Soft electronics are intensively studied as the integration of electronics with dynamic nonplanar surfaces has become necessary. Here, a discussion of the strategies in materials innovation and structural design to build soft electronic devices and systems is provided. For each strategy, the presentation focuses on the fundamental materials science and mechanics, and example device applications are highlighted where possible. Finally, perspectives on the key challenges and future directions of this field are presented.

Materials and Structures toward Soft Electronics.

Nowadays, great effort has been devoted to establishing wearable electronics with excellent stretchability, high sensitivity, good mechanical strength, and multifunctional characteristics. Herein, a soft conductive hydrogel is rationally designed by proportionally mixing silk fibroin, polyacrylamide, graphene oxide, and poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate). The resultant hydrogel has considerable stretchability and compressibility, which enables it to be assembled into a strain/pressure sensor with a wide sensing range (strain, 2%-600%; pressure, 0.5-119.4 kPa) and reliable stability. Then, the corresponding sensor is capable of monitoring a series of physical signals of the human body (e.g., joint movement, facial gesture, pulse, breathing, etc.). In particular, the hydrogel-based sensor is biocompatible, with no anaphylactic reaction on human skin. More interestingly, this conductive hydrogel exhibits a positive response when it works in a triboelectric nanogenerator; consequently, it lights up 20 commericial green light-emitting diodes. Thus, this silk fibroin-based hydrogel is a kind of multifunctional material toward wearable electronics with versatile applications in health and exercise monitors, soft robots, and power sources.

Stretchable, Biocompatible, and Multifunctional Silk Fibroin-Based Hydrogels toward Wearable Strain/Pressure Sensors and Triboelectric Nanogenerators.

Conductive hydrogels have generated great interest in biomedical and electrical fields. However, conventional conductive hydrogels usually lack self-healing properties, which might be unfavorable for their application. Conductive self-healing hydrogels with excellent performance for applications in the biomedical and electrical fields are growing in number. In this review paper, the progress related to conductive self-healing hydrogels is summarized. The self-healing mechanism is classified to demonstrate the design and synthesis of conductive self-healing hydrogels and their applications in tissue engineering, wound healing, electronic skin, sensors and self-repaired circuits are presented and discussed. The future development of conductive self-healing hydrogels and problems that need to be solved are also described.

Self-healing conductive hydrogels: preparation, properties and applications

In this review, we focus on the very recent developments on the use of the stimuli responsive properties of polymer hydrogels for targeted drug delivery, tissue engineering, and biosensing utilizing their different optoelectronic properties. Besides, the stimuli-responsive hydrogels, the conducting polymer hydrogels are discussed, with specific attention to the energy generation and storage behavior of the xerogel derived from the hydrogel. The electronic and ionic conducting gels have been discussed that have applications in various electronic devices, e.g., organic field effect transistors, soft robotics, ionic skins, and sensors. The properties of polymer hybrid gels containing carbon nanomaterials have been exemplified here giving attention to applications in supercapacitors, dye sensitized solar cells, photocurrent switching, etc. Recent trends in the properties and applications of some natural polymer gels to produce thermal and acoustic insulating materials, drug delivery vehicles, self-healing material, tissue engineering, etc., are discussed. Besides the polymer gels, peptide gels of different dipeptides, tripeptides, oligopeptides, polypeptides, cyclic peptides, etc., are discussed, giving attention mainly to biosensing, bioimaging, and drug delivery applications. The properties of peptide-based hybrid hydrogels with polymers, nanoparticles, nucleotides, fullerene, etc., are discussed, giving specific attention to drug delivery, cell culture, bio-sensing, and bioimaging properties. Thus, the present review delineates, in short, the preparation, properties, and applications of different polymer and peptide hydrogels prepared in the past few years.

A review on recent advances in polymer and peptide hydrogels

Advances in injectable self-healing biomedical hydrogels.

Conductive hydrogels are a class of composite materials that usually comprise hydrated polymers and conductive materials. Practical application requires the conductive hydrogels to have various properties such as high conductivity, toughness, self-healing, facile processing ability, and so on. Although challenging to have all the above-mentioned properties, a composite material composed of polymer hydrogel with embedded Au nanoparticles (i.e., P(NaSS)/P(VBIm-Cl)/PVA@Au) was found to show the comprehensive properties above in this paper. For example, P(NaSS)/P(VBIm-Cl)/PVA@Au exhibits mechanical and electrical self-healing properties at ambient conditions. In addition, P(NaSS)/P(VBIm-Cl)/PVA@Au is tough and thermoplastic, potentially making it useful for a variety of applications.

