Closed-Loop Recyclable and Totally Renewable Liquid Crystal Networks with Room-Temperature Programmability and Reconfigurable Functionalities.

Dynamic covalent liquid crystal networks (DCv-LCNs) with straightforward (re)programmability, reprocessability, and recyclability facilitates the manufacture of sophisticated LCN actuators and intelligent robots. However, the DCv-LCNs are still limited to heat-assisted programming and polymer-to-polymer reprocessing/recycling, which inevitably lead to deterioration of the LCN structures and the actuation performances after repeated programming/processing treatments, owing to the thermal degradation of the polymer network and/or external agent interference. Here, a totally renewable azobenzene-based DCv-LCN with room-temperature programmability and polymer-to-monomers chemical recyclability is reported, which was synthesized by crosslinking the azobenzene-containing dibenzaldehyde monomer and the triamine monomer via the dynamic and dissociable imine bonds.

Ultrastable, Superrobust, and Recyclable Supramolecular Polymer Networks.

Supramolecular polymer networks (SPNs), crosslinked by noncovalent bonds, have emerged as reorganizable and recyclable polymeric materials with unique functionality. However, poor stability is an imperative challenge faced by SPNs, because SPNs are susceptible to heat, water, and/or solvents due to the dynamic and reversible nature of noncovalent bonds. Herein, the design of a noncovalent cooperative network (NCoN) to simultaneously stabilize and reinforce SPNs is reported, resulting in an ultrastable, superrobust, and recyclable SPN.

One-Pot Preparation of Skin-Inspired Multifunctional Hybrid Hydrogel with Robust Wound Healing Capacity.

Bioinspired hydrogels have demonstrated multiple superiorities over traditional wound dressings for wound healing applications. However, the fabrication of bioinspired hydrogel-based wound dressings with desired functionalities always requires multiple successive steps, time-consuming processes, and/or sophisticated protocols, plaguing their clinical applications. Here, a facile one-pot strategy is developed to prepare a skin-inspired multifunctional hydrogel within 30 min by incorporating elastin (an essential functional component of the dermal extracellular matrix), tannic acid, and chitosan into the covalently cross-linked poly(acrylamide) network through noncovalent interactions.

Solvent-Free and Skin-Like Supramolecular Ion-Conductive Elastomers with Versatile Processability for Multifunctional Ionic Tattoos and On-Skin Bioelectronics.

The development of stable and biocompatible soft ionic conductors, alternatives to hydrogels and ionogels, will open up new avenues for the construction of stretchable electronics. Here, a brand-new design, encapsulating a naturally occurring ionizable compound by a biocompatible polymer via high-density hydrogen bonds, resulting in a solvent-free supramolecular ion-conductive elastomer (SF-supra-ICE) that eliminates the dehydration problem of hydrogels and possesses excellent biocompatibility, is reported. The SF-supra-ICE with high ionic conductivity (>3.

Collective photothermal bending of flexible organic crystals modified with MXene-polymer multilayers as optical waveguide arrays.

The performance of any engineering material is naturally limited by its structure, and while each material suffers from one or multiple shortcomings when considered for a particular application, these can be potentially circumvented by hybridization with other materials. By combining organic crystals with MXenes as thermal absorbers and charged polymers as adhesive counter-ionic components, we propose a simple access to flexible hybrid organic crystal materials that have the ability to mechanically respond to infrared light. The ensuing hybrid organic crystals are durable, respond fast, and can be cycled between straight and deformed state repeatedly without fatigue.

Bioinspired soft robots based on organic polymer-crystal hybrid materials with response to temperature and humidity.

The capability of stimulated response by mechanical deformation to induce motion or actuation is the foundation of lightweight organic, dynamic materials for designing light and soft robots. Various biomimetic soft robots are constructed to demonstrate the vast versatility of responses and flexibility in shape-shifting. We now report that the integration of organic molecular crystals and polymers brings about synergistic improvement in the performance of both materials as a hybrid materials class, with the polymers adding hygroresponsive and thermally responsive functionalities to the crystals.

Electrically conductive hybrid organic crystals as flexible optical waveguides.

Hybrid materials capitalize on the properties of individual materials to attain a specific combination of performance assets that is not available with the individual components alone. We describe a straightforward approach to preparation of sandwich-type hybrid dynamic materials that combine metals as electrically conductive components and polymers as bending, momentum-inducing components with flexible organic crystals as mechanically compliant and optically transducive medium. The resulting hybrid materials are conductive to both electricity and light, while they also respond to changes in temperature by deformation.

