Functionally antagonistic polyelectrolyte for electro-ionic soft actuator.

Electro-active ionic soft actuators have been intensively investigated as an artificial muscle for soft robotics due to their large bending deformations at low voltages, small electric power consumption, superior energy density, high safety and biomimetic self-sensing actuation. However, their slow responses, poor durability and low bandwidth, mainly resulting from improper distribution of ionic conducting phase in polyelectrolyte membranes, hinder practical applications to real fields. We report a procedure to synthesize efficient polyelectrolyte membranes that have continuous conducting network suitable for electro-ionic artificial muscles. This functionally antagonistic solvent procedure makes amphiphilic Nafion molecules to assemble into micelles with ionic surfaces enclosing non-conducting cores. Especially, the ionic surfaces of these micelles combine together during casting process and form a continuous ionic conducting phase needed for high ionic conductivity, which boosts the performance of electro-ionic soft actuators by 10-time faster response and 36-time higher bending displacement. Furthermore, the developed muscle shows exceptional durability over 40 days under continuous actuation and broad bandwidth below 10 Hz, and is successfully applied to demonstrate an inchworm-mimetic soft robot and a kinetic tensegrity system.

Polysulfonated covalent organic framework as active electrode host for mobile cation guests in electrochemical soft actuator.

Tailoring transfer dynamics of mobile cations across solid-state electrolyte-electrode interfaces is crucial for high-performance electrochemical soft actuators. In general, actuation performance is directly proportional to the affinity of cations and anions in the electrolyte for the opposite electrode surfaces under an applied field. Herein, to maximize electrochemical actuation, we report an electronically conjugated polysulfonated covalent organic framework (pS-COF) used as a common electrolyte-electrode host for 1-ethyl-3-methylimidazolium cation embedded into a Nafion membrane. The pS-COF-based electrochemical actuator exhibits remarkable bending deflection at near-zero voltage (~0.01 V) and previously unattainable blocking force, which is 34 times higher than its own weight. The ultrafast step response shows a very short rising time of 1.59 seconds without back-relaxation, and substantial ultralow-voltage actuation at higher frequencies up to 5.0 hertz demonstrates good application prospects of common electrolyte-electrode hosts. A soft fluidic switch is constructed using the proposed soft actuator as a potential engineering application.

A Dual-Responsive Magnetoactive and Electro-Ionic Soft Actuator Derived from a Nickel-Based Metal-Organic Framework.

There is growing demand for multiresponsive soft actuators for the realization of natural, safe, and complex motions in robotic interactions. In particular, soft actuators simultaneously stimulated by electrical and magnetic fields are always under development owing to their simple controllability and reliability during operation. Herein, magnetically and electrically driven dual-responsive soft actuators (MESAs) derived from novel nickel-based metal-organic frameworks (Ni-MOFs-700C), are reported. Nanoscale Ni-MOFs-700C has excellent electrochemical and magnetic properties that allow it to be used as a multifunctional material under both magnetoactive and electro-ionic actuations. The dual-responsive MESA exhibits a bending displacement of 30 mm and an ultrafast rising time of 1.5 s under a very low input voltage of 1 V and also exerts a bending deflection of 12.5 mm at 50 mT under a high excitation frequency of 5 Hz. By utilizing a dual-responsive MESA, the hovering motion of a hummingbird robot is demonstrated under magnetic and electrical stimuli.

Antagonistically Functionalized Diatom Biosilica for Bio-Triboelectric Generators.

Although biomaterial-based triboelectric nanogenerators (Bio-TENGs) for use in wearable electronics and implantable sensors have been developed, power generation is not suitable for satisfying the basic requirements for practical applications. Here, to greatly enhance output performances of Bio-TENG devices, an antagonistic approach of diatom frustules (DFs) with amine and fluorine chemical functionalizations is reported. The DFs are treated with piranha solution to increase the density of hydroxyl groups and tribo-positive and tribo-negative composite films are designed with antagonistically functionalized DFs. The tribo-positive composites having electron donating functionality consist of aminated DFs and cellulose nanocrystals (CNCs), while the tribo-negative composite is composed of fluorinated DFs and polydimethylsiloxane (PDMS). An antagonistically and chemically functionalized TENG (ACF TENG) with an efficient contact area of 9.6 cm2 under a force of 8 N and a frequency of 5 Hz exhibits an output voltage of 248 V, a short-circuit current of 16.4 µA, and a power density of 2.01 W m-2 , which is 16.6 times higher than a reference (CNC:PDMS) TENG. This study shows a simple antagonistic approach for chemical functionalization as an efficient method to manipulate the tribo-polarity of bio-additives for enhancing power generation of Bio-TENGs.

Electro-Active and Photo-Active Vanadium Oxide Nanowire Thermo-Hygroscopic Actuators for Kirigami Pop-up.

