Electrochemically-driven actuators: from materials to mechanisms and from performance to applications.

Soft actuators, pivotal for converting external energy into mechanical motion, have become increasingly vital in a wide range of applications, from the subtle engineering of soft robotics to the demanding environments of aerospace exploration. Among these, electrochemically-driven actuators (EC actuators), are particularly distinguished by their operation through ion diffusion or intercalation-induced volume changes. These actuators feature notable advantages, including precise deformation control under electrical stimuli, freedom from Carnot efficiency limitations, and the ability to maintain their actuated state with minimal energy use, akin to the latching state in skeletal muscles. This review extensively examines EC actuators, emphasizing their classification based on diverse material types, driving mechanisms, actuator configurations, and potential applications. It aims to illuminate the complicated driving mechanisms of different categories, uncover their underlying connections, and reveal the interdependencies among materials, mechanisms, and performances. We conduct an in-depth analysis of both conventional and emerging EC actuator materials, casting a forward-looking lens on their trajectories and pinpointing areas ready for innovation and performance enhancement strategies. We also navigate through the challenges and opportunities within the field, including optimizing current materials, exploring new materials, and scaling up production processes. Overall, this review aims to provide a scientifically robust narrative that captures the current state of EC actuators and sets a trajectory for future innovation in this rapidly advancing field.

More Powerful Twistron Carbon Nanotube Yarn Mechanical Energy Harvesters.

Stretching a coiled carbon nanotube (CNT) yarn can provide large, reversible electrochemical capacitance changes, which convert mechanical energy to electricity. Here, it is shown that the performance of these "twistron" harvesters can be increased by optimizing the alignment of precursor CNT forests, plastically stretching the precursor twisted yarn, applying much higher tensile loads during precoiling twist than for coiling, using electrothermal pulse annealing under tension, and incorporating reduced graphene oxide nanoplates. The peak output power for a 1 and a 30 Hz sinusoidal deformation are 0.73 and 3.19 kW kg-1 , respectively, which are 24- and 13-fold that of previous twistron harvesters at these respective frequencies. This performance at 30 Hz is over 12-fold that of other prior-art mechanical energy harvesters for frequencies between 0.1 and 600 Hz. The maximum energy conversion efficiency is 7.2-fold that for previous twistrons. Twistron anode and cathode yarn arrays are stretched 180° out-of-phase by locating them in the negative and positive compressibility directions of hinged wine-rack frames, thereby doubling the output voltage and reducing the input mechanical energy.

Scalable fluid-spinning nanowire-based inorganic semiconductor yarns for electrochromic actuators.

Semiconductor yarns with unique functional characteristics have great potential applications in next-generation electronic devices. However, scalable inorganic semiconductor yarns with excellent mechanical and electrical properties, and environmental stability have not been discovered. In this study, we explored a unique fluid-spinning strategy to obtain a series of scalable inorganic semiconductor yarns including neat and hybrid semiconductor yarns. Different from the conventional yarn spinning strategy through a mechanical motor, we utilized the fluid force from the triple-phase interface to assemble and twist inorganic nanofiber building blocks simultaneously, and eventually obtained highly oriented inorganic nanowire-based semiconductor yarns. The obtained semiconductor yarns showed an excellent flexibility (curvature exceeding 2 cm-1) and mechanical strength (tensile strength of 443 MPa) because of their highly oriented hierarchical nanostructures, which make them coiling able with highly twisted insertion. Additionally, coiled yarns were obtained by combining the host core material and functional guest sheath in a fluid-spinning process, which are flexible in deep cryogenic temperature owing to the pure inorganic building blocks (26.28% tensile strain in liquid nitrogen). In particular, inorganic yarn-based electrochromic actuators can obtain as high as 15.3% tensile stroke and 0.82 J g-1 work capacity by electrochemical charge injection-associated multicolor switching.

Unipolar stroke, electroosmotic pump carbon nanotube yarn muscles.

Success in making artificial muscles that are faster and more powerful and that provide larger strokes would expand their applications. Electrochemical carbon nanotube yarn muscles are of special interest because of their relatively high energy conversion efficiencies. However, they are bipolar, meaning that they do not monotonically expand or contract over the available potential range. This limits muscle stroke and work capacity. Here, we describe unipolar stroke carbon nanotube yarn muscles in which muscle stroke changes between extreme potentials are additive and muscle stroke substantially increases with increasing potential scan rate. The normal decrease in stroke with increasing scan rate is overwhelmed by a notable increase in effective ion size. Enhanced muscle strokes, contractile work-per-cycle, contractile power densities, and energy conversion efficiencies are obtained for unipolar muscles.

Torsional refrigeration by twisted, coiled, and supercoiled fibers.

