Hydrogel shows great potential as a flexible wearable electronic device. However, the practical application of hydrogel is still significantly limited due to the poor functional stability caused by swelling behavior, non-frost resistance caused by high water content, and obvious creep behavior under repeated external force. In this work, macromolecular lignin with a three-dimensional network structure, and active functional groups are introduced into the hydrogel through the esterification grafting reaction of methacryloyl chloride. The introduction of lignin effectively improves the antiswelling, antifreezing, and creep resistance of the hydrogel sensor, while maintaining the mechanical properties (elongation at break > 350%, tensile strength > 1.5 MPa) and electrical conductivity (10 S/m). Under extreme environments, the toughness, tensile strength, and elongation at break of the hydrogel remain at more than 96%. Furthermore, the antifreezing, creep resistance, and conductivity of hydrogel sensors are not significantly affected after immersion in water for a long time (72 h). This work proposes a simple strategy to improve the antiswelling, antifreezing, and anticreep properties of hydrogels, which has guiding significance for the preparation of high-performance flexible wearable electronic materials. 

Novel Lignin Hydrogel Sensors with Antiswelling, Antifreezing, and Anticreep Properties

Biodegradable conductive films are crucial for the sustainable development of wearable electronics. In this work, a flexible and degradable conductive film was prepared based on a carefully designed interface of polylactic acid (PLA) electrospun fibers and silver nanowires (AgNWs). The amphiphilic triblock copolymer was added to PLA solution for electrospinning, followed by solvent posttreatment to induce the hydrophilic block of the amphiphilic triblock copolymer to migrate to the fiber surface. Dopamine can be uniformly polymerized on the surface of hydrophilic PLA fibers, and the prepared PLA@PDA fiber film can form a good interface combination with AgNWs. The electrical conductivity of AgNWs/PLA@PDA flexible film can reach 258.5 S cm−1, showing obvious Joule heating effect and good mechanical properties. Degradation experiments showed that in phosphate buffered saline, the PLA molecular chain showed a dynamic equilibrium due to the scission and rearrangement of the ester groups and degraded slowly, while AgNWs/PLA@PDA degraded rapidly under alkaline conditions. Our study provides a simple and controllable method to prepare flexible degradable electronic films, which is expected to be applied to flexible wearable bioelectrodes.

Biodegradable flexible conductive film based on sliver nanowires and PLA electrospun fibers

The complete healing of skin wounds has been a challenge in clinical treatment. Self-healing hydrogels are special hydrogels formed by distinctive physicochemically reversible bonds, and they are considered promising biomaterials in the biomedical field owing to their inherently good drug-carrying capacity as well as self-healing and repair abilities. Moreover, natural polymeric materials have received considerable attention in skin tissue engineering owing to their low cytotoxicity, low immunogenicity, and excellent biodegradation rates. In this paper, we review recent advances in the design of self-healing hydrogels based on natural polymers for skin-wound healing applications. First, we outline a variety of natural polymers that can be used to construct self-healing hydrogel systems and highlight the advantages and disadvantages of different natural polymers. We then describe the principle of self-healing hydrogels in terms of two different crosslinking mechanisms—physical and chemical—and dissect their performance characteristics based on the practical needs of skin-trauma applications. Next, we outline the biological mechanisms involved in the healing of skin wounds and describe the current application strategies for self-healing hydrogels based on these mechanisms. Finally, we analyze and summarize the challenges and prospects of natural-material-based self-healing hydrogels for skin applications. 

Self-healing hydrogels based on biological macromolecules in wound healing: A review.

The electrospinning technology has set off a tide and given rise to the attention of a widespread range of research territories, benefiting from the enhancement of nanofibers which made a spurt of progress. Nanofibers, continuously produced via electrospinning technology, have greater specific surface area and higher porosity and play a non-substitutable key role in many fields. Combined with the degradability and compatibility of the natural structure characteristics of polysaccharides, electrospun polysaccharide nanofiber membranes gradually infiltrate into the life field to help filter air contamination particles and water pollutants, treat wounds, keep food fresh, monitor electronic equipment, etc., thus improving the life quality. Compared with the evaluation of polysaccharide-based nanofiber membranes in a specific field, this paper comprehensively summarized the existing electrospinning technology and focused on the latest research progress about the application of polysaccharide-based nanofiber in different fields, represented by starch, chitosan, and cellulose. Finally, the benefits and defects of electrospun are discussed in brief, and the prospects for broadening the application of polysaccharide nanofiber membranes are presented for the glorious expectation dedicated to the progress of the eras. 

Electrospinning and electrospun polysaccharide-based nanofiber membranes: A review.

Polysaccharide based transdermal patches for chronic wound healing: Recent advances and clinical perspective.

Tunable and Self-Healing Properties of Polysaccharide-Based Hydrogels through Polymer Architecture Modulation

A nanofiber membrane is an ideal carrier for constructing a typical three-dimensional conductive network. Inspired by the biomimetic scale-like nanostructure, polysaccharide-based piezoresistive material with outstanding Joule heating performance, thermal efficiency, and high conductivity is developed, presenting a potential indicator material with the color shifting function for intelligent skin or soft robots in practical applications. The stable core-shell structure due to the in-situ polymerization of polypyrrole (PPy) on the electrospun nanofiber endows the piezoresistive sensor (s-PGG@PPy) with a broad pressure range (0.13–128.46 kPa), high sensitivity (52.42 kPa−1) and fast response time (26 ms). The free motion of π electrons along the nanofibers between carbon atoms perfectly made it an attractive candidate for real-time monitoring of human activities, including bending of fingers, wrist, knee, and facial expression. In addition, designing s-PGG@PPy is to be connected in parallel and composed of an indication function glove, which shows different brightness with finger pressure. Consequently, the reported piezoresistive sensor represents a potential for wearable bioelectronics. 

Biomimetic scale-like polysaccharide-based highly-sensitive piezoresistive sensor with “shell-core” nanostructure

The development of a natural polysaccharide-based nanofiber membrane to satisfy the requirements of slight, tenuous, and multi-performance is of great significance but still challenging. Herein, we exemplified a simple yet general strategy combining electrospinning to engineer conventional nanofiber membrane containing poly(vinyl alcohol), plant polysaccharide, and glycerol, scaling up visibility and keeping haze by soaking in deep eutectic solvent (DES) in the wake of noticeable variation of fiber morphology. The high optical haze (up to 92% at 550 nm) membrane with a great tensile stress of 2.5 MPa is a degradable and recyclable green material. The ultrathin membrane (0.1 mm) achieved health monitoring with a rapid response time of 2 s due to the conductivity of DES (choline chloride and urea). In addition, the DES fully expresses that not only the degradation of nanofiber membrane belongs to nature, but also urea could be utilized as fertilizer for heterogeneous soils and crops. 

Polysaccharides-based ultra-thin membrane with high haze, conductivity, and recyclability

Enzymatically mediated Gleditsia sinensis galactomannan based hydrogel inspired by wound healing process.

Sustainable bacterial cellulose-based composite aerogels with excellent flame retardant and heat insulation

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