Unveiling Gating Behavior in Piezoionic Effect: toward Neuromimetic Tactile Sensing.

The human perception system's information processing is intricately linked to the nonlinear response and gating effect of neurons. While piezoionics holds potential in emulating the pressure sensing capability of biological skin, the incorporation of information processing functions seems neglected. Here, ionic gating behavior in piezoionic hydrogels is uncovered as a notable extension beyond the previously observed linear responses. The hydrogel can generate remarkably high voltages (700 mV) and currents (7 mA) when indentation forces surpass the threshold. Through a comprehensive analysis involving simulations and experimental investigations, it is proposed that the gating behavior emerges due to significant diffusion differences between cations and anions. To showcase the practical implications of this breakthrough, the piezoionic hydrogels are successfully integrated with prostheses and robot hands, demonstrating that the gating effect enables accurate discrimination between gentle and harsh touch. The advancement in neuromimetic tactile sensing has significant potential for emerging applications such as humanoid robotics and biomedical engineering, offering valuable opportunities for further development of embodied neuromorphic intelligence.

Design of AI-Enhanced and Hardware-Supported Multimodal E-Skin for Environmental Object Recognition and Wireless Toxic Gas Alarm.

Post-earthquake rescue missions are full of challenges due to the unstable structure of ruins and successive aftershocks. Most of the current rescue robots lack the ability to interact with environments, leading to low rescue efficiency. The multimodal electronic skin (e-skin) proposed not only reproduces the pressure, temperature, and humidity sensing capabilities of natural skin but also develops sensing functions beyond it-perceiving object proximity and NO2 gas. Its multilayer stacked structure based on Ecoflex and organohydrogel endows the e-skin with mechanical properties similar to natural skin. Rescue robots integrated with multimodal e-skin and artificial intelligence (AI) algorithms show strong environmental perception capabilities and can accurately distinguish objects and identify human limbs through grasping, laying the foundation for automated post-earthquake rescue. Besides, the combination of e-skin and NO2 wireless alarm circuits allows robots to sense toxic gases in the environment in real time, thereby adopting appropriate measures to protect trapped people from the toxic environment. Multimodal e-skin powered by AI algorithms and hardware circuits exhibits powerful environmental perception and information processing capabilities, which, as an interface for interaction with the physical world, dramatically expands intelligent robots' application scenarios.

In Situ Structural Densification of Hydrogel Network and Its Interface with Electrodes for High-Performance Multimodal Artificial Skin.

The multisensory responsiveness of hydrogels positions them as promising candidates for artificial skin, whereas the mismatch of modulus between soft hydrogels and hard electrodes as well as the poor adhesion and conductance at the interface greatly impairs the stability of electronics devices. Herein, we propose an in situ postprocessing approach utilizing electrochemical reactions between metals (Zn, etc.) and hydrogels to synergistically achieve strong adhesion of the hydrogel-electrode interface, low interfacial impedance, and local strain isolation due to the structural densification of the hydrogel network. The mechanism is that Zn electrochemically oxidizes to Zn2+ and injects into the hydrogel, gradually forming a mechanically interlocked structure, Zn2+-polymer dual-helix structural nodes, and a high-modulus ZnO from the surface to the interior. Compared to untreated samples, the treated sample displays 8.7 times increased interfacial adhesion energy between the hydrogel and electrode (87 J/m2), 95% decreased interfacial impedance (218.8 Ω), and a high-strain isolation efficiency (εtotal/εisolation > 400). Akin to human skin, the prepared sensor demonstrates multimodal sensing capabilities, encompassing highly sensitive strain perception and simultaneous perception of temperature, humidity, and oxygen content unaffected by strain interference. This easy on-chip preparation of hydrogel-based multimodal sensor array shows great potential for health and environment monitoring as artificial skin.

Recent advances in flexible hydrogel sensors: Enhancing data processing and machine learning for intelligent perception.

