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.

Hydrogel Adhesion: A Supramolecular Synergy of Chemistry, Topology, and Mechanics

Cellulose Nanofibrils Enhanced, Strong, Stretchable, Freezing‐Tolerant Ionic Conductive Organohydrogel for Multi‐Functional Sensors

Hydrogel soft robotics

As many devices for human utility aim for fast and convenient communication with users, superb electronic devices are demonstrated to serve as hardware for human-machine interfaces in wearable forms. Wearable devices for daily healthcare and self-diagnosis offer more human-like properties unconstrained by deformation. In this sense, stretchable ionics based on flexible and stretchable hydrogels are on the rise as another means to develop wearable devices for bioapplications for two main reasons: i) ionic currents and choosing the same signal carriers for biological areas, and ii) the adoption of hydrogel ionic conductors, which are intrinsically stretchable materials with biocompatibility. Here, the current status of stretchable ionics and future applications are introduced, whose positive effects can be magnified by stretchable ionics.

Stretchable Ionics - A Promising Candidate for Upcoming Wearable Devices.

The emergence of stretchable electronics and its potential integration with textiles have highlighted a challenge: Textiles are wearable and washable, but electronic devices are not. Many stretchable conductors have been developed to enable wearable active textiles, but little has been done to make them washable. Here we demonstrate a new class of stretchable conductors that can endure wearing and washing conditions commonly associated with textiles. Such a conductor consists of a hydrogel, a dissolved hygroscopic salt, and a butyl rubber coating. The hygroscopic salt enables ionic conduction and matches the relative humidity of the hydrogel to the average ambient relative humidity. The butyl rubber coating prevents the loss and gain of water due to the daily fluctuation of ambient relative humidity. We develop the chemistry of dip-coating the butyl rubber onto the hydrogel, using silanes to achieve both the cross-link of the butyl rubber and the adhesion between the butyl rubber and the hydrogel. We test...

/pdf/wearable-and-washable-conductors-for-active-textiles-4s788sth9o.pdf

Wearable and Washable Conductors for Active Textiles

The interface between ground rubber particles (GRPs) and virgin rubber is the focus of this investigation that aims to mitigate the detriments caused by recycled GRPs blended in virgin rubber. By studying laminates of cured and uncured rubber strips as models for the interface, modulus contrast across the interface has been identified as another cause for the poor mechanical properties of vulcanizates containing GRPs, in additional to poor interfacial bonding. A surface-devulcanization method was established to improve molecular contact between the GRPs and virgin rubber and consequently raised the adhesion energy to the level of cohesion energy. The interfacial modulus contrast that causes stress concentration at the interface was likely a result of diffusion of curatives from the virgin rubber to the GRPs. The modulus contrast was erased by diffusion of piperidine from the GRPs into the virgin rubber. Piperidine acted as a vulcanization accelerator, making sulfur cross-linking within the virgin rubber outcompete sulfur diffusion into the GRPs. Mending the interface improved the tensile strength of vulcanizates containing GRPs to a level close to that of the virgin rubber vulcanizate but did not improve the extensibility.

Rubber Recycling: Mending the Interface between Ground Rubber Particles and Virgin Rubber

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Wearable and Washable Conductors for Active Textiles

Rubber Recycling: Mending the Interface between Ground Rubber Particles and Virgin Rubber