Emerging technologies such as soft robotics, active biomedical devices, wearable electronics, haptic feedback systems, and healthcare systems require high-fidelity soft actuators showing reliable responses under multi-stimuli. In this study, the authors report an electro-active and photo-active soft actuator based on a vanadium oxide nanowire (VONW) hybrid film with greatly improved actuation performances. The VONWs directly grown on a cellulose fiber network increase the surface area up to 30-fold and boost the hydrophilicity owing to the presence of oxygen-rich functional groups in the nanowire surfaces. Taking advantage of the high surface area and hydrophilicity of VONWs, a soft thermo-hygroscopic VONW actuator capable of being controlled by both light and electric sources shows greatly enhanced actuation deformation by almost 70% and increased actuation speed over 3 times during natural convection cooling. Most importantly, the proposed VONW actuator exhibits a remarkably improved blocking force of up to 200% compared with a bare paper actuator under light stimulation, allowing them to realize a complex kirigami pop-up and to accomplish repeatable shape transformation from a 2D planar surface to a 3D configuration.

Diatom Bio-Silica and Cellulose Nanofibril for Bio-Triboelectric Nanogenerators and Self-Powered Breath Monitoring Masks.

The application of biodegradable and biocompatible materials to triboelectric nanogenerators (TENGs) for harvesting energy from motions of the human body has been attracting significant research interest. Herein, we report diatom bio-silica as a biomaterial additive to enhance the output performance of cellulose nanofibril (CNF)-based TENGs. Diatom frustules (DFs), which are tribopositive bio-silica having hierarchically porous three-dimensional structures and high surface area, have hydrogen bonds with CNFs, resulting in enhanced electron-donating capability and a more roughened surface of the DF-CNF composite film. Hence, DFs were applied to form a tribopositive composite film with CNFs. The DF-CNF biocomposite film is mechanically strong, electron-rich, low-cost, and frictionally rough. The DF-CNF TENG showed an output voltage of 388 V and time-averaged power of 85.5 mW/m2 in the contact-separation mode with an efficient contact area of 4.9 cm2, and the generated power was sufficient for instantaneous illumination of 102 light-emitting diodes. In addition, a cytotoxicity study and biocompatibility tests on rabbit skin suggested that the DF-CNF composite was biologically safe. Moreover, a practical application of the DF-CNF TENG was examined with a self-powered smart mask for human breathing monitoring. This study not only suggests high output performance of biomaterial-based TENGs but also presents the diverse advantages of the DFs in human body-related applications such as self-powered health monitoring masks, skin-attachable power generators, and tactile feedback systems.

CTF-based soft touch actuator for playing electronic piano.

In the field of bioinspired soft robotics, to accomplish sophisticated tasks in human fingers, electroactive artificial muscles are under development. However, most existing actuators show a lack of high bending displacement and irregular response characteristics under low input voltages. Here, based on metal free covalent triazine frameworks (CTFs), we report an electro-ionic soft actuator that shows high bending deformation under ultralow input voltages that can be implemented as a soft robotic touch finger on fragile displays. The as-synthesized CTFs, derived from a polymer of intrinsic microporosity (PIM-1), were combined with poly(3,4-ethylenedioxythiophene)-poly(styrenesulfonate) (PEDOT-PSS) to make a flexible electrode for a high-performance electro-ionic soft actuator. The proposed soft touch finger showed high peak-to-peak displacement of 17.0 mm under ultralow square voltage of ±0.5 V, with 0.1 Hz frequency and 4 times reduced phase delay in harmonic response compared with that of a pure PEDOT-PSS-based actuator. The significant actuation performance is mainly due to the unique physical and chemical configurations of CTFs electrode with highly porous and electrically conjugated networks. On a fragile display, the developed soft robotic touch finger array was successfully used to perform soft touching, similar to that of a real human finger; device was used to accomplish a precise task, playing electronic piano.

Graphene Mesh for Self-Sensing Ionic Soft Actuator Inspired from Mechanoreceptors in Human Body.

Here, inspired by mechanoreceptors in the human body, a self-sensing ionic soft actuator is developed that precisely senses the bending motions during actuating utilizing a 3D graphene mesh electrode. The graphene mesh electrode has the permeability of mobile ions inside the ionic exchangeable polymer and shows low electrical resistance of 6.25 Ω Sq-1, maintaining high electrical conductivity in large bending deformations of 180°. In this sensing system, the graphene woven mesh is embedded inside ionic polymer membrane to interact with mobile ions and to trace their movements. The migration of mobile ions inside the membrane induces an electrical signal on the mesh and provides the information regarding ion distribution, which is proven to be highly correlated with the bending deformation of the actuator. Using this integrated self-sensing system, the responses of an ionic actuator to various input stimulations are precisely estimated for both direct current and alternating current inputs. Even though the generated displacement is extremely small around 300 µm at very low driving voltage of 0.1 V, high level accuracy (96%) of estimated deformations could be achieved using the self-sensing actuator system.