With the advent of flexible electronics and sensing technology, hydrogel-based flexible sensors have exhibited considerable potential across a diverse range of applications, including wearable electronics and soft robotics. Recently, advanced machine learning (ML) algorithms have been integrated into flexible hydrogel sensing technology to enhance their data processing capabilities and to achieve intelligent perception. However, there are no reviews specifically focusing on the data processing steps and analysis based on the raw sensing data obtained by flexible hydrogel sensors. Here we provide a comprehensive review of the latest advancements and breakthroughs in intelligent perception achieved through the fusion of ML algorithms with flexible hydrogel sensors, across various applications. Moreover, this review thoroughly examines the data processing techniques employed in flexible hydrogel sensors, offering valuable perspectives expected to drive future data-driven applications in this field.

High-Performance Hydrogel Sensors Enabled Multimodal and Accurate Human-Machine Interaction System for Active Rehabilitation.

Human-machine interaction (HMI) technology shows an important application prospect in rehabilitation medicine, but it is greatly limited by the unsatisfactory recognition accuracy and wearing comfort. Here, this work develops a fully flexible, conformable, and functionalized multimodal HMI interface consisting of hydrogel-based sensors and a self-designed flexible printed circuit board. Thanks to the component regulation and structural design of the hydrogel, both electromyogram (EMG) and forcemyography (FMG) signals can be collected accurately and stably, so that they are later decoded with the assistance of artificial intelligence (AI). Compared with traditional multichannel EMG signals, the multimodal human-machine interaction method based on the combination of EMG and FMG signals significantly improves the efficiency of human-machine interaction by increasing the information entropy of the interaction signals. The decoding accuracy of the interaction signals from only two channels for different gestures reaches 91.28%. The resulting AI-powered active rehabilitation system can control a pneumatic robotic glove to assist stroke patients in completing movements according to the recognized human motion intention. Moreover, this HMI interface is further generalized and applied to other remote sensing platforms, such as manipulators, intelligent cars, and drones, paving the way for the design of future intelligent robot systems.

A Strong and Double-sided Self-Adhesive Hydrogel Sensor.

Flexible self-adhesive hydrogel sensors are attracting considerable concerns in recent years. However, creating a self-adhesive hydrogel sensor with excellent mechanical properties remains to be challenging. Herein, a double-sided self-adhesive hydrogel capable of strain sensor with high strength is demonstrated by penetration strategy. The middle poly(acrylic acid)-polyacrylamide/Fe3+ (PAA-PAM/Fe3+ ) tough layer endows the double-sided self-adhesive hydrogel with high mechanical properties, while the bilateral poly[2-(methacryloyloxy) ethyl]dimethyl-(3-sulfopropyl)ammonium hydroxide-polyacrylamide (PSBMA-PAM) adhesive layers are used to ensure excellent adhesiveness on diverse substrates. The tough layer of the double-sided self-adhesive hydrogel sensor shows a strong interface bonding force against the adhesive layer. The double-sided self-adhesive hydrogel sensor enables excellent adhesiveness on diverse substrates. More importantly, it can accurately detect different strains and human motions as a self-adhesive hydrogel strain sensor. This work manifests a new route of structural design to develop a self-adhesive hydrogel sensor with excellent mechanical properties that is suitable for a wide range of applications.

Ultrasensitive and Highly Stretchable Multiple-Crosslinked Ionic Hydrogel Sensors with Long-Term Stability.

