Conductive gels have received extensive attention in flexible electronics due to their diverse characteristics. The requirement for versatility and incompatibility of the conductive fillers with the hydrogel matrix remain a challenge for hydrogels. Herein, the cellulose nanofiber stabilized liquid metal droplets are utilized to initiate the polymerization and simultaneously serve as solid conductive fillers to construct the polyacrylamide/MXene/glycerol hydrogel with eligible stretchability (1000%) and high environmental adaptability (−25 to 80 °C) for multifunctional sensing. The hydrogel is utilized as a flexible electrode to construct the triboelectric nanogenerator for mechanical energy harvesting and conversion as well as self-powered sensing. Importantly, as a versatile sensor, it combines temperature sensing and deformation sensing with a wide range of stimulus responses and exceptional sensing performance. The flexible temperature and strain sensors are realized with superior thermosensitivity and strain sensitivity. In addition, the hydrogel exhibits favorable photothermal antibacterial ability. This work opens new avenues for the preparation of photothermal, conductive, stress and thermal sensitive hydrogels for multimodal sensors, sketching a promising future for them in flexible and wearable electronics. 

A stretchable, environmentally tolerant, and photoactive liquid metal/MXene hydrogel for high performance temperature monitoring, human motion detection and self-powered application

Stretchable on-skin touchless screen sensor enabled by ionic hydrogel

As personal portable devices, wearable sensors supply a leading-edge pathway to diagnose various diseases through actuating biological, physical, and chemical sensing capabilities. This could be commonly carried out via recording continuous and real-time of the patient's physiological statuses, as well as pathophysiological information. Although wearable sensor technology is in the infancy stage, tremendous attempts have been devoted to approaching flexible polymeric sensors. Among various polymer candidates applicable for synthesizing flexible and wearable sensors, the bio-based ones have piqued more interest due to their biocompatibility, biodegradability, eco-friendly features, and cost-effectiveness. Additionally, several fabrication techniques have been professed to architect efficient frameworks, such as films, hydrogels, aerogels, ferrogels, 3D layers, electrospun mats, and textiles. In this review, different mechanisms declared to engineer wearable sensors are overviewed. Then, regarding the advantages observed for bio-based polymers, the focused studies on the fabrication of natural-based wearable sensors are described. Notably, cellulose, chitosan, silk, gelatin, and alginate's role in sensing functionality is highlighted. Accordingly, this review has opened a new window to ahead opportunities for wearable sensors based on natural polymers. It is hoped that the new generation of sensors will be launched by combining emerging achievements obtained from employing sustainable and green elements and miniaturized sensor structures. 

Recent progress of bio-based smart wearable sensors for healthcare applications

Kirigami, a traditional paper‐cutting art, is a promising method for creating mechanically robust circuitry for unconventional devices capable of extreme stretchability through structural deformation. In this study, this design approach is expanded upon by introducing Liquid Metal based Elastic Kirigami Electrodes (LM‐eKE) in which kirigami‐patterned soft elastomers are coated with eutectic gallium‐indium (EGaIn) alloy. Overcoming the mechanical and electrical limitations of previous efforts with paper‐like kirigami, the all soft LM‐eKE can be stretched to 820% strain while the electrical resistance only increases by 33%. This is enabled by the fluidic properties of the EGaIn coating, which maintains high electrical conductivity even as the elastic substrate undergoes extreme deformation. Applying the LM‐eKE to human knee joints and fingers, the resistance change during physical activities is under 1.7%, thereby allowing for stable electrical operation of wearable health monitoring devices for tracking electroencephalogram (EEG) signals and other physiological activity.

Highly Stretchable and Strain‐Insensitive Liquid Metal based Elastic Kirigami Electrodes (LM‐eKE)

Continuous temperature monitoring by flexible hydrogel-based electronics achieves rapid advances, overcoming the drawbacks of rigid and unportable thermocouples. However, an open question is whether and how the thermosensitive hydrogel designing can prevent mechanical mismatching between devices and skin-tissues and reduces interfacial failure. Herein, a versatile hydrogel-based thermistor epidermal sensor (HTES) paradigm is engineered consisting of thermosensitive and self-adhesive function layer (PEST) in tandem with a surface spraying Ag interdigital electrode. Leveraging the advantage of catechol chemistry inspired tannic acid-coated cellulose nanocrystals, the resultant PEST achieves the adhesion-cohesion equilibrium along with superior thermosensitivity. The assembled HTES thereby yields unprecedented features of superior thermosensitivity (TCR = 1.43% °C−1), exceptional mechanical integrity (hammering 200 cycles, current variation <9%), impressive interfacial compatibility (adhesion strength, 25 kPa), and environmental stability (thermosensation retention of 98% over 5 days). By in-situ microstructure observation, the unique geometrical synchronization of HTES with arbitrary curvilinear surfaces (e.g., sphere, cone, and saddle) stemming from elastic dissipation and discrete rupture of the adhesive fibrillar bridges is validated, affording competitive advantages than that of the state-of-the-art thermistor electronics for alleviating the interfacial deterioration, which dramatically inspires advanced HTES design strategies and paves the way for commercialization of attachable thermistor electronics. 

A Robust and Adhesive Hydrogel Enables Interfacial Coupling for Continuous Temperature Monitoring

As an on‐skin electronic device, artificial skin shows great potential in medical monitoring and personal electronics, which also holds promise to develop human‐machine merging interfaces. However, merging artificial skins with human bodies is largely restricted by the dissimilarity of material compositions in existing artificial skins and biological tissues. Naturally conductive protein is a potential material candidate for artificial skins, nevertheless, it suffers from the critical issue of dehydration which harms its proton conductivity. Inspired by the sebum membrane of human skin, herein, a protein‐based bioprotonic hydrogel (PBH) with reliable water retention ability is reported for artificial skins. The bovine serum albumin with natural proton conductivity is utilized in the PBH, and the glycerol that originally presents on human skin surface is used as an artificial sebum membrane to retain water. The PBH can act as a bioprotonic skin (B‐skin) for collecting electrophysiological signals and self‐powered sensing. Based on the B‐skin, intelligent robot and cellphone control systems are demonstrated. Compared with present artificial skins, this B‐skin is all made out of biological materials that are consistent with material components of human skin tissues including proteins, endogenous glycerol, and water. Such a B‐skin may enable the development of next‐generation human‐machine merging interfaces.

Sebum‐Membrane‐Inspired Protein‐Based Bioprotonic Hydrogel for Artificial Skin and Human‐Machine Merging Interface

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Sebum‐Membrane‐Inspired Protein‐Based Bioprotonic Hydrogel for Artificial Skin and Human‐Machine Merging Interface