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Materials with stimuli-switchable properties are widespread in nature. Through biomimicry, stimuli-responsive hydrogels have received increasing research in recent years. In particular, hydrogels with stimuli-tunable mechanical properties provide an important platform for designing new materials with specific applications such as 3D printing, soft robot, and tunable adhesion. Herein, the state-of-the-art of hydrogels with stimuli-responsive toughness is reviewed in detail. Characteristic reinforcement mechanisms are fully discussed first, followed by systematical demonstrations of various smart hydrogels responding to various stimuli. In particular, special attention is paid to thermal, light, pH, and salt triggers because of their broad applications and easy implementation. Furthermore, the applications of these smart hydrogels are included. In addition to the overview of recent advances, we finally summarize the critical challenges of current discoveries and make an outlook for the following work, which we anticipate to lead to substantial progress of these responsive materials in the future.

Abstract:In this paper, water-soluble 2,2,6,6-tetramethylpiperidine-1-oxyl (TEMPO)-oxidized cellulose with a high degree of oxidation was prepared by a two-step process using bamboo dissolving pulp. The first step was to destroy the cellulose crystal I by NaOH/urea solution to obtain cellulose powder with decreased crystallinity. The second step was to oxidize the cellulose powder by TEMPO oxidation. The TEMPO-oxidized cellulose was analyzed by Fourier transform infrared spectroscopy (FTIR), conductimetry, X-ray diffraction (XRD), fiber analyzer, and transmission electron microscopy (TEM). FTIR showed that the hydroxymethyl groups in cellulose chains were converted into carboxyl groups. The degree of oxidation measured by conductimetry titration was as high as 91.0%. The TEMPO-oxidized cellulose was soluble in water for valuable polyelectrolytes and intermediates.

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The nonantibacterial and low strength properties of sodium alginate films negatively impact their application for food packaging. In order to improve these properties, a novel chitosan-benzalkonium chloride (C-BC) complex was prepared by ionic gelation using tripolyphosphate (TPP) as a coagulant, and a biocomposite obtained through the adsorption of C-BC complex on microfibrillated cellulose, MFC/C-BC, was then incorporated into a sodium alginate film. The TEM image showed that the C-BC nanoparticles were spherical in shape with a diameter of about 30 nm, and the adsorption equilibrium time of these nanoparticles on the surface of MFC was estimated to be 6 min under the driving forces of hydrogen bonds and electrostatic interactions. According to the disc diffusion method, the MFC/C-BC biocomposite-incorporated sodium alginate film exhibited remarkable antibacterial activity against Staphylococcus aureus and certain antibacterial activity against Escherichia coli . The strength tests indicated that the tensile strength of the composite sodium alginate film increased about 225% when the loading of MFC/C-BC biocomposite was 10 wt %. These results suggested that the MFC/C-BC biocomposite-incorporated sodium alginate film with excellent antibacterial and strength properties would be a promising material for food packaging, and the MFC/C-BC may also be a potential multifunctional biocomposite for other biodegradable materials.

Self-healing gels based on reshuffling disulfide bonds have attracted great attention due to their ability to restore structure and mechanical properties after damage. In this work, self-healing gels with different cellulose nanocrystals (CNC) contents were prepared by embedding the thiuram disulfide bonds into gels via polyaddition. By the reshuffling of thiuram disulfide bonds, the CNC-containing gels repair the crack and recover mechanical properties rapidly under visible light in air. The thiuram disulfide-functionalized gels with a CNC content of 2.2% are highly stretchable and can be stretched approximately 42.6 times of their original length. Our results provide useful approaches for the preparation of dynamic CNC-containing gels with implications in many related engineering applications.

Novel magnetic superhydrophobic cellulose-based microspheres were fabricated using poly(DOPAm-co-PFOEA), which provide remarkable stability to liquid marbles with various liquids for liquid droplet transportation and manipulation.

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