Crumpled Quaternary Nanoarchitecture of Sulfur-Doped Nickel Cobalt Selenide Directly Grown on Carbon Cloth for Making Stronger Ionic Soft Actuators.

A novel crumpled quaternary sulfur-doped nickel cobalt selenide nanoarchitecture grown on carbon cloth (S-(NiCo)Se/CC) has been successfully synthesized as an electrode material for high-performance ionic polymer-carbon cloth composite (IP-CCC) actuators. A facile one-step solvothermal process has been introduced here to synthesize S-(NiCo)Se/CC, resolving the time-consuming, complicated, and costly problems of existing methods. Taking advantage of the outstanding electron transport kinetics and three-dimensionally interconnected nature of the transition-metal chalcogenide structure, the hybrid carbon cloth electrode with quaternary sulfur-doped selenide nanoarchitectures exhibits low electrical resistivity (3 times lower than that of bare CC), high areal capacitance (409 mF/cm2), and excellent cycle stability (over 4000 cycles). Moreover, due to the synergistic effect between S-(NiCo)Se and a carbon cloth substrate, the S-(NiCo)Se/CC electrode-based actuator exhibits high blocking force (38.5 mN), 6 h durability, and large bending strain (0.47%). Compared with other actuators reported in the literature, the S-(NiCo)Se/CC electrode-based actuator shows much higher normalized blocking force, leading to opening of new potential applications in the field of next-generation soft electronics. Moreover, stacked multiple IP-CCC actuators in parallel exhibit an exceptional blocking force of 0.174 N under direct current 4 V.

Electroactive Artificial Muscles Based on Functionally Antagonistic Core-Shell Polymer Electrolyte Derived from PS-b-PSS Block Copolymer.

Electroactive ionic soft actuators, a type of artificial muscles containing a polymer electrolyte membrane sandwiched between two electrodes, have been intensively investigated owing to their potential applications to bioinspired soft robotics, wearable electronics, and active biomedical devices. However, the design and synthesis of an efficient polymer electrolyte suitable for ion migration have been major challenges in developing high-performance ionic soft actuators. Herein, a highly bendable ionic soft actuator based on an unprecedented block copolymer is reported, i.e., polystyrene-b-poly(1-ethyl-3-methylimidazolium-4-styrenesulfonate) (PS-b-PSS-EMIm), with a functionally antagonistic core-shell architecture that is specifically designed as an ionic exchangeable polymer electrolyte. The corresponding actuator shows exceptionally good actuation performance, with a high displacement of 8.22 mm at an ultralow voltage of 0.5 V, a fast rise time of 5 s, and excellent durability over 14 000 cycles. It is envisaged that the development of this high-performance ionic soft actuator could contribute to the progress toward the realization of the aforementioned applications. Furthermore, the procedure described herein can also be applied for developing novel polymer electrolytes related to solid-state lithium batteries and fuel cells.

MXene artificial muscles based on ionically cross-linked Ti3C2T x electrode for kinetic soft robotics.

Existing ionic artificial muscles still require a technology breakthrough for much faster response speed, higher bending strain, and longer durability. Here, we report an MXene artificial muscle based on ionically cross-linked Ti3C2T x with poly(3,4 ethylenedioxythiophene)-poly(styrenesulfonate), showing ultrafast rise time of within 1 s in DC responses, extremely large bending strain up to 1.37% in very low input voltage regime (0.1 to 1 V), long-term cyclic stability of 97% up to 18,000 cycles, markedly reduced phase delay, and very broad frequency bandwidth up to 20 Hz with good structural reliability without delamination under continuous electrical stimuli. These artificial muscles were successfully applied to make an origami-inspired narcissus flower robot as a wearable brooch and dancing butterflies and leaves on a tree as a kinetic art piece. These successful demonstrations elucidate the wide potential of MXene-based soft actuators for the next-generation soft robotic devices including wearable electronics and kinetic art pieces.

Graphene-coated meshes for electroactive flow control devices utilizing two antagonistic functions of repellency and permeability.

The wettability of graphene on various substrates has been intensively investigated for practical applications including surgical and medical tools, textiles, water harvesting, self-cleaning, oil spill removal and microfluidic devices. However, most previous studies have been limited to investigating the intrinsic and passive wettability of graphene and graphene hybrid composites. Here, we report the electrowetting of graphene-coated metal meshes for use as electroactive flow control devices, utilizing two antagonistic functions, hydrophobic repellency versus liquid permeability. Graphene coating was able to prevent the thermal oxidation and corrosion problems that plague unprotected metal meshes, while also maintaining its hydrophobicity. The shapes of liquid droplets and the degree of water penetration through the graphene-coated meshes were controlled by electrical stimuli based on the functional control of hydrophobic repellency and liquid permeability. Furthermore, using the graphene-coated metal meshes, we developed two active flow devices demonstrating the dynamic locomotion of water droplets and electroactive flow switching.