For the development of wearable electronics, the replacement of rigid, metallic components with fully elastomeric materials is crucial. However, current elastomeric electrodes suffer from low electrical conductivity and poor electrical stability. Herein, a metal‐like conductive elastomer with exceptional electrical performance and stability is presented, which is used to fabricate fully elastomeric electronics. The key feature of this material is its wrinkled structure, which is induced by in situ cooperation of solvent swelling and densely packed nanoparticle assembly. Specifically, layer‐by‐layer assembly of metal nanoparticles and small‐molecule linkers on elastomers generates the hierarchical wrinkled elastomer. The elastomer demonstrates remarkable electrical conductivity (170 000 and 11 000 S cm−1 at 0% and 100% strain, respectively), outperforming previously reported elastomeric electrodes based on nanomaterials. Furthermore, a fully elastomeric triboelectric nanogenerator based on wrinkled elastomeric electrode exhibits excellent electric power generation performance due to the compressible, large contact area of the wrinkled surface during periodic contact and separation.
One of the most critical issues in preparing high-performance transparent supercapacitors (TSCs) is to overcome the trade-off between areal capacitance and optical transmittance as well as that between areal capacitance and rate capability. Herein, we introduce a TSC with high areal capacitance, fast rate capability, and good optical transparency by minimizing the charge transfer resistance between pseudocapacitive nanoparticles (NPs) using molecular linker-and conductive NPmediated layer-by-layer (LbL) assembly. For this study, bulky ligand-stabilized manganese oxide (MnO) and indium tin oxide (ITO) NP multilayers are LbL-assembled through a ligand exchange reaction between native ligands and small multidentate linkers (tricarballylic acid). The introduced molecular linker substantially decreases the separation distance between neighboring NPs, thereby reducing the contact resistance of electrodes. Moreover, the periodic insertion of ITO NPs into the MnO NP-based electrodes can lower the charge transfer resistance without a meaningful loss of transmittance, which can significantly improve the areal capacitance. The areal capacitances of the ITO NP-free electrode and the ITO NP-incorporated electrode are 24.6 mF cm −2 (at 61.6% transmittance) and 40.5 mF cm −2 (at 60.8%), respectively, which outperforms state of the art TSCs. Furthermore, we demonstrate a flexible symmetric solid-state TSC that exhibits scalable areal capacitance and optical transmittance.
Development of soft actuators with higher performance and more versatile controllability has been strongly required for further innovative advancement of various soft applications. Among various soft actuators, electrochemical actuators have attracted much attention due to their lightweight, simple device configuration, and facile low-voltage control. However, the reported performances have not been satisfactory because their working mechanism depends on the limited electrode expansion by conventional electrochemical reactions. Herein, we report an electroosmosis-driven hydrogel actuator with a fully soft monolithic structure-based whole-body actuation mechanism using an amphiphilic interaction-induced layer-by-layer assembly. For this study, cracked electrodes with interconnected metal nanoparticles are prepared on hydrogels through layer-by-layer assembly and shape transformation of metal nanoparticles at hydrophobic/hydrophilic solvent interfaces. Electroosmotic pumping by cracked electrodes instantaneously induces hydrogel swelling through reversible and substantial hydraulic flow. The resultant actuator exhibits actuation strain of higher than 20% and energy density of 1.06 × 105 J m–3, allowing various geometries (e.g., curved-planar and square-pillared structures) and motions (e.g., slow-relaxation, spring-out, and two degree of freedom bending). In particular, the energy density of our actuators shows about 10-fold improvement than those of skeletal muscle, electrochemical actuators, and various stimuli-responsive hydrogel actuators reported to date.
Hydrogels have diverse chemical properties and can exhibit reversibly large mechanical deformations in response to external stimuli; these characteristics suggest that hydrogels are promising materials for soft robots. However, reported actuators based on hydrogels generally suffer from slow response speed and/or poor controllability due to intrinsic material limitations and electrode fabrication technologies. Here, we report a hydrogel actuator that operates at low voltages (<3 volts) with high performance (strain > 50%, energy density > 7 × 10 5 joules per cubic meter, and power density > 3 × 10 4 watts per cubic meter), surpassing existing hydrogel actuators and other types of electroactive soft actuators. The enhanced performance of our actuator is due to the formation of wrinkled nanomembrane electrodes that exhibit high conductivity and excellent mechanical deformation through capillary-assisted assembly of metal nanoparticles and deswelling-induced wrinkled structures. By applying an electric potential through the wrinkled nanomembrane electrodes that sandwich the hydrogel, we were able to trigger a reversible and substantial electroosmotic water flow inside a hydrogel film, which drove the controlled swelling of the hydrogel. The high energy efficiency and power density of our wrinkled nanomembrane electrode–induced actuator enabled the fabrication of an untethered insect-scale aquabot integrated with an on-board control unit demonstrating maneuverability with fast locomotion speed (1.02 body length per second), which occupies only 2% of the total mass of the robot.
Electrical conductivity, mechanical flexibility, and large electroactive surface areas are the most important factors in determining the performance of various flexible electrodes in energy storage devices. Herein, a layer‐by‐layer (LbL) assembly‐induced metal electrodeposition approach is introduced to prepare a variety of highly porous 3D‐current collectors with high flexibility, metallic conductivity, and large surface area. In this study, a few metal nanoparticle (NP) layers are LbL‐assembled onto insulating paper for the preparation of conductive paper. Subsequent Ni electroplating of the metal NP‐coated substrates reduces the sheet resistance from ≈103 to <0.1 Ω sq−1 while maintaining the porous structure of the pristine paper. Particularly, this approach is completely compatible with commercial electroplating processes, and thus can be directly extended to electroplating applications using a variety of other metals in addition to Ni. After depositing high‐energy MnO NPs onto Ni‐electroplated papers, the areal capacitance increases from 68 to 811 mF cm−2 as the mass loading of MnO NPs increases from 0.16 to 4.31 mg cm−2. When metal NPs are periodically LbL‐assembled with the MnO NPs, the areal capacitance increases to 1710 mF cm−2.
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