Flexible hydrogels are receiving significant attention for their application in wearable sensors. However, most hydrogel materials exhibit weak and one-time adhesion, low sensitivity, ice crystallization, water evaporation, and poor self-recovery, thereby limiting their application as sensors. These issues are only partly addressed in previous studies. Herein, a multiple-crosslinked poly(2-(methacryloyloxy)ethyl)dimethyl-(3-sulfopropyl)ammonium hydroxide-co-acrylamide) (P(SBMA-co-AAm)) multifunctional hydrogel is prepared via a one-pot synthesis method to overcome the aforementioned limitations. Specifically, ions, glycerol, and 2-(methacryloyloxy)ethyl)dimethyl-(3-sulfopropyl)ammonium hydroxide are incorporated to reduce the freezing point and improve the moisture retention ability. The proposed hydrogel is superior to existing hydrogels because it exhibits good stretchability (a strain of 2900%), self-healing properties, and transparency through effective energy dissipation in its dynamic crosslinked network. Further, 2-(methacryloyloxy)ethyl)dimethyl-(3-sulfopropyl)ammonium hydroxide as a zwitterion monomer results in an excellent gauge factor of 43.4 at strains of 1300-1600% by improving the ion transportability and achieving a strong adhesion of 20.9 kPa owing to the dipole-dipole moment. The proposed hydrogel is promising for next-generation biomedical applications, such as soft robots, and health monitoring.

Manufacturing and post-engineering strategies of hydrogel actuators and sensors: From materials to interfaces.

Living bodies are made of numerous bio-sensors and actuators for perceiving external stimuli and making movement. Hydrogels have been considered as ideal candidates for manufacturing bio-sensors and actuators because of their excellent biocompatibility, similar mechanical and electrical properties to that of living organs. The key point of manufacturing hydrogel sensors/actuators is that the materials should not only possess excellent mechanical and electrical properties but also form effective interfacial connections with various substrates. Traditional hydrogel normally shows high electrical resistance (~ MΩ•cm) with limited mechanical strength (<1 MPa), and it is prone to fatigue fracture during continuous loading-unloading cycles. Just like iron should be toughened and hardened into steel, manufacturing and post-treatment processes are necessary for modifying hydrogels. Besides, advanced design and manufacturing strategies can build effective interfaces between sensors/actuators and other substrates, thus enhancing the desired mechanical and electrical performances. Although various literatures have reviewed the manufacture or modification of hydrogels, the summary regarding the post-treatment strategies and the creation of effective electrical and mechanically sustainable interfaces are still lacking. This paper aims at providing an overview of the following topics: (i) the manufacturing and post-engineering treatment of hydrogel sensors and actuators; (ii) the processes of creating sensor(actuator)-substrate interfaces; (iii) the development and innovation of hydrogel manufacturing and interface creation. In the first section, the manufacturing processes and the principles for post-engineering treatments are discussed, and some typical examples are also presented. In the second section, the studies of interfaces between hydrogels and various substrates are reviewed. Lastly, we summarize the current manufacturing processes of hydrogels, and provide potential perspectives for hydrogel manufacturing and post-treatment methods.

Stretchable, compressible, and conductive hydrogel for sensitive wearable soft sensors.

Conductive hydrogels hold great promises in wearable soft electronics. However, the weak mechanical properties, low sensitivity and the absence of multifunctionalities (e.g., self-healing, self-adhesive, etc.) of the conventional conductive hydrogels limit their applications. Thus, developing multifunctional hydrogels may address some of these technical issues. In this work, a multifunctional conductive hydrogel strain sensor is fabricated by incorporating a conductive polymer Poly(3,4-ethylenedioxythiophene)-poly(styrenesulfonate) (PEDOT: PSS) into a mechanically robust poly (vinyl alcohol) (PVA)/ poly (acrylic acid) (PAA) double network (DN) hydrogel. The as-prepared hydrogel sensor could span a wide spectrum of mechanical properties by simply tuning the polymer composition and the number of freezing-thawing cycles. In addition, the dynamic hydrogen bonding interactions endow the hydrogel sensor with self-healing property and reversible adhesiveness on diverse substrates. Moreover, the hydrogel sensor shows high sensitivity (Gauge Factor from 2.21 to 3.82) and can precisely detect some subtle human motions (e.g., pulse and vocal cord vibration). This work provides useful insights into the development of conductive hydrogel-based wearable soft electronics.

