Energy and water are of fundamental importance for our modern society, and advanced technologies on sustainable energy storage and conversion as well as water resource management are in the focus of intensive research worldwide. Beyond their traditional biological applications, hydrogels are emerging as an appealing materials platform for energy- and water-related applications owing to their attractive and tailorable physiochemical properties. In this review, we highlight the highly tunable synthesis of various hydrogels, involving key synthetic elements such as monomer/polymer building blocks, cross-linkers, and functional additives, and discuss how hydrogels can be employed as precursors and templates for architecting three-dimensional frameworks of electrochemically active materials. We then present an in-depth discussion of the structure-property relationships of hydrogel materials based on fundamental gelation chemistry, ultimately targeting properties such as enhanced ionic/electronic conductivities, mechanical strength, flexibility, stimuli-responsiveness, and desirable swelling behavior. The unique interconnected porous structures of hydrogels enable fast charge/mass transport while offering large surface areas, and the polymer-water interactions can be regulated to achieve desirable water retention, absorption, and evaporation within hydrogels. Such structure-derived properties are also intimately coordinated to realize multifunctionality and stability for different target devices. The plethora of stimulating examples is expounded with a focus on batteries, supercapacitors, electrocatalysts, solar water purification, and atmospheric water harvesting, which showcase the unprecedented technological potential enabled by hydrogels and hydrogel-derived materials. Finally, we study the challenges and potential ways of tackling them to reveal the underlying mechanisms and transform the current development of hydrogel materials into sustainable energy and water technologies.

Hydrogels and Hydrogel-Derived Materials for Energy and Water Sustainability.

Recently, flexible and wearable electronics have gained considerable research interest due to their potential applications in wearable devices, energy storage materials, electronic skins, sensors, etc. Compared to elastomers, hydrogels demonstrate more potential for flexible electronics because of their biomimetic structures, suitable mechanical properties and excellent biocompatibility. Among all the designs, nanocomposite hydrogel-based strain and pressure sensors which can transmit external stimulus to electrical signals have been intensely investigated due to their high mechanical strength, considerable conductivity and outstanding sensitivity. Numerous reports have been dedicated to the designs, preparations and applications of nanocomposite hydrogels. This review provides an up-to-date and comprehensive summary of research progresses of nanocomposite hydrogel-based strain and pressure sensors including designing strategies, preparing methods and applications of the five nanofiller based hydrogel sensors including carbon nanotube based, graphene oxide based, MXene based, polymer nanofiller based and other nanofiller based sensors. Representative cases are carefully selected and discussed regarding the fabrication, merits and demerits, respectively. Finally, perspectives and challenges are presented for the designs of future nanocomposite hydrogel-based strain and pressure sensors.

Nanocomposite hydrogel-based strain and pressure sensors: a review

Conductive hydrogels are widely used in various applications, such as artificial skin, flexible and implantable bioelectronics, and tissue engineering. However, it is still a challenge to formulate...

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Functional Conductive Hydrogels for Bioelectronics

Flexible sensors have shown great potential in remote health monitoring, body movements track, electronic skin, human-machine interfaces, and soft robotics. Hydrogels possess exceptional stretchability, flexibility and biocompatibility that render them appealing candidates for wearable flexible sensors. Among them, considerable efforts have been devoted to developing conductive hydrogels to achieve multifunctional wearable sensing through using functional groups/additives/nanofillers to modify the hydrogel network in recent years. This review summarizes recent advances of applications of hydrogels in flexible wearable sensors, such as sweat sampling and flexible electrodes, strain/pressure sensors and touch panels, focuses on the multifunctional conductive hydrogels-based flexible wearable sensors with self-healing, self-adhesion, or anti-freezing capabilities. A brief introduction to representative synthesis methods and strategies of conductive hydrogels is also presented. In the end, we also provide a personal perspective on the future development, and address the remaining challenges in the commercialization of conductive hydrogels-based multifunctional flexible wearable sensors.

Multifunctional conductive hydrogel-based flexible wearable sensors

Recently, flexible wearable electronic devices have attracted immense interest as an alternative for conventional rigid metallic conductors in personal healthcare monitoring, human motion detection, and sensory skins, owing to their intrinsic characteristics. However, the practical applications of most wearable sensors are generally limited by their poor stretchability and sensitivity, unsatisfactory strength, lower conductivity, and single sensory function. Here a hydrogen bond cross-linked network based on carboxylic styrene butadiene rubber (XSBR) and hydrophilic sericin (SS) non-covalently modified carbon nanotubes (CNTs) is rationally designed and then fabricated into multi-functional sensors. The resultant versatile sensors are able to detect both weak and large deformations, which owns a low detection limit of 1% strain, high stretchability up to 217%, superior strength of 12.58 MPa, high sensitivity with a gauge factor up to 25.98, high conductivity of 0.071 S m-1 , and lower percolation threshold of 0.504 wt%. Moreover, the prepared sensors also possess an impressively thermal response (0.01636 °C-1 ) and realize the application in the measurement of human body temperature. The multifunctional and scalable XSBR/SSCNT sensor with the integrated tracking capabilities of real-time and in situ physiological signals, providing a promising route to develop wearable artificial intelligence in human health and sporting applications.