Strong and Tough Supramolecular Covalent Adaptable Networks with Room-Temperature Closed-Loop Recyclability.

Development of closed-loop chemically recyclable plastics (CCRPs) that can be widely used in daily life can be a fundamental solution to the global plastic waste crisis. Hence, it is of great significance to develop easy-to-recycle CCRPs that possess superior or comparable material properties to the commodity plastics. Here, a novel dual crosslinked CCRP, namely, supramolecular covalent adaptable networks (supra-CANs), is reported, which not only displays mechanical properties higher than the strong and tough commodity polycarbonate, but also exhibits excellent solvent resistance as thermosets.

Stretchable Ionic Conductors for Soft Electronics.

With the rapid development of soft electronics in the era of Internet of Everything (IoE), electrical conductors with stretchability, the indispensable components of soft electronics, have gained new opportunities and also faced increasing challenges. According to the principles of electrical conductivity, stretchable electrical conductors can be divided into electronic conductors and ionic conductors. Different from the stretchable electronic conductors derived from stretchable polymeric matrices integrated with electronically conductive fillers, stretchable ionic conductors are constructed by embedding mobile ions into the crosslinked polymer networks.

Remote and precise control over morphology and motion of organic crystals by using magnetic field.

Elastic organic crystals are the materials foundation of future lightweight flexible electronic, optical and sensing devices, yet precise control over their deformation has not been accomplished. Here, we report a general non-destructive approach to remote bending of organic crystals. Flexible organic crystals are coupled to magnetic nanoparticles to prepare hybrid actuating elements whose shape can be arbitrarily and precisely controlled simply by using magnetic field.

Organic Single-Crystal Actuators and Waveguides that Operate at Low Temperatures.

Applications in extreme conditions, such as those encountered in space exploration, require lightweight materials that can retain their elasticity in extremely cold environments. However, cryogenic treatment of most soft polymeric and elastomeric materials results in complete loss of their ability for elastic flow, whereby such materials that are normally ductile become stiff, brittle, and prone to cracking. Here, a facile method for preparation of hybrid organic crystalline materials that are not only cryogenically robust but are also capable of large, recoverable, and reversible deformation at low temperatures is reported.

Hybrid Elastic Organic Crystals that Respond to Aerial Humidity.

Reshaping of elongated organic crystals that can be used as semiconductors, waveguides or soft robotic grippers by application of force or light is now a commonplace, however mechanical response of organic crystals to changes in humidity has not been accomplished yet. Here, we report a universal approach to instigating a humidity response into elastically bendable organic crystals that elicits controllable deformation with linear response to aerial humidity while retaining their physical integrity entirely intact. Hygroresponsive bilayer elements are designed by mechanically coupling a humidity-responsive polymer with elastic molecular crystals that have been mechanically reinforced by a polymer coating.

Thermal Dynamic Self-Healing Supramolecular Dopant Towards Efficient and Stable Flexible Perovskite Solar Cells.

Flexible perovskite solar cells (FPSCs) have attracted great attention due to their advantageous traits such as low cost, portability, light-weight, etc. However, mechanical stability is still the weak point in their practical application. Herein, we prepared efficient FPSCs with remarkable mechanical stability by a dynamic thermal self-healing effect, which can be realized by the usage of a supramolecular adhesive.

Healable and Recyclable Elastomers with Record-High Mechanical Robustness, Unprecedented Crack Tolerance, and Superhigh Elastic Restorability.

Spider silk is one of the most robust natural materials, which has extremely high strength in combination with great toughness and good elasticity. Inspired by spider silk but beyond it, a healable and recyclable supramolecular elastomer, possessing superhigh true stress at break (1.21 GPa) and ultrahigh toughness (390.

Polymer-Coated Organic Crystals with Solvent-Resistant Capacity and Optical Waveguiding Function.

Recently, luminescent organic crystals have been widely studied as new optoelectronic materials. However, corrosion and dissolution of organic crystals by solvents have always been a great challenge for the application of organic crystals in various fields. In this work, we propose a general method of fabricating a solvent-resistant coating to prevent organic crystals from being corroded or dissolved by organic solvents.

Mechanically Robust, Elastic, and Healable Ionogels for Highly Sensitive Ultra-Durable Ionic Skins.

The fabrication of highly durable skin-mimicking sensors remains challenging because of the unavoidable fatigue and physical damage that sensors are subjected to in practical applications. In this study, ultra-durable ionic skins (I-skins) with excellent healability and high sensitivity are fabricated by impregnating ionic liquids (ILs) into a mechanically robust poly(urea-urethane) (PU) network. The PU network is composed of crystallized poly(ε-caprolactone) and flexible poly(ethylene glycol) that are dynamically cross-linked with hindered urea bonds and hydrogen bonds.

Remalleable, Healable, and Highly Sustainable Supramolecular Polymeric Materials Combining Superhigh Strength and Ultrahigh Toughness.

To build a sustainable society, it is of significant importance but highly challenging to develop remalleable, healable, and biodegradable polymeric materials with integrated high strength and high toughness. Here, we report a superstrong and ultratough sustainable supramolecular polymeric material with a toughness of . 282.

Substrate-Independent, Reversible, and Easy-Release Ionogel Adhesives with High Bonding Strength.

It is highly desirable to develop reversible and easy-release adhesives with high bonding strength for a broad range of substrates, while the adhesion of low-surface-energy materials (e.g., polytetrafluoretyhylene, PTFE) is challenging.

Fast Modulation of Surface Amphiphobicity/Amphiphilicity via Bidirectional Substitution between Perfluorinated Surfactants and Polyanions throughout Pre-Assembled Polyelectrolyte Multilayers.

In the present work, we demonstrate a bidirectional substitution between perfluorooctanoate (PFO) surfactants and polyanions throughout the pre-assembled polyelectrolyte multilayers (PEMs) for a rapid modulation of surface wettability between amphiphobicity and amphiphilicity. Upon incubation of the PEMs made of alternating deposition of poly(diallyldimethylammonium) (PDDA) and poly(styrenesulfonate) (PSS) in PFO solutions at concentrations above or around its critical micelle concentration, the majority (ca. >75%) of PSS molecules throughout the PDDA/PSS PEMs can be substituted by PFO anions within 10 s, generating PFO-substituted PDDA/PSS (PFO-PDDA/PSS) films.

Healable, Highly Conductive, Flexible, and Nonflammable Supramolecular Ionogel Electrolytes for Lithium-Ion Batteries.

High-performance solid-state electrolytes with healability to repair mechanical damages are important for the fabrication of Li-ion batteries (LIBs) with enhanced safety and prolonged service life. In this study, we present the fabrication of healable, highly conductive, flexible, and nonflammable ionogel electrolytes for use in LIBs by loading ionic liquids and Li salts within a hydrogen-bonded supramolecular poly(ionic liquid) copolymer network. The ionogel electrolytes exhibit ionic conductivities as high as 10 S/cm, which is comparable to the conventional liquid electrolytes.

Effect of the Self-Assembled Structures of Hydrated Polyzwitterionic and Polyanionic Brushes on Their Self-Cleaning Capabilities.

The capability of polyelectrolyte brushes to spontaneously clean oil fouling via water is determined by factors including water wettability and the self-assembled structures of hydrated polyelectrolytes. Although the charged groups of polyelectrolytes provide the original source of water wettability, the self-assembled structures play a significant role in the self-cleaning performances. Here, we employ coarse-grained molecular dynamics simulations to study the general self-cleaning characteristics of two types of surface-grafted polyelectrolyte brushes (i.

Author Correction: Ultra-fast Hygrometer based on U-shaped Optical Microfiber with Nanoporous Polyelectrolyte Coating.

A correction to this article has been published and is linked from the HTML and PDF versions of this paper. The error has been fixed in the paper.

Counteranion-Mediated Intrinsic Healing of Poly(ionic liquid) Copolymers.

Fabrication of self-healing/healable materials using reversible interactions that are governed by their inherent chemical features is highly desirable because it avoids the introduction of extra groups that may present negative effects on their functions. The present study exploits the inherently featured electrostatic interactions of the ion pairs in polymeric ionic liquids (PILs) as the driving force to fabricate healable PIL copolymers. The healable PIL copolymers are fabricated through the copolymerization of the IL monomers with ethyl acrylate followed by the replacement of Br counteranions with bulkier ones such as bis(trifluoromethanesulfonyl)imide (TFSI).

Ultra-fast Hygrometer based on U-shaped Optical Microfiber with Nanoporous Polyelectrolyte Coating.

Real-time measurement of the relative humidity of air has applications ranging from process control to safety. By using a microfiber form-factor, we demonstrate a miniature and fast-response hygrometer with the shortest-ever response time (3 ms). The sensor head consists of an optical microfiber of 10 µm diameter and 2 mm length configured to form a compact U-shaped probe, and functionalized with a polyelectrolyte multilayer coating of 1.