Active entanglement enables stochastic, topological grasping.

Grasping, in both biological and engineered mechanisms, can be highly sensitive to the gripper and object morphology, as well as perception and motion planning. Here, we circumvent the need for feedback or precise planning by using an array of fluidically actuated slender hollow elastomeric filaments to actively entangle with objects that vary in geometric and topological complexity. The resulting stochastic interactions enable a unique soft and conformable grasping strategy across a range of target objects that vary in size, weight, and shape. We experimentally evaluate the grasping performance of our strategy and use a computational framework for the collective mechanics of flexible filaments in contact with complex objects to explain our findings. Overall, our study highlights how active collective entanglement of a filament array via an uncontrolled, spatially distributed scheme provides options for soft, adaptable grasping.

A soft microrobot with highly deformable 3D actuators for climbing and transitioning complex surfaces.

The climbing microrobots have attracted growing attention due to their promising applications in exploration and monitoring of complex, unstructured environments. Soft climbing microrobots based on muscle-like actuators could offer excellent flexibility, adaptability, and mechanical robustness. Despite the remarkable progress in this area, the development of soft microrobots capable of climbing on flat/curved surfaces and transitioning between two different surfaces remains elusive, especially in open spaces. In this study, we address these challenges by developing voltage-driven soft small-scale actuators with customized 3D configurations and active stiffness adjusting. Combination of programmed strain distributions in liquid crystal elastomers (LCEs) and buckling-driven 3D assembly, guided by mechanics modeling, allows for voltage-driven, complex 3D-to-3D shape morphing (bending angle > 200°) at millimeter scales (from 1 to 10 mm), which is unachievable previously. These soft actuators enable development of morphable electroadhesive footpads that can conform to different curved surfaces and stiffness-variable smart joints that allow different locomotion gaits in a single microrobot. By integrating such morphable footpads and smart joints with a deformable body, we report a multigait, soft microrobot (length from 6 to 90 mm, and mass from 0.2 to 3 g) capable of climbing on surfaces with diverse shapes (e.g., flat plane, cylinder, wavy surface, wedge-shaped groove, and sphere) and transitioning between two distinct surfaces. We demonstrate that the microrobot could navigate from one surface to another, recording two corresponding ceilings when carrying an integrated microcamera. The developed soft microrobot can also flip over a barrier, survive extreme compression, and climb bamboo and leaf.

Soft Actuator with Biomass Porous Electrode: A Strategy for Lowering Voltage and Enhancing Durability.

Electroactive artificial muscles with deformability have attracted widespread interest in the field of soft robotics. However, the design of artificial muscles with low-driven voltage and operational durability remains challenging. Herein, novel biomass porous carbon (BPC) electrodes are proposed. The nanoporous BPC enables the electrode to provide exposed active surfaces for charge transfer and unimpeded channels for ion migration, thus decreasing the driving voltage, enhancing time durability, and maintaining the actuation performances simultaneously. The proposed actuator exhibits a high displacement of 13.6 mm (bending strain of 0.54%) under 0.5 V and long-term durability of 99.3% retention after 550,000 cycles (∼13 days) without breaks. Further, the actuators are integrated to perform soft touch on a smartphone and demonstrated as bioinspired robots, including a bionic butterfly and a crawling robot (moving speed = 0.08 BL s-1). This strategy provides new insight into the design and fabrication of high-performance electroactive soft actuators with great application potential.

Wireless Electrochemical Gel Actuators.

Soft actuators generate motion in response to external stimuli and are indispensable for soft robots, particularly future miniature robots with complex structure and motion. Similarly to conventional hard robots, electricity is suitable for the stimulation. However, previous electrochemical soft actuators require a tethered connection to a power supply, limiting their size, structure, and motion. Here, wireless electrochemical soft actuators composed of hydrogels and driven by bipolar electrochemistry are reported. Viologen, which dimerizes by one-electron reduction and dissociates by one-electron oxidation, is incorporated in the side chains of the gel networks and works as a reversible cross-link. Wireless and reversible electrochemical actuation of the hydrogels, i.e., muscle-like shrinking and swelling, is demonstrated at microscopic and even macroscopic scales.

Reprogrammable Magnetic Soft Actuators with Microfluidic Functional Modules via Pixel-Assembly.

Magnetic soft actuators and robots have attracted considerable attention in biomedical applications due to their speedy response, programmability, and biocompatibility. Despite recent advancements, the fabrication process of magnetic actuators and the reprogramming approach of their magnetization profiles continue to pose challenges. Here, a facile fabrication strategy is reported based on arrangements and distributions of reusable magnetic pixels on silicone substrates, allowing for various magnetic actuators with customizable architectures, arbitrary magnetization profiles, and integration of microfluidic technology. This approach enables intricate configurations with decent deformability and programmability, as well as biomimetic movements involving grasping, swimming, and wriggling in response to magnetic actuation. Moreover, microfluidic functional modules are integrated for various purposes, such as on/off valve control, curvature adjustment, fluid mixing, dynamic microfluidic architecture, and liquid delivery robot. The proposed method fulfills the requirements of low-cost, rapid, and simplified preparation of magnetic actuators, since it eliminates the need to sustain pre-defined deformations during the magnetization process or to employ laser heating or other stimulation for reprogramming the magnetization profile. Consequently, it is envisioned that magnetic actuators fabricated via pixel-assembly will have broad prospects in microfluidics and biomedical applications.

3D Printable Active Hydrogels with Supramolecular Additive-Driven Adaptiveness.

Smart hydrogels are a promising candidate for the development of next-generation soft materials due to their stimuli-responsiveness, deformability, and biocompatibility. However, it remains challenging to enable hydrogels to actively adapt to various environmental conditions like living organisms. In this work, supramolecular additives are introduced to the hydrogel matrix to confer environmental adaptiveness. Specifically, their microstructures, swelling behaviors, mechanical properties, and transparency can adapt to external environmental conditions. Moreover, the presence of hydrogen bonding provides the hydrogel with applicable rheological properties for 3D extrusion printing, thus allowing for the facile preparation of thickness-dependent camouflage and multistimuli responsive complex. The environmentally adaptive hydrogel developed in this study offers new approaches for manipulating supramolecular interactions and broadens the capability of smart hydrogels in information security and multifunctional integrated actuation.

Mutable Collagenous Tissue: A Concept Generator for Biomimetic Materials and Devices.

Echinoderms (starfish, sea-urchins and their close relations) possess a unique type of collagenous tissue that is innervated by the motor nervous system and whose mechanical properties, such as tensile strength and elastic stiffness, can be altered in a time frame of seconds. Intensive research on echinoderm 'mutable collagenous tissue' (MCT) began over 50 years ago, and over 20 years ago, MCT first inspired a biomimetic design. MCT, and sea-cucumber dermis in particular, is now a major source of ideas for the development of new mechanically adaptable materials and devices with applications in diverse areas including biomedical science, chemical engineering and robotics. In this review, after an up-to-date account of present knowledge of the structural, physiological and molecular adaptations of MCT and the mechanisms responsible for its variable tensile properties, we focus on MCT as a concept generator surveying biomimetic systems inspired by MCT biology, showing that these include both bio-derived developments (same function, analogous operating principles) and technology-derived developments (same function, different operating principles), and suggest a strategy for the further exploitation of this promising biological resource.

Programmable droplet manipulation and wetting with soft magnetic carpets.

The ability to regulate interfacial and wetting properties is highly demanded in anti-icing, anti-biofouling, and medical and energy applications. Recent work on liquid-infused systems achieved switching wetting properties, which allow us to turn between slip and pin states. However, patterning the wetting of surfaces in a dynamic fashion still remains a challenge. In this work, we use programmable wetting to activate and propel droplets over large distances. We achieve this with liquid-infused soft magnetic carpets (SMCs) that consist of pillars that are responsive to external magnetic stimuli. Liquid-infused SMCs, which are sticky for a water droplet, become slippery upon application of a magnetic field. Application of a patterned magnetic field results in a patterned wetting on the SMC. A traveling magnetic field wave translates the patterned wetting on the substrate, which allows droplet manipulation. The droplet speed increases with an increased contact angle and with the droplet size, which offers a potential method to sort and separate droplets with respect to their contact angle or size. Furthermore, programmable control of the droplet allows us to conduct reactions by combining droplets loaded with reagents. Such an ability of conducting small-scale reactions on SMCs has the potential to be used for automated analytical testing, diagnostics, and screening, with a potential to reduce the chemical waste.

Thermally and Magnetically Programmable Hydrogel Microactuators.

The rapid development in micro-machinery enabled the investigation of smart materials that can embody fast response, programmable actuation, and flexibility to perform mechanical work. Soft magnetic actuators represent an interesting platform toward combining those properties. This study focuses on the synthesis of micro-actuators that respond to thermal and magnetic stimuli using micro-molding with a soft template as a fabrication technique. These microsystems consist of a hydrogel matrix loaded with anisotropic magnetic nanospindles. When a homogeneous magnetic field is applied, the nanospindles initially dispersed in monomer solution, align and assemble into dipolar chains. The ensuing UV-polymerization creates a network and conveniently arrests these nanostructures. Consequently, the magnetic dipole moment is coplanar with the microgel. Varying the shape, volume, and composition of the micro-actuators during synthesis provides a temperature-dependent control over the magnetic response and the polarizability. Beyond isotropic swelling, shaping the hydrogel as long thin ribbons with a passive layer on one side allows for differential swelling leading to bending and twisting deformations, for example, 2D- or 3D-spiral. These deformations involve a reversible amplification of the magnetic response and orientation of the hydrogels under magnetic field. Temperature control herewith determines the conformation and simultaneously the magnetic response of the micro-actuators.

Liquid Crystalline Elastomer for Separate or Collective Sensing and Actuation Functions.

A porous liquid crystalline elastomer actuator filled with an ionic liquid (PLCE-IL) is shown to exhibit the functions of two classes of materials: electrically responsive, deformable materials for sensing and soft active materials for stimuli-triggered actuation. On one hand, upon the order-disorder phase transition of aligned mesogens, PLCE-IL behaves like a typical actuator capable of reversible shape change and can be used to assemble light-fuelled soft robot. On the other hand, at temperatures below the phase transition, PLCE-IL is an elastomer that can sustain and sense large deformations of various modes as well as environmental condition changes by reporting the corresponding electrical resistance variation. The two distinguished functions can also be used collectively with PLCE-IL integrated in one device. This intelligent feature is demonstrated with an artificial arm. When the arm is manually powered to fold and unfold, the PLCE-IL strip serves as a deformation sensor; while when the manual power is not available, the role of the PLCE-IL strip is switched to an actuator that enables light-driven folding and unfolding of the arm. This study shows that electrically responsive LCEs are a potential materials platform that offers possibilities for merging deformable electronic and actuation applications.

Magnetically and Electrically Responsive Soft Actuator Derived from Ferromagnetic Bimetallic Organic Framework.

The advancement in smart devices and soft robotics necessitates the use of multiresponsive soft actuators with high actuation stroke and stable reversibility for their use in real-world applications. Here, this work reports a magnetically and electrically dual responsive soft actuator based on neodymium and iron bimetallic organic frameworks (NdFeMOFs@700). The ferromagnetic NdFeMOFs@700 exhibits a porous carbon structure with excellent magnetization saturation (166.96 emu g-1 ) which allows its application to a dual functional material in both magnetoactive and electro-ionic actuations. The electro-ionic soft actuator, which is fabricated using NdFeMOFs@700 and PEDOT-PSS, demonstrates 4.5 times higher ionic charge storage capacity (68.21 mF cm-2 ) and has excellent cycle stability compared with the PEDOT-PSS based actuator. Under a low sinusoidal input voltage of 1 V, the dual-responsive actuator displays bending displacement of 15.46 mm and also generates deflection of 10 mm at 50 mT. Present results show that the ferromagnetic bimetallic organic frameworks can open a new way to make dual responsive soft actuators due to the hierarchically porous structures with its high redox activity, superior magnetic properties, and larger electrochemical capacitance. With the NdFeMOFs@700 based soft actuators, walking movement of a starfish robot is demonstrated by applying both the magnetic and electric fields.

Carbon-Based Nanomaterials Electrodes of Ionic Soft Actuators: From Initial 1D Structure to 3D Composite Structure for Flexible Intelligent Devices.