A General Protein Unfolding-Chemical Coupling Strategy for Pure Protein Hydrogels with Mechanically Strong and Multifunctional Properties.

Protein-based hydrogels have attracted great attention due to their excellent biocompatible properties, but often suffer from weak mechanical strength. Conventional strengthening strategies for protein-based hydrogels are to introduce nanoparticles or synthetic polymers for improving their mechanical strength, but often compromise their biocompatibility. Here, a new, general, protein unfolding-chemical coupling (PNC) strategy is developed to fabricate pure protein hydrogels without any additives to achieve both high mechanical strength and excellent cell biocompatibility. This PNC strategy combines thermal-induced protein unfolding/gelation to form a physically-crosslinked network and a -NH2/-COOH coupling reaction to generate a chemicallycrosslinked network. Using bovine serum albumin (BSA) as a globular protein, PNC-BSA hydrogels show macroscopic transparency, high stability, high mechanical properties (compressive/tensile strength of 115/0.43 MPa), fast stiffness/toughness recovery of 85%/91% at room temperature, good fatigue resistance, and low cell cytotoxicity and red blood cell hemolysis. More importantly, the PNC strategy can be not only generally applied to silk fibroin, ovalbumin, and milk albumin protein to form different, high strength protein hydrogels, but also modified with PEDOT/PSS nanoparticles as strain sensors and fluorescent fillers as color sensors. This work demonstrates a new, universal, PNC method to prepare high strength, multi-functional, pure protein hydrogels beyond a few available today.

Chitosan-driven skin-attachable hydrogel sensors toward human motion and physiological signal monitoring.

Recently, flexible and wearable sensors assembled from conductive hydrogels have attracted widespread attention. However, it is still a great challenge to make hydrogels with sufficient mechanical properties, self-adhesiveness and strain sensitivity. Here, a strong, tough, and self-adhesive hydrogel is successfully fabricated by a one-pot method, which introducing chitosan and 2-acrylamido-2-methylpropane sulfonic acid into the polyacrylamide network. The hydrogels exhibited adhesion (the peel strength reaches 798 N/m), mechanical property (The breaking strength and strain can reach 111 kPa and 2839%) and electrical conductivity (conductivity up to 0.0848 S/cm), which are suitable for wearable epidermal sensors. Besides, the hydrogels also possessed transparency. Therefore, this work would provide a novel insight on the fabrication of multi-functional self-adhesive hydrogel sensors.

Passive and wireless, implantable glucose sensing with phenylboronic acid hydrogel-interlayer RF resonators.

A phenylboronic acid-based, hydrogel-interlayer Radio-Frequency (RF) resonator is demonstrated as a highly-responsive, passive and wireless sensor for glucose monitoring. Constructs are composed of unanchored, capacitively-coupled split rings interceded by glucose-responsive hydrogels. Phenylboronic acid-hydrogels exhibit volumetric and dielectric variations in response to environmental glucose concentrations-these are efficiently converted to large shifts in the resonant response of interlayer-RF sensors. These tiny, stretchable and scalable sensors (5 mm × 5 mm x 250 µm) require no microelectronics or power at the sensing node and can be read-out remotely via near-field coupling. Sensors exhibit high sensitivities (~10% shift in resonant frequency-corresponding to 50 MHz-per 150 mg/dL of glucose), possess a limit of detection of 10 mg/dL, and a step response time of approximately 1 h to abrupt shifts in carbohydrate concentration. Notably, these sensors exhibited no signal drift or hysteresis over the time periods characterized herein (45 days at room temperature). We transform sensors into bioelectronic RF reporter-tags via the attachment of a single LED-these remotely report on glucose concentration via emitted light. We anticipate the non-degradative, long-term nature of both RF read-out and phenylboronic acid-based hydrogels will enable biosensors capable of long-term, remote read-out of glucose.