Flexible,Stretchable, and Rechargeable Fiber‐Shaped Zinc–Air Battery Based on Cross‐Stacked Carbon Nanotube Sheets

The fabrication of flexible, stretchable and rechargeable devices with a high energy density is critical for next‐generation electronics. Herein, fiber‐shaped Zn–air batteries, are realized for the first time by designing aligned, cross‐stacked and porous carbon nanotube sheets simultaneously that behave as a gas diffusion layer, a catalyst layer, and a current collector. The combined remarkable electronic and mechanical properties of the aligned carbon nanotube sheets endow good electrochemical properties. They display excellent discharge and charge performances at a high current density of 2 A g⁻¹. They are also flexible and stretchable, which is particularly promising to power portable and wearable electronic devices.     

An All‐Solid‐State Fiber‐Shaped Aluminum–Air Battery with Flexibility,Stretchability, and High Electrochemical Performance

Owing to the high theoretical energy density of metal–air batteries, the aluminum–air battery has been proposed as a promising long‐term power supply for electronics. However, the available energy density from the aluminum–air battery is far from that anticipated and is limited by current electrode materials. Herein we described the creation of a new family of all‐solid‐state fiber‐shaped aluminum–air batteries with a specific capacity of 935 mAh g⁻¹ and an energy density of 1168 Wh kg⁻¹. The synthesis of an electrode composed of cross‐stacked aligned carbon‐nanotube/silver‐nanoparticle sheