Toughening Self-Healing Elastomers with Chain Mobility.

Enhancing fracture toughness and self-healing within soft elastomers is crucial to prolonging the operational lifetimes of soft devices. Herein, it is revealed that tuning the polymer chain mobilities of carboxylated-functionalized polyurethane through incorporating plasticizers or thermal treatment can enhance these properties. Self-healing is promoted as polymer chains gain greater mobility toward the broken interface to reassociate their bonds. Raising the temperature from 80 to 120 °C, the recovered work of fracture is increased from 2.86 to 123.7 MJ m-3. Improved fracture toughness is realized through two effects. First, strong carboxyl hydrogen bonds dissipate large energies when broken. Second, chain mobilities enable the redistribution of localized stress concentrations to allow crack blunting, enlarging the size of dissipation zones. At optimal conditions of plasticizers (3 wt.%) or temperature (40 °C) to promote chain mobilities, fracture toughness improves from 16.3 to 19.9 and 25.6 kJ m-2, respectively. Insights of fracture properties at healed soft interfaces are revealed through double cantilever beam tests. These measurements indicate that fracture mechanics play a critical role in delaying complete failure at partial self-healing. By imparting optimal polymer chain mobilities within tough and self-healing elastomers, effective prevention against damage and better recovery are realized.

Dual-Responsive MXene-Functionalized Wool Yarn Artificial Muscles.

Fiber-based artificial muscles are promising for smart textiles capable of sensing, interacting, and adapting to environmental stimuli. However, the application of current artificial muscle-based textiles in wearable and engineering fields has largely remained a constraint due to the limited deformation, restrictive stimulation, and uncomfortable. Here, dual-responsive yarn muscles with high contractile actuation force are fabricated by incorporating a very small fraction (<1 wt.%) of Ti3C2Tx MXene/cellulose nanofibers (CNF) composites into self-plied and twisted wool yarns. They can lift and lower a load exceeding 3400 times their own weight when stimulated by moisture and photothermal. Furthermore, the yarn muscles are coiled homochirally or heterochirally to produce spring-like muscles, which generated over 550% elongation or 83% contraction under the photothermal stimulation. The actuation mechanism, involving photothermal/moisture-mechanical energy conversion, is clarified by a combination of experiments and finite element simulations. Specifically, MXene/CNF composites serve as both photothermal and hygroscopic agents to accelerate water evaporation under near-infrared (NIR) light and moisture absorption from ambient air. Due to their low-cost facile fabrication, large scalable dimensions, and robust strength coupled with dual responsiveness, these soft actuators are attractive for intelligent textiles and devices such as self-adaptive textiles, soft robotics, and wearable information encryption.

Towards high performance and durable soft tactile actuators.

Soft actuators are gaining significant attention due to their ability to provide realistic tactile sensations in various applications. However, their soft nature makes them vulnerable to damage from external factors, limiting actuation stability and device lifespan. The susceptibility to damage becomes higher with these actuators often in direct contact with their surroundings to generate tactile feedback. Upon onset of damage, the stability or repeatability of the device will be undermined. Eventually, when complete failure occurs, these actuators are disposed of, accumulating waste and driving the consumption of natural resources. This emphasizes the need to enhance the durability of soft tactile actuators for continued operation. This review presents the principles of tactile feedback of actuators, followed by a discussion of the mechanisms, advancements, and challenges faced by soft tactile actuators to realize high actuation performance, categorized by their driving stimuli. Diverse approaches to achieve durability are evaluated, including self-healing, damage resistance, self-cleaning, and temperature stability for soft actuators. In these sections, current challenges and potential material designs are identified, paving the way for developing durable soft tactile actuators.

Encoding of multi-modal emotional information via personalized skin-integrated wireless facial interface.

Human affects such as emotions, moods, feelings are increasingly being considered as key parameter to enhance the interaction of human with diverse machines and systems. However, their intrinsically abstract and ambiguous nature make it challenging to accurately extract and exploit the emotional information. Here, we develop a multi-modal human emotion recognition system which can efficiently utilize comprehensive emotional information by combining verbal and non-verbal expression data. This system is composed of personalized skin-integrated facial interface (PSiFI) system that is self-powered, facile, stretchable, transparent, featuring a first bidirectional triboelectric strain and vibration sensor enabling us to sense and combine the verbal and non-verbal expression data for the first time. It is fully integrated with a data processing circuit for wireless data transfer allowing real-time emotion recognition to be performed. With the help of machine learning, various human emotion recognition tasks are done accurately in real time even while wearing mask and demonstrated digital concierge application in VR environment.