An Electrically and Mechanically Autonomic Self-healing Hybrid Hydrogel with Tough and Thermoplastic Properties

In nature, living organisms evolve unique functional components with mechanically adaptive compatibility to cater dynamic change of interface friction/lubrication. This mechanism can be used for developing intelligent artificial lubrication-regulation systems. Inspired by the muscle hardening-triggered lubrication of longsnout catfish, here we report a modulus adaptive lubricating hydrogel prototype consisting of top mucus-like hydrophilic lubricating layer and muscle-like bottom hydrogel that can stiffen via thermal-triggered phase separation. It exhibits instant switch from soft/high frictional state (~0.3 MPa, μ~0.37) to stiff/lubricating state (~120 MPa, μ~0.027) in water upon heating up. Such switchable lubrication is effective for wide range of normal loads and attributed to the modulus-dominated adaptive contact mechanism. As a proof-of-concept, switchable lubricating hydrogel bullets and patches are engineered for realizing controllable interface movements. These important results demonstrate potential applications in the fields of intelligent motion devices and soft robots. 

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Modulus adaptive lubricating prototype inspired by instant muscle hardening mechanism of catfish skin

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Controllably coating the surfaces of substrates/medical devices with hydrogels exhibits great application potential, but lacks universal techniques. Herein, a new method, namely ultraviolet‐triggered surface catalytically initiated radical polymerization (UV‐SCIRP) from a sticky initiation layer (SIL) (SIL@UV‐SCIRP), is proposed for growing hydrogel coatings. The method involves three key steps: 1) depositing a sticky polydopamine/Fe3+ coating on the surface of the substrates‐SIL, 2) reducing Fe3+ ions to Fe2+ ions as active catalysts by UV illumination with the assistance of citric acid, and 3) conducting SCIRP in a monomer solution at room temperature for growing hydrogel coatings. In this manner, practically any substrate's surface (natural or artificial materials) can be modified by hydrogel coatings with controllable thickness and diverse compositions. The hydrogel coatings exhibit good interface bonding with the substrates and enable easy changes in their wettability and lubrication performances. Importantly, this novel method facilitates the smooth growth of uniform hydrogel lubrication coatings on the surface of a range of medical devices with complex geometries. Finally, as a proof‐of‐concept, the slippery balls coated with hydrogel exhibited smooth movement within the catheter and esophagus. Hence, this method can prove to be a pioneering universal modification tool, especially in surface/interface science and engineering.

A Universal Strategy for Growing a Tenacious Hydrogel Coating from a Sticky Initiation Layer

Natural articular cartilages show extraordinary tribological performance based on their penetrated surface lubricated biomacromolecules and good mechanical tolerance. Hydrogels are considered to be potential alternatives to cartilages due to their low surface friction and good biocompatibility, although the poor mechanical properties limited their applications. Inspired by the excellent mechanical properties and the remarkable surface lubrication mechanism of natural articular cartilages, one kind of cartilage-like composite material with a lubrication phase (Composite-LP) was developed by chemically grafting a thick hydrophilic polyelectrolyte brush layer onto the subsurface of a three-dimensional manufactured elastomer scaffold-hydrogel composite architecture. The Composite-LP exhibited good load-bearing capacities because of the nondissipation strategy and the stress dispersion mechanism resulting from the elastomer scaffold enhancement. In the presence of the top lubrication layer, the Composite-LP showed superior friction reduction functionality and wear resistance under a dynamic shearing process. This design concept of coupling the non-dissipative mechanism and interface lubrication provides a new avenue for developing cartilage-like hydrogels and soft robots.

Yunlei Zhang

Papers

An Electrically and Mechanically Autonomic Self-healing Hybrid Hydrogel with Tough and Thermoplastic Properties

Modulus adaptive lubricating prototype inspired by instant muscle hardening mechanism of catfish skin

Modulus adaptive lubricating prototype inspired by instant muscle hardening mechanism of catfish skin

A Universal Strategy for Growing a Tenacious Hydrogel Coating from a Sticky Initiation Layer

Bioinspired Design of a Cartilage-like Lubricated Composite with Mechanical Robustness.