Solvent Engineering of Thermo-Responsive Hydrogels Facilitates Strong and Large Contractile Actuations.

Thermo-responsive hydrogels can generate the actuation force through volumetric transitions in response to temperature changes. However, their weak mechanical properties and fragile actuation performance limit robust applications. Existing approaches to enhance these properties have typically depended on additional components, leading to an unavoidable interference to the actuation performance. In this work, robust thermo-responsive hydrogels are fabricated through solvent engineering. A particular solvent, N-methylformamide, interacts affinitively with the carbonyl group of N-isopropylacrylamide monomer, solubilizes the monomer with extremely high concentration, stabilizes chain propagation during polymerization, and greatly increases chain lengths and entanglements of the resulting polymer. The synthesized hydrogels are highly elastic, strong, and tough, displaying remarkable thermo-responsive contractile actuation. The simple synthetic process can broaden its applicability in designing robust functional hydrogel applications.

Stimuli-bioresponsive hydrogels as new generation materials for implantable, wearable, and disposable biosensors for medical diagnostics: Principles, opportunities, and challenges.

Hydrogels are excellent water-swollen polymeric materials for use in wearable, implantable, and disposable biosensors. Hydrogels have unique properties such as low cost, ease of preparation, transparency, rapid response to external conditions, biocompatibility and self-adhesion to the skin, flexibility, and strain sensitivity, making them ideal for use in biosensor platforms. This review provides a detailed overview of advanced applications of stimuli-responsive hydrogels in biosensor platforms, from hydrogel synthesis and functionalization for bioreceptor immobilization to several important diagnostic applications. Emphasis is placed on recent advances in the fabrication of ultrasensitive fluorescent and electrically conductive hydrogels and their applications in wearable, implantable, and disposable biosensors for quantitative measurements. Design, modification, and assembly techniques of fluorescent, ionically conductive, and electrically conductive hydrogels to improve performance will be addressed. The advantages and performance improvements of immobilizing bioreceptors (e.g., antibodies, enzymes, and aptamers), and incorporating fluorescent and electrically conductive nanomaterials are described, as are their limitations. Potential applications of hydrogels in implantable, wearable, disposable portable biosensors for quantitative detection of the various bioanalytes (ions, molecules, drugs, proteins, and biomarkers) are discussed. Finally, the global market for hydrogel-based biosensors and future challenges and prospects are discussed in detail.

Polymeric hydrogels-based materials for wastewater treatment.

Low-cost and reliable wastewater treatment is a relevant issue worldwide to reduce the concentration of environmental pollutants. Industrial effluents containing dyes, heavy metals, and other inorganic and organic compounds can pollute water resources; therefore, novel technologies are required to mitigate and control their release into the environment. Adsorption is one of the simplest methods for treating contaminated water in which a wide spectrum of adsorbents can be used to remove emerging compounds. Hydrogels are interesting materials with high adsorption capacities that can be synthesized via green routes. These adsorbents are promising for large-scale industrial wastewater treatment applications; however, gaps still exist in achieving sustainable commercial implementation. This review focuses on the discussion and analysis of preparation, characterization, and adsorption properties of hydrogels for water purification. The advantages of these polymeric materials for water treatment were analyzed, including their performance in the removal of different organic and inorganic contaminants. Recent advances in the functionalization of hydrogels and the synthesis of novel composites have also been described. The adsorption capacities of hydrogel-based adsorbents are higher than 500 mg/g for different organic and inorganic pollutants, and can reach values of up to >2000 mg/g for organic compounds, significantly outperforming other materials reported for water cleaning. The main interactions involved in the adsorption of water pollutants using hydrogel-based adsorbents were described and explained to allow the interpretation of their removal mechanisms. The current challenges in the implementation of hydrogels for water purification in real-life operations are also highlighted. This review provides an updated picture of hydrogels as interesting materials to address water depollution worldwide.

Thermally tunable hydrogel crosslinking mediated by temperature sensitive liposome.

Hydrogel crosslinking by external stimuli is a versatile strategy to control and modulate hydrogel properties. Besides photonic energy, thermal energy is one of the most accessible external stimuli and widely applicable for many biomedical applications. However, conventional thermal crosslinking systems require a relatively high temperature (over 100 °C) to initiate covalent bond formation. To our knowledge, there has not been a thermally tunable hydrogel crosslinking system suitable for biological applications. This work demonstrates a unique approach to utilize temperature sensitive liposomes to control and modulate hydrogel crosslinking over mild temperature range (below 50 °C). Temperature sensitive liposomes were used to control the release of chemical crosslinkers by moderate temperature changes. The thermally controlled crosslinker release resulted in tunable mechanical and transport properties of the hydrogel. No significant inflammable response observed in the histology results ensured the biocompatibility of the liposome-mediated crosslinkable hydrogel. This work opens new opportunities to implement thermal energy system for control and modulate hydrogel properties.

A Modular and Practical Synthesis of Zwitterionic Hydrogels through Sequential Amine-Epoxy "Click" Chemistry and N-Alkylation Reaction.

In this work, the amine-epoxy "click" reaction is shown to be a valuable general tool in the synthesis of reactive hydrogels. The practicality of this reaction arises due to its catalyst-free nature, its operation in water, and commercial availability of a large variety of amine and epoxide molecules that can serve as hydrophilic network precursors. Therefore, hydrogels can be prepared in a modular fashion through a simple mixing of the precursors in water and used as produced (without requiring any post-synthesis purification step). The gelation behavior and final hydrogel properties depend upon the molecular weight of the precursors and can be changed as per the requirement. A post-synthesis modification through alkylation at the nitrogen atom of the newly formed ß-hydroxyl amine linkages allows for functionalizing the hydrogels. For example, ring-opening reaction of cyclic sulfonic ester gives rise to surfaces with a zwitterionic character. Finally, the established gelation chemistry can be combined with soft lithography techniques such as micromolding in capillaries (MIMIC) to obtain hydrogel microstructures.