With the rapid development of autonomous and intelligent devices driven by soft actuators, ion soft actuators in flexible intelligent devices have several advantages over other actuators, including their light weight, low voltage drive, large strain, good flexibility, fast response, etc. Traditional ionic polymer metal composites have received a lot of attention over the past decades, but they suffer from poor driving performance and short service lives since the precious metal electrodes are not only expensive, heavy, and labor-intensive, but also prone to cracking with repeated actuation. As excellent candidates for the electrode materials of ionic soft actuators, carbon-based nanomaterials have received a lot of interest because of their plentiful reserves, low cost, and excellent mechanical, electrical, and electrochemical properties. This research reviewed carbon-based nanomaterial electrodes of ion soft actuators for flexible smart devices from a fresh perspective from 1D to 3D combinations. The design of the electrode structure is introduced after the driving mechanism of ionic soft actuators. The details of ionic soft actuator electrodes made of carbon-based nanomaterials are then provided. Additionally, a summary of applications for flexible intelligent devices is provided. Finally, suggestions for challenges and prospects are made to offer direction and inspiration for further development.

Hybrid Fabrication of Prestrain-Locked Acrylic Dielectric Elastomer Thin Films and Multilayer Stacks.

Dielectric elastomers based on commercial acrylic dielectric elastomers (VHB adhesive films) are widely investigated for soft actuators due to their large electrically driven actuation strain and high work density. However, the VHB films require prestretching to overcome electromechanical instability, which adds fabrication complexity. In addition, their high viscoelasticity leads to a low response speed. Interpenetrated polymer networks (IPNs) are developed to lock the prestrain in VHB films, resulting in free-standing films that are capable of large-strain actuation. In this work, a prestrain-locked high-performance dielectric elastomer thin film (VHB-IPN-P) by introducing 1,6-hexanediol diacrylate to create an IPN in the VHB network and a plasticizer to enhance the actuation speed is reported. VHB-IPN-P based actuators exhibit stable actuation at 60% strain up to 10 Hz and reach a peak energy density of 102 J kg⁻1 . In addition, a hybrid process is also developed for the fabrication of multilayer stacks of VHB-IPN-P with strong inter-layer bonding and structural integrity. Four-layer stacks fabricated preserve the strain and energy density of single-layer VHB-IPN-P films but with linearly scaled force and work output.

Underactuated fluidic control of a continuous multistable membrane.

This work addresses the challenge of underactuated pattern generation in continuous multistable structures. The examined configuration is a slender membrane which can concurrently sustain two different equilibria states, separated by transition regions, and is actuated by a viscous fluid. We first demonstrate the formation and motion of a single transition region and then sequencing of several such moving transition regions to achieve arbitrary patterns by controlling the inlet pressure of the actuating fluid. Finally, we show that nonuniform membrane properties, along with transient dynamics of the fluid, can be leveraged to directly snap through any segment of the membrane.

Simultaneous Sensing and Actuating Capabilities of a Triple-Layer Biomimetic Muscle for Soft Robotics.

This work presents the fabrication and characterization of a triple-layered biomimetic muscle constituted by polypyrrole (PPy)-dodecylbenzenesulfonate (DBS)/adhesive tape/PPy-DBS demonstrating simultaneous sensing and actuation capabilities. The muscle was controlled by a neurobiologically inspired cortical neural network sending agonist and antagonist signals to the conducting polymeric layers. Experiments consisted of controlled voluntary movements of the free end of the muscle at angles of ±20°, ±30°, and ±40° while monitoring the muscle's potential response. Results show the muscle's potential varies linearly with applied current amplitude during actuation, enabling current sensing. A linear dependence between muscle potential and temperature enabled temperature sensing. Electrolyte concentration changes also induced exponential variations in the muscle's potential, allowing for concentration sensing. Additionally, the influence of the electric current density on the angular velocity, the electric charge density, and the desired angle was studied. Overall, the conducting polymer-based soft biomimetic muscle replicates properties of natural muscles, permitting simultaneous motion control, current, temperature, and concentration sensing. The integrated neural control system exhibits key features of biological motion regulation. This muscle actuator with its integrated sensing and control represents an advance for soft robotics, prosthetics, and biomedical devices requiring biomimetic multifunctionality.

Fast Light-Driven Motion of Polydopamine Nanomembranes.

