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Enabling the living capability of secreting liquids dynamically triggered by external stimuli while maintaining the bulk frame is a significant challenge for mucosa-inspired hydrogels. A mucosa-inspired electro-responsive hydrogel is developed in this study using the synergy between electro-responsive silk fibroin supramolecular non-covalent networks and covalent polyacrylamide and polyvinyl alcohol polymer networks. The formed supramolecular-covalent hydrogel exhibits a partial gel-sol transition upon the application of an electric field, and the liquid layer on the hydrogel surface near the cathode is used to mimic the mucus-secreting capability to regulate lubrication. The electro-responsive lubricating process can operate under a safe voltage and exhibits good reversibility. It is also a universal strategy to construct an electro-responsive hydrogel by introducing an electro-responsive supramolecular network into the polymer network. This mucosa-inspired electro-responsive supramolecular-covalent hydrogel offers a promising method for designing soft actuators or robots that can regulate lubrication using an electric strategy.

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A facile, universal and highly efficient approach for producing a self-cleaning electrochemical protein-imprinting biosensor based on dual stimuli-responsive memory hydrogels via free-radical polymerisation is described. As confirmed by static contact angle and scanning electron microscopy results, the imprinted hydrogels exhibited reversible conformational changes after being simulated by an external electric field and temperature. By exploring the properties of imprinted hydrogels for sensing applications, the electrochemical protein-imprinting biosensor was originally fabricated on a glassy carbon electrode using the drop-casting method. Because of the trigger gates of the temperature and electric field, the biosensor demonstrated excellent self-cleaning behaviours compared with other corresponding electric-field or thermo-responsive imprinting biosensors. Moreover, the prepared biosensor exhibited satisfactory selectivity, good biocompatibility, comparable limits of detection and linearity ranges as well as acceptable stability toward bovine serum albumin. Consequently, the biosensor was successfully employed to simultaneously enrich, detect and extract bovine serum albumin from complex biological samples; the process was dynamic, controllable and harmless to the template under the dual external stimuli. Thus, the proposed biosensor exhibited considerable potential in controlled drug/chemical delivery and smart sensing for bioanalyses involving dual stimuli-responsive behaviours.

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In this work, electro-responsive chitosan/ionic liquid-based hydrogels were synthetized for the first time, envisaging the development of iontophoretic biomaterials for the controlled release/permeation of charged biomolecules. The main goal was to enhance and tune the physicochemical, mechanical, electro-responsive, and haemostatic properties of chitosan-based biomaterials to obtain multi-stimuli responsive (responsive to electrical current, ionic strength, and pH) and mechanically stable hydrogels. To accomplish this objective, polycationic semi-interpenetrating copolymer networks (semi-IPN) were prepared by combining chitosan (CS) and ionic liquid-based polymers and copolymers, namely poly(1-butyl-3-vinylimidazolium chloride) (poly(BVImCl)) and poly(2-hydroxymethyl methacrylate-co-1-butyl-3-vinylimidazolium chloride) (poly(HEMA-co-BVImCl)). Results show that prepared semi-IPNs presented high mechanical stability and were positively charged over a broad pH range, including basic pH. Semi-IPNs also presented faster permeation and release rates of lidocaine hydrochloride (LH), under external electrical stimulus (0.56 mA/cm2) in aqueous media at 32 °C. The kinetic release constants and the LH diffusion coefficients measured under electrical stimulus were ~1.5 and > 2.7 times higher for those measured for passive release. Finally, both semi-IPNs were non-haemolytic (haemolytic index ≤0.2%) and showed strong haemostatic activity (blood clotting index of ~12 ± 1%). Altogether, these results show that the prepared polycationic semi-IPN hydrogels presented advantageous mechanical, responsive and biological properties that enable them to be potentially employed for the design of new, safer, and advanced stimuli-responsive biomaterials for several biomedical applications such as haemostatic and wound healing dressings and iontophoretic patches.

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Electric fields are among physical stimuli that have revolutionized therapy. Occurring endogenously or exogenously, the electric field can be used as a trigger for controlled drug release from electroresponsive drug delivery systems, can stimulate wound healing and cell proliferation, may enhance endocytosis or guide stem cell differentiation. Electric field pulses may be applied to induce cell fusion, can increase the penetration of therapeutic agents into cells, or can be applied as a standalone therapy to ablate tumors. This review describes the main therapeutic trends and overviews the main physical, chemical and biological mechanisms underlying the actions of electric fields. Overall, the electric field can be used in therapeutic approaches in several ways. The electric field can act on drug carriers, cells and tissues. Understanding the multiple effects of this powerful tool will help harnessing its full therapeutic potential in an efficient and safe way.

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