) and polyacrylic acid (PAA) hydrogel matrix, and the mechanical and self-healing properties of the prepared hydrogels were investigated. In PAM-GOBC hydrogels, it has been observed that the mechanical properties such as tensile strength, Young's modulus, and toughness are significantly improved by the incorporation of GOBC without compromising the self-healing efficiency. The PAM-GOBC hydrogel with a modulus of about 0.446 MPa exhibited about 70% stress healing efficiency after 40 h. Whereas, under the same conditions a PAM hydrogel with commonly used crosslinker N,N'-methylene-bis(acrylamide) of approximately the same modulus demonstrated no self-healing at all. Similar improvement of self-healing properties and toughness in PAA-GOBC hydrogel has also been observed which demonstrated the universality of the crosslinker. This crosslinker-based approach to improve the self-healing properties is expected to offer the possibility of the application of commonly used hydrogels in many different sectors, particularly in developing artificial tissues.

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Conflict of interest statement

There are no conflicts to declare.

Figures

Fig. 1
Fig. 1. Comparison of (a) UV-Vis spectra and (b) FT-IR spectra of GO, CGO, and GOBC.
Fig. 2
Fig. 2. (a) Comparison of stress–strain curves of PAM hydrogels with different crosslinkers obtained from the tensile tests performed at the same velocity of 100 mm min−1. (b) Comparison of Young's modulus, tensile strength, and toughness of PAM hydrogels with different crosslinkers.
Fig. 3
Fig. 3. The variation of the swelling ratio of different PAM hydrogels in water with immersion time.
Fig. 4
Fig. 4. Stress–strain curves of self-healed PAM hydrogel with (a) 0.01%, (b) 0.025%, (c) 0.035%, and (d) 0.05% GOBC.
Fig. 5
Fig. 5. Real-time images of PAM-GOBC-0.05%; (a) fresh sample, (b) cut sample, (c) healed sample after 20 h, (d) stretched healed sample, (e) a double twist of the healed sample, and (f) bent healed sample.
Fig. 6
Fig. 6. (a) Variation of stress healing efficiency of PAM hydrogels prepared with different crosslinkers. (b) A plot of the self-healing efficiency of different PAM-GOBC hydrogels with the corresponding Young's modulus of the original samples.
Fig. 7
Fig. 7. Self-healing mechanism of PAA-GOBC composite hydrogel; (a) fresh sample, (b) cut sample, and (c) healed sample.
Fig. 8
Fig. 8. Stress–strain curves of self-healing ability for PAA-GOBC-0.05% after 5 min and 40 h healing time.
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