The actuation of micro- and nanostructures controlled by external stimuli remains one of the exciting challenges in nanotechnology due to the wealth of fundamental questions and potential applications in energy harvesting, robotics, sensing, biomedicine, and tunable metamaterials. Photoactuation utilizes the conversion of light into motion through reversible chemical and physical processes and enables remote and spatiotemporal control of the actuation. Here, we report a fast light-to-motion conversion in few-nanometer thick bare polydopamine (PDA) membranes stimulated by visible light. Light-induced heating of PDA leads to desorption of water molecules and contraction of membranes in less than 140 µs. Switching off the light leads to a spontaneous expansion in less than 20 ms due to heat dissipation and water adsorption. Our findings demonstrate that pristine PDA membranes are multiresponsive materials that can be harnessed as robust building blocks for soft, micro-, and nanoscale actuators stimulated by light, temperature, and moisture level.

Bending Actuation of Hydrogels through Rotation of Light-Driven Molecular Motors.

The unidirectional rotation of chemically crosslinked light-driven molecular motors is shown to progressively shift the swelling equilibrium of hydrogels. The concentration of molecular motors and the initial strand density of the polymer network are key parameters to modulate the macroscopic contraction of the material, and both parameters can be tuned using polymer chains of different molecular weights. These findings led to the design of optimized hydrogels revealing a half-time contraction of approximately 5 min. Furthermore, under inhomogeneous stimulation, the local contraction event was exploited to design useful bending actuators with an energy output 400 times higher than for previously reported self-assembled systems involving rotary motors. In the present configuration, we measure that a single molecular motor can lift up loads of 200 times its own molecular weight.

One-Step Manufacturing of Supramolecular Liquid-Crystal Elastomers by Stress-Induced Alignment and Hydrogen Bond Exchange.

Liquid-crystal elastomers (LCEs) capable of performing large and reversible deformation in response to an external stimulus are an important class of soft actuators. However, their manufacturing process typically involves a multistep approach that requires harsh conditions. For the very first time, LCEs with customized geometries that can be manufactured by a rapid one-step approach at room temperature are developed. The LCEs are hydrogen bond (H-bond) crosslinked main chain polymers comprising flexible short side chains. Applying a stretching/shear force to the LCE can simultaneously induce mesogen alignment and H-bond exchange, allowing for the formation of well-aligned LCE networks stabilized by H-bonds. Based on this working principle, soft actuators in fibers and 2D/3D objects can be manufactured by mechanical stretching or melt extrusion within a short time (e.g. <1 min). These actuators can perform reversible macroscopic motions with large, controlled deformations up to 38 %. The dynamic nature of H-bonds also provides the actuators with reprocessability and reprogrammability. Thus, this work opens the way for the one-step and custom manufacturing of soft actuators.

Bioinspired Freeze-Tolerant Soft Materials: Design, Properties, and Applications.

In nature, many biological organisms have developed the exceptional antifreezing ability to survive in extremely cold environments. Inspired by the freeze resistance of these organisms, researchers have devoted extensive efforts to develop advanced freeze-tolerant soft materials and explore their potential applications in diverse areas such as electronic skin, soft robotics, flexible energy, and biological science. Herein, a comprehensive overview on the recent advancement of freeze-tolerant soft materials and their emerging applications from the perspective of bioinspiration and advanced material engineering is provided. First, the mechanisms underlying the freeze tolerance of cold-enduring biological organisms are introduced. Then, engineering strategies for developing antifreezing soft materials are summarized. Thereafter, recent advances in freeze-tolerant soft materials for different technological applications such as smart sensors and actuators, energy harvesting and storage, and cryogenic medical applications are presented. Finally, future challenges and opportunities for the rapid development of bioinspired freeze-tolerant soft materials are discussed.

One-Pot Synthesis of Melt-Processable Supramolecular Soft Actuators.

The application of reprocessable and reprogrammable soft actuators is limited by the synthetic strategies, 3D-shaping capabilities, and small deformations. In this work, melt-processable supramolecular soft actuators based on segmented copolymers containing thiourethane and liquid crystal segments have been prepared via sequential thiol addition reactions in a one-pot approach using commercially available building blocks. The actuators demonstrated immediate, reversible response and weightlifting capabilities with large deformations up to 32 %. Through exploiting the supramolecular cross-links, the material could be recycled and reprogrammed into 3D actuators and welded into an actuator assembly with different deformation modes. Our work offers a one-pot synthesis and straightforward melt-processable approach to prepare supramolecular soft actuators with large deformations that can be reprocessed and reprogrammed into arbitrary 3D shapes.