Bioinspired structural hydrogels with highly ordered hierarchical orientations by flow-induced alignment of nanofibrils.

Natural structural materials often possess unique combinations of strength and toughness resulting from their complex hierarchical assembly across multiple length scales. However, engineering such well-ordered structures in synthetic materials via a universal and scalable manner still poses a grand challenge. Herein, a simple yet versatile approach is proposed to design hierarchically structured hydrogels by flow-induced alignment of nanofibrils, without high time/energy consumption or cumbersome postprocessing. Highly aligned fibrous configuration and structural densification are successfully achieved in anisotropic hydrogels under ambient conditions, resulting in desired mechanical properties and damage-tolerant architectures, for example, strength of 14 ± 1 MPa, toughness of 154 ± 13 MJ m-3, and fracture energy of 153 ± 8 kJ m-2. Moreover, a hydrogel mesoporous framework can deliver ultra-fast and unidirectional water transport (maximum speed at 65.75 mm s-1), highlighting its potential for water purification. This scalable fabrication explores a promising strategy for developing bioinspired structural hydrogels, facilitating their practical applications in biomedical and engineering fields.

Functionalized MXene Films with Substantially Improved Low-Voltage Actuation.

Ti3 C2 Tx MXene film is promising for low-voltage electrochemical actuators (ECAs) due to its excellent electrical conductivity, volumetric capacitance, and mechanical properties. However, its in-plane actuation is limited to little intralayer strain of MXene sheets under polarization. Here it is demonstrated that a simple tetrabutylammonium (TBA) functionalization of MXene improves the in-plane actuation strain by 337% and also enhances the mechanical property and stability in air and the electrolyte. Various in situ characterizations reveal that the improved actuation is ascribed to the co-insertion/desertion of TBA and Li ions into/from MXene interlayer galleries and inter-edge gaps that causes a large in-plane sliding of MXene sheets under negative/positive polarizations. The assembled bending actuator has a high strength and modulus and generates a peak-to-peak strain difference of 0.771% and a blocking force up to 51.5 times its own weight under 1 V. The designed soft robotic tweezer can grasp an object under 1 V and hold it firmly under 0 V. The novel sheet sliding mechanism resembling the filament sliding theory in skeletal muscles may inspire the design of high-performance actuators with other nanomaterials.

Triboelectric Nanogenerators Based on Fluid Medium: From Fundamental Mechanisms toward Multifunctional Applications.

Fluid-based triboelectric nanogenerators (FB-TENGs) are at the forefront of promising energy technologies, demonstrating the ability to generate electricity through the dynamic interaction between two dissimilar materials, wherein at least one is a fluidic medium (such as gas or liquid). By capitalizing on the dynamic and continuous properties of fluids and their interface interactions, FB-TENGs exhibit a larger effective contact area and a longer-lasting triboelectric effect in comparison to their solid-based counterparts, thereby affording longer-term energy harvesting and higher-precision self-powered sensors in harsh conditions. In this review, various fluid-based mechanical energy harvesters, including liquid-solid, gas-solid, liquid-liquid, and gas-liquid TENGs, have been systematically summarized. Their working mechanism, optimization strategies, respective advantages and applications, theoretical and simulation analysis, as well as the existing challenges, have also been comprehensively discussed, which provide prospective directions for device design and mechanism understanding of FB-TENGs.

The Role of 3D Printing Technologies in Soft Grippers.

Soft grippers are essential for precise and gentle handling of delicate, fragile, and easy-to-break objects, such as glassware, electronic components, food items, and biological samples, without causing any damage or deformation. This is especially important in industries such as healthcare, manufacturing, agriculture, food handling, and biomedical, where accuracy, safety, and preservation of the objects being handled are critical. This article reviews the use of 3D printing technologies in soft grippers, including those made of functional materials, nonfunctional materials, and those with sensors. 3D printing processes that can be used to fabricate each class of soft grippers are discussed. Available 3D printing technologies that are often used in soft grippers are primarily extrusion-based printing (fused deposition modeling and direct ink writing), jet-based printing (polymer jet), and immersion printing (stereolithography and digital light processing). The materials selected for fabricating soft grippers include thermoplastic polymers, UV-curable polymers, polymer gels, soft conductive composites, and hydrogels. It is conclude that 3D printing technologies revolutionize the way soft grippers are being fabricated, expanding their application domains and reducing the difficulties in customization, fabrication, and production.

Printed sustainable elastomeric conductor for soft electronics.

The widespread adoption of renewable and sustainable elastomers in stretchable electronics has been impeded by challenges in their fabrication and lacklustre performance. Here, we realize a printed sustainable stretchable conductor with superior electrical performance by synthesizing sustainable and recyclable vegetable oil polyurethane (VegPU) elastomeric binder and developing a solution sintering method for their composites with Ag flakes. The binder impedes the propagation of cracks through its porous network, while the solution sintering reaction reduces the resistance increment upon stretching, resulting in high stretchability (350%), superior conductivity (12833 S cm-1), and low hysteresis (0.333) after 100% cyclic stretching. The sustainable conductor was used to print durable and stretchable impedance sensors for non-obstructive detection of fruit maturity in food sensing technology. The combination of sustainable materials and strategies for realizing high-performance stretchable conductors provides a roadmap for the development of sustainable stretchable electronics.

Size-Selective Ionic Crosslinking Provides Stretchable Mixed Ionic-Electronic Conductors.

Mechanically compliant conductors are of utmost importance for the emerging fields of soft electronics and robotics. However, the development of intrinsically deformable organic conductors remains a challenge due to the trade-off between mechanical performance and charge mobility. In this study, we report a solution to this issue based on size-selective ionic crosslinking. This rationally designed crosslinking mediated by length-regulated oligo(ethylene glycol) pendant groups and metal ions simultaneously improved the softness and toughness and ensured excellent mixed ionic-electronic conductivity in poly(3,4-ethylenedioxythiophene):polystyrene sulfonate composite materials. Moreover, the added ions remarkably promoted accumulation of charge carriers in response to temperature gradient, thus offering a viable approach to stretchable thermoelectric generators with enhanced stability against humidity.

Ferroelectric Modulation in Flexible Lead-Free Perovskite Schottky Direct-Current Nanogenerator for Capsule-Like Magnetic Suspension Sensor.

The tribovoltaic nanogenerator (TVNG), a promising semiconductor energy technology, displays outstanding advantages such as low matching impedance and continuous direct-current output. However, the lack of controllable and stable performance modulation strategies is still a major bottleneck that impedes further practical applications of TVNG. Herein, by leveraging the ferroelectricity-enhanced mechanism and the control of interfacial energy band bending, a lead-free perovskite-based (3,3-difluorocyclobutylammonium)2 CuCl4 ((DF-CBA)2 CuCl4 )/Al Schottky junction TVNG is constructed. The multiaxial ferroelectricity of (DF-CBA)2 CuCl4 enables an excellent surface charge modulating capacity, realizing a high work function regulation of ≈0.7 eV and over 15-fold current regulation (from 6 to 93 µA) via an electrical poling control. The controllable electrical poling leads to elevated work function difference between the Al electrode and (DF-CBA)2 CuCl4 compared to traditional semiconductors and halide perovskites, which creates a stronger built-in electric field at the Schottky interface to enhance the electrical output. This TVNG device exhibits outstanding flexibility and long-term stability (>20 000 cycles) that can endure extreme mechanical deformations, and can also be used in a capsule-like magnetic suspension device capable of detecting vibration and weights of different objects as well as harvesting energy from human motions and water waves.

Melanin and Polypyrrole-Coated Nanocellulose Hydrogel Networks for Environmental Sensing and Energy Storage.

Melanins are black-brown pigments of a specific class of poly indolequinones found in nature and in the human body. They are responsible for photoprotection, radical scavenging, and metal ion chelation. Recently, there has been significant interest in eumelanin as a functional material due to its macromolecular structure and the exploitation of the quinone-hydroquinone redox equilibrium. While eumelanin can be used in many promising applications, it is insoluble in most solvents, limiting its processing into homogeneous materials and coatings. A promising approach is to use a carrier system to stabilize eumelanin by incorporating cellulose nanofibrils (CNFs), a nanoscopic material that originates from plant biomass. In this work, a flexible network consisting of CNFs coupled with vapor-phase polymerized conductive polypyrrole (PPy) is utilized to form a functional eumelanin hydrogel composite (MelaGel) for environmental sensing and battery applications. Flexible sensors for detecting pH or metal ions made from MelaGel can detect both pH values in a range from 4 to 10 and metal ions like zinc(II), copper(II), and iron(III), paving the way for environmental and biomedical sensor applications. The reduced internal resistance in the MelaGel leads to improved charge storage ability compared to synthetic eumelanin composite electrodes. Other noteworthy advantages of the MelaGel are the amphiphilic nature of PPy and the additionally offered redox centers. Lastly, this material was tested in aqueous electrolyte zinc coin cells, where it was shown to have charge/discharge stability for over 1200 cycles, showcasing this MelaGel composite as a promising eumelanin-based composite hybrid sensor/energy storage material.

Recent Advances in Triboelectric Nanogenerators: From Technological Progress to Commercial Applications.

Serious climate changes and energy-related environmental problems are currently critical issues in the world. In order to reduce carbon emissions and save our environment, renewable energy harvesting technologies will serve as a key solution in the near future. Among them, triboelectric nanogenerators (TENGs), which is one of the most promising mechanical energy harvesters by means of contact electrification phenomenon, are explosively developing due to abundant wasting mechanical energy sources and a number of superior advantages in a wide availability and selection of materials, relatively simple device configurations, and low-cost processing. Significant experimental and theoretical efforts have been achieved toward understanding fundamental behaviors and a wide range of demonstrations since its report in 2012. As a result, considerable technological advancement has been exhibited and it advances the timeline of achievement in the proposed roadmap. Now, the technology has reached the stage of prototype development with verification of performance beyond the lab scale environment toward its commercialization. In this review, distinguished authors in the world worked together to summarize the state of the art in theory, materials, devices, systems, circuits, and applications in TENG fields. The great research achievements of researchers in this field around the world over the past decade are expected to play a major role in coming to fruition of unexpectedly accelerated technological advances over the next decade.

A supramolecular gel-elastomer system for soft iontronic adhesives.

Electroadhesion provides a promising route to augment robotic functionalities with continuous, astrictive, and reversible adhesion force. However, the lack of suitable conductive/dielectric materials and processing capabilities have impeded the integration of electroadhesive modules into soft robots requiring both mechanical compliance and robustness. We present herein an iontronic adhesive based on a dynamically crosslinked gel-elastomer system, including an ionic organohydrogel as adhesive electrodes and a resilient polyurethane with high electrostatic energy density as dielectric layers. Through supramolecular design and synthesis, the dual-material system exhibits cohesive heterolayer bonding and autonomous self-healing from damages. Iontronic soft grippers that seamlessly integrate actuation, adhesive prehension, and exteroceptive sensation are devised via additive manufacturing. The grippers can capture soft and deformable items, bear high payload under reduced voltage input, and rapidly release foreign objects in contrast to electroadhesives. Our materials and iontronic mechanisms pave the way for future advancement in adhesive-enhanced multifunctional soft devices.

Effective Surface Modification of 2D MXene toward Thermal Energy Conversion and Management.

Thermal energy management is a crucial aspect of many research developments, such as hybrid and soft electronics, aerospace, and electric vehicles. The selection of materials is of critical importance in these applications to manage thermal energy effectively. From this perspective, MXene, a new type of 2D material, has attracted considerable attention in thermal energy management, including thermal conduction and conversion, owing to its unique electrical and thermal properties. However, tailored surface modification of 2D MXenes is required to meet the application requirements or overcome specific limitations. Herein, a comprehensive review of surface modification of 2D MXenes for thermal energy management is discussed. First, this work discusses the current progress in the surface modification of 2D MXenes, including termination with functional groups, small-molecule organic compound functionalization, and polymer modification and composites. Subsequently, an in situ analysis of surface-modified 2D MXenes is presented. This is followed by an overview of the recent progress in the thermal energy management of 2D MXenes and their composites, such as Joule heating, heat dissipation, thermoelectric energy conversion, and photothermal conversion. Finally, some challenges facing the application of 2D MXenes are discussed, and an outlook on surface-modified 2D MXenes is provided.

Ultrafast, High-Strain, and Strong Uniaxial Hydrogel Actuators from Recyclable Nanofibril Networks.

Polymer hydrogels mimic biological tissues and are suitable for future lifelike machines. However, their actuation is isotropic, so they must be crosslinked or placed in a turgor membrane to achieve high actuation pressures, severely impeding their performance. Here, it is shown that organizing cellulose nanofibrils (CNFs) in anisotropic hydrogel sheets leads to mechanical in-plane reinforcement that generates a uniaxial, out-of-plane strain with performance far surpassing polymer hydrogels. These fibrillar hydrogel actuators expand uniaxially by 250 times with an initial rate of 100-130% s-1 , compared to <10 times and <1% s-1 in directional strain rate for isotropic hydrogels, respectively. The blocking pressure reaches 0.9 MPa, similar to turgor actuators, while the time to reach 90% of the maximum pressure is 1-2 min, compared to 10 min to hours for polymer hydrogel actuators. Uniaxial actuators that lift objects 120 000 times their weight and soft grippers are showcased. In addition, the hydrogels can be recycled without a loss in performance. The uniaxial swelling allows adding channels through the gel for local solvent delivery, further increasing the actuation rate and cyclability. Thus, fibrillar networks can overcome the major drawbacks of hydrogel actuators and is a significant advancement towards hydrogel-based lifelike machines.