Higher-efficiency, lower-cost refrigeration is needed for both large- and small-scale cooling. Refrigerators using entropy changes during cycles of stretching or hydrostatic compression of a solid are possible alternatives to the vapor-compression fridges found in homes. We show that high cooling results from twist changes for twisted, coiled, or supercoiled fibers, including those of natural rubber, nickel titanium, and polyethylene fishing line. Using opposite chiralities of twist and coiling produces supercoiled natural rubber fibers and coiled fishing line fibers that cool when stretched. A demonstrated twist-based device for cooling flowing water provides high cooling energy and device efficiency. Mechanical calculations describe the axial and spring-index dependencies of twist-enhanced cooling and its origin in a phase transformation for polyethylene fibers.

Sheath-run artificial muscles.

Although guest-filled carbon nanotube yarns provide record performance as torsional and tensile artificial muscles, they are expensive, and only part of the muscle effectively contributes to actuation. We describe a muscle type that provides higher performance, in which the guest that drives actuation is a sheath on a twisted or coiled core that can be an inexpensive yarn. This change from guest-filled to sheath-run artificial muscles increases the maximum work capacity by factors of 1.70 to 2.15 for tensile muscles driven electrothermally or by vapor absorption. A sheath-run electrochemical muscle generates 1.98 watts per gram of average contractile power-40 times that for human muscle and 9.0 times that of the highest power alternative electrochemical muscle. Theory predicts the observed performance advantages of sheath-run muscles.

Wearable Thermoelectric Devices Based on Au-Decorated Two-Dimensional MoS2.

Two-dimensional (2D) materials have recently opened a new avenue to flexible thermoelectric materials with enhanced performance because of their unique electronic transport properties. Here, we report a feasible approach to improve the thermoelectric performance of transition-metal dichalcogenides by effectively decorating 2D MoS2 with Au nanoparticles using in situ growth. The present Au-decorated MoS2-assembled heterojunction system shows a certain decoupled phenomenon, that is, the Seebeck coefficient and conductivity increased simultaneously. This is due to the occurrence of p-type doping of the MoS2 2H phase and injection energy filtering of dopant-originated carriers around the local band bending at the interface. The composite flexible films can achieve a power factor value of 166.3 µW m-1 K-2 at room temperature, which have great potential for harvesting human body heat.

Sequentially bridged graphene sheets with high strength, toughness, and electrical conductivity.

We here show that infiltrated bridging agents can convert inexpensively fabricated graphene platelet sheets into high-performance materials, thereby avoiding the need for a polymer matrix. Two types of bridging agents were investigated for interconnecting graphene sheets, which attach to sheets by either π-π bonding or covalent bonding. When applied alone, the π-π bonding agent is most effective. However, successive application of the optimized ratio of π-π bonding and covalent bonding agents provides graphene sheets with the highest strength, toughness, fatigue resistance, electrical conductivity, electromagnetic interference shielding efficiency, and resistance to ultrasonic dissolution. Raman spectroscopy measurements of stress transfer to graphene platelets allow us to decipher the mechanisms of property improvement. In addition, the degree of orientation of graphene platelets increases with increasing effectiveness of the bonding agents, and the interlayer spacing increases. Compared with other materials that are strong in all directions within a sheet, the realized tensile strength (945 MPa) of the resin-free graphene platelet sheets was higher than for carbon nanotube or graphene platelet composites, and comparable to that of commercially available carbon fiber composites. The toughness of these composites, containing the combination of π-π bonding and covalent bonding, was much higher than for these other materials having high strengths for all in-plane directions, thereby opening the path to materials design of layered nanocomposites using multiple types of quantitatively engineered chemical bonds between nanoscale building blocks.

Molecular-channel driven actuator with considerations for multiple configurations and color switching.

The ability to achieve simultaneous intrinsic deformation with fast response in commercially available materials that can safely contact skin continues to be an unresolved challenge for artificial actuating materials. Rather than using a microporous structure, here we show an ambient-driven actuator that takes advantage of inherent nanoscale molecular channels within a commercial perfluorosulfonic acid ionomer (PFSA) film, fabricated by simple solution processing to realize a rapid response, self-adaptive, and exceptionally stable actuation. Selective patterning of PFSA films on an inert soft substrate (polyethylene terephthalate film) facilitates the formation of a range of different geometries, including a 2D (two-dimensional) roll or 3D (three-dimensional) helical structure in response to vapor stimuli. Chemical modification of the surface allowed the development of a kirigami-inspired single-layer actuator for personal humidity and heat management through macroscale geometric design features, to afford a bilayer stimuli-responsive actuator with multicolor switching capability.

Ultrathin, Washable, and Large-Area Graphene Papers for Personal Thermal Management.