A High-Performance, Sensitive, Wearable Multifunctional Sensor Based on Rubber/CNT for Human Motion and Skin Temperature Detection

Conductive self-healing hydrogels (CSHs) that match the mechanical properties of biological tissues are highly desired for emerging wearable electronics. However, it is still a fundamental challenge to balance the trade-offs among the mechanical, electronic, and self-healing properties in CSHs. In this study, we presented supramolecular double-network (DN) CSHs by pre-infiltrating conductive polyaniline (PANI) precursor into the self-healable hydrophobic association poly(acrylic acid) (HAPAA) hydrogel matrix. The dynamic interfacial interactions between the HAPAA and PANI networks efficiently enhanced the mechanical performances of the HAPAA/PANI (PAAN) hydrogel and could compensate for the negative effect of the enhanced mechanical strength on self-healing. In addition, the interconnected PANI network endowed the PAAN hydrogel with high conductivity and excellent sensory performances. As such, the mechanical and electronic properties of the PAAN hydrogel were simultaneously enhanced significantly without compromising the self-healing performance of the HAPAA matrix, achieving balanced mechanical, electronic, and self-healing properties in the PAAN hydrogel. Lastly, proof-of-concept applications like human physiological monitoring electronics, flexible touch screens, and artificial electronic skin are successfully demonstrated using the PAAN hydrogel with the capability of restoring their electronic performances after the healing process. It is anticipated that such hydrogel network design can be extended into next-generation hydrogel electronics for human–machine-interfaces and soft robotics.

Balancing the mechanical, electronic, and self-healing properties in conductive self-healing hydrogel for wearable sensor applications

The emerging applications of hydrogels in flexible electronics require hydrogels to possess excellent anti-fatigue fracture and self-healing properties; this remains an important unmet scientific challenge. Herein, inspired by human tissues, an effective and simple strategy is proposed to prepare a multifunctional hydrogel that shows ultra-stretchable (>2900%), anti-fatigue-fracture, and self-healable properties. Moreover, the hydrogel exhibits high sensitivity in a wide strain window when used as a strain sensor. More importantly, benefiting from the self-healing and anti-fatigue-fracture properties, the sensing properties of the hydrogel are fully restored after a cutting-and-healing process and it keeps working for a very long time (>20 000 cycles) even after being severely damaged. This hydrogel shows great potential for future artificial intelligence and human–machine interface applications.

Human-tissue-inspired anti-fatigue-fracture hydrogel for a sensitive wide-range human–machine interface

Water-rich conductive hydrogels with excellent stretchability are promising in strain sensors due to their potential application in flexible electronics. However, the features of being water-rich also limit their working environment. Hydrogels must be frozen at subzero temperatures and dried out under ambient conditions, leading to a loss of mechanical and electric properties. Herein, we prepare HAGx hydrogels (a polyacrylic acid (HAPAA) hydrogel in a binary water–glycerol solution, where x is the mass ratio of water to glycerol), in which the water is replaced with water–glycerol mixed solutions. The as-prepared HAGx hydrogels show great anti-freezing properties at a range of −70 to 25 °C, as well as excellent moisture stability (the weight retention rate was as high as 93% after 14 days). With the increase of glycerol, HAGx hydrogels demonstrate a superior stretchable and self-healing ability, which could even be stretched to more than 6000% without breaking, and had a 100% self-healing efficiency. The HAGx hydrogels had good self-healing ability at subzero temperatures. In addition, HAGx hydrogels also had eye-catching adhesive properties and transparency, which is helpful when used as strain sensors.

Shuya Yin

Papers

Balancing the mechanical, electronic, and self-healing properties in conductive self-healing hydrogel for wearable sensor applications

Human-tissue-inspired anti-fatigue-fracture hydrogel for a sensitive wide-range human–machine interface

Ultra-Stretchable and Self-Healing Anti-Freezing Strain Sensors Based on Hydrophobic Associated Polyacrylic Acid Hydrogels.