Multilayer Dielectric Elastomer with Reconfigurable Electrodes for Artificial Muscle.

High-performance multilayer dielectric elastomer actuators (DEAs) are well-positioned to overcome the insufficient output force and energy density as artificial muscles. However, due to the fabrication process, the multilayer DEAs with nonmodifiable structures often suffer from the limitation of short lifespans and scalable preparation. Herein, reusable multilayer DEAs with the detachable and reconfigurable structure are fabricated. This is achieved by realizing scalable compliant electrodes using the continuous spatial confining forced network assembly (CSNA) method and combining the vacuum lamination (VL) approach to have good attachability and detachability with the VHB dielectric elastomer. The flexible roller-based CSNA method is used to prepare the large area compliant electrodes composed of α, ω-dihydroxy polydimethylsiloxane and electrically conductive nanoparticles. The fabricated electrodes can continuously work over 10 000 cycles at 40% strained stretching and maintain smooth surfaces to construct multilayer DEAs. Moreover, owing to the detachable configuration of the DEAs, the electrodes can also be recovered and reused for building new actuators. The lower limb assistive device is demonstrated by detachable multilayer spring roll DEAs, achieving approximately 3.1 degrees of flexion and extension movement of knee models under a voltage of 7 kV. The detachable and reconfigurable multilayer DEAs shed new light on the applications of wearable assistive devices.

Reliability of printed stretchable electronics based on nano/micro materials for practical applications.

Recent decades have witnessed the booming development of stretchable electronics based on nano/micro composite inks. Printing is a scalable, low-cost, and high-efficiency fabrication tool to realize stretchable electronics through additive processes. However, compared with conventional flexible electronics, stretchable electronics need to experience more severe mechanical deformation which may cause destructive damage. Most of the reported works in this field mainly focus on how to achieve a high stretchability of nano/micro composite conductors or single working modules/devices, with limited attention given to the reliability for practical applications. In this minireview, we summarized the failure modes when printing stretchable electronics using nano/micro composite ink, including dysfunction of the stretchable interconnects, the stress-concentrated rigid-soft interfaces for hybrid electronics, the vulnerable vias upon stretching, thermal accumulation, and environmental instability of stretchable materials. Strategies for tackling these challenges to realize reliable performances are proposed and discussed. Our review provides an overview on the importance of reliable, printable, and stretchable electronics, which are the key enablers in propelling stretchable electronics from fancy demos to practical applications.

Ion rectification based on gel polymer electrolyte ionic diode.

Biological ion channels rely on ions as charge carriers and unidirectional ion flow to produce and transmit signals. To realize artificial biological inspired circuitry and seamless human-machine communication, ion-transport-based rectification devices should be developed. In this research, poly(methyl methacrylate) (PMMA) and poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP) gel polymer electrolytes (GPEs) are assembled to construct a novel ionic diode, enabling ion rectification through ion-diffusion/migration that emulates biological systems. This ion rectification results from the different diffusion/migration behaviors of mobile ions transporting in the GPE heterojunction. The electrical tests of the GPE heterojunction reveal outstanding rectifying ratio of 23.11. The GPE ionic diode operates in wide temperature window, from -20 °C (anti-freezing) to 125 °C (thermal tolerance). The absence of redox reactions is verified in the cyclic voltammogram. The GPE ionic diodes are used to construct ionic logic gates for signal communication. Furthermore, rectification of a triboelectric nanogenerator and potential for synaptic devices are demonstrated.

Photothermal modulated dielectric elastomer actuator for resilient soft robots.

Soft robots need to be resilient to extend their operation under unpredictable environments. While utilizing elastomers that are tough and healable is promising to achieve this, mechanical enhancements often lead to higher stiffness that deteriorates actuation strains. This work introduces liquid metal nanoparticles into carboxyl polyurethane elastomer to sensitize a dielectric elastomer actuator (DEA) with responsiveness to electric fields and NIR light. The nanocomposite can be healed under NIR illumination to retain high toughness (55 MJ m-3) and can be recycled at lower temperatures and shorter durations due to nanoparticle-elastomer interactions that minimize energy barriers. During co-stimulation, photothermal effects modulate the elastomer moduli to lower driving electric fields of DEAs. Bilayer configurations display synergistic actuation under co-stimulation to improve energy densities, and enable a DEA crawler to achieve longer strides. This work paves the way for a generation of soft robots that achieves both resilience and high actuation performance.