Freestanding, flexible/foldable, and wearable bifuctional ultrathin graphene paper for heating and cooling is fabricated as an active material in personal thermal management (PTM). The promising electrical conductivity grants the superior Joule heating for extra warmth of 42 °C using a low supply voltage around 3.2 V. Besides, based on its high out-of-plane thermal conductivity, the graphene paper provides passive cooling via thermal transmission from the human body to the environment within 7 s. The cooling effect of graphene paper is superior compared with that of the normal cotton fiber, and this advantage will become more prominent with the increased thickness difference. The present bifunctional graphene paper possesses high durability against bending cycles over 500 times and wash time over 1500 min, suggesting its great potential in wearable PTM.

A flexible metallic actuator using reduced graphene oxide as a multifunctional component.

Flexible actuators are widely in demand for many real-life applications. Considering that existing actuators based on polymers, low-dimensional materials and pore-rich materials are mostly limited by slow response rate, high driving voltage and poor stability, we report here a novel metal based flexible actuator which is fabricated simply through partial oxidation and nano-function of copper foil with the assistance of reduced graphene oxide. The obtained asymmetric metallic actuator is (electric-)thermally driven and exhibits fast response rate (∼2 s) and large curvature (2.4 cm-1) under a low voltage (∼1 V) with a sustainable operation of up to ∼50 000 cycles. The actuator can also be triggered by infrared irradiation and direct-heating under various conditions including air, water, and vacuum.

An Elastic Transparent Conductor Based on Hierarchically Wrinkled Reduced Graphene Oxide for Artificial Muscles and Sensors.

Using a 3D stretching method, a highly elastic reduced graphene oxide (rGO)/polyacrylic ester hierarchically wrinkled elastic transparent conductor (HWETC) is fabricated. Periodic hierarchical N-rGO layer wrinkling allows the HWETC to show high conductivity (100-457 Ω â—»-1 ) and transmittance (67-85%) under substantial stretching (>400%) and bending deformation (≈180°), which enables electrothermal actuation and strain sensing.

Origami-inspired active graphene-based paper for programmable instant self-folding walking devices.

Origami-inspired active graphene-based paper with programmed gradients in vertical and lateral directions is developed to address many of the limitations of polymer active materials including slow response and violent operation methods. Specifically, we used function-designed graphene oxide as nanoscale building blocks to fabricate an all-graphene self-folding paper that has a single-component gradient structure. A functional device composed of this graphene paper can (i) adopt predesigned shapes, (ii) walk, and (iii) turn a corner. These processes can be remote-controlled by gentle light or heating. We believe that this self-folding material holds potential for a wide range of applications such as sensing, artificial muscles, and robotics.

A multi-responsive water-driven actuator with instant and powerful performance for versatile applications.

Mechanical actuators driven by water that respond to multiple stimuli, exhibit fast responses and large deformations, and generate high stress have potential in artificial muscles, motors, and generators. Meeting all these requirements in a single device remains a challenge. We report a graphene monolayer paper that undergoes reversible deformation. Its graphene oxide cells wrinkle and extend in response to water desorption and absorption, respectively. Its fast (~0.3 s), powerful (>100 MPa output stress, 7.5 × 10(5) N kg(-1) unit mass force), and controllable actuation can be triggered by moisture, heat, and light. The graphene monolayer paper has potential in artificial muscles, robotic hands, and electromagnetic-free generators.

All-nanoparticle self-assembly ZnO/TiO2 heterojunction thin films with remarkably enhanced photoelectrochemical activity.

The multilaminated ZnO/TiO2 heterojunction films were successfully deposited on conductive substrates including fluorine-doped tin oxide (FTO) glass and flexible indium tin oxide coated poly(ethylene terephthalate) via the layer-by-layer (LBL) self assembly method from the oxide colloids without using any polyelectrolytes. The positively charged ZnO nanoparticles and the negatively charged TiO2 nanoparticles were directly used as the components in the consecutive deposition process to prepare the heterojunction thin films by varying the thicknesses. Moreover, the crystal growth of both oxides could be efficiently inhibited by the good connection between ZnO and TiO2 nanoparticles even after calcination at 500 °C, especially for ZnO which was able to keep the crystallite size under 25 nm. The as-prepared films were used as the working electrodes in the three-electrode photoelectrochemical cells. Because the well-contacted nanoscale heterojunctions were formed during the LBL self-assembling process, the ZnO/TiO2 all-nanoparticle films deposited on both substrates showed remarkably enhanced photoelectrochemical properties compared to that of the well-established TiO2 LBL thin films with similar thicknesses. The photocurrent response collected from the ZnO/TiO2 electrode on the FTO glass substrate was about five times higher than that collected from the TiO2 electrode. Owing to the absence of the insulating layer of dried polyelectrolytes, the ZnO/TiO2 all-nanoparticle heterojunction films were expected to be used in the photoelectrochemical device before calcination.