Liquid Metal Nanoparticles Physically Hybridized with Cellulose Nanocrystals Initiate and Toughen Hydrogels with Piezoionic Properties.

Liquid metal (LM) particles can serve as initiators, functional fillers, and cross-linkers for hydrogels. Herein, we show that cellulose nanocrystals (CNCs) stabilize LM particles in aqueous solutions, such as those used to produce hydrogels. The CNC-coated LM particles initiate free-radical polymerization to form poly(acrylic acid) (PAA) hydrogel with exceptional properties─stretchability ∼2000%, excellent toughness ∼1.8 MJ/m3, mechanical resilience, and efficient self-healing─relative to cross-linked PAA networks polymerized using conventional molecular initiators. FTIR spectroscopy, rheology, and mechanical measurements suggest that physical bonds between PAA and both Ga3+ and LM-CNC particles contribute to the excellent mechanical properties. The gels are used to sense a wide range of strains, such as those associated with human motion, via changes in resistance through the gel. The sensitivity at low strains enables monitoring subtle physiological signals, such as pulse. Without significantly compromising the toughness, soaking the gels in salt solution brings about high ionic conductivity (3.8 S/m), enabling them to detect touch via piezoionic principles; the anions in the gel have higher mobility than cations, resulting in significant charge separation (current ∼30 µA, ∼10 µA/cm2) through the gel in response to touch. These attractive properties are promising for wearable sensors, energy harvesters, and self-powered ionic touch panels.

A review on the features, performance and potential applications of hydrogel-based wearable strain/pressure sensors.

Over the past few years, development of wearable devices has gained increasing momentum. Notably, the demand for stretchable strain sensors has significantly increased due to many potential and emerging applications such as human motion monitoring, prosthetics, robotic systems, and touch panels. Recently, hydrogels have been developed to overcome the drawbacks of the elastomer-based wearable strain sensors, caused by insufficient biocompatibility, brittle mechanical properties, complicated fabrication process, as the hydrogels can provide a combination of various exciting properties such as intrinsic electrical conductivity, suitable mechanical properties, and biocompatibility. There are numerous research works reported in the literature which consider various aspects as preparation approaches, design strategies, properties control, and applications of hydrogel-based strain sensors. This article aims to present a review on this exciting topic with a new insight on the hydrogel-based wearable strain sensors in terms of their features, strain sensory performance, and prospective applications. In this respect, we first briefly review recent advances related to designing the materials and the methods for promoting hydrogels' intrinsic features. Then, strain (both tensile and pressure) sensing performance of prepared hydrogels is critically studied, and alternative approaches for their high-performance sensing are proposed. Subsequently, this review provides several promising applications of hydrogel-based strain sensors, including bioapplications and human-machine interface devices. Finally, challenges and future outlooks of conductive and stretchable hydrogels employed in the wearable strain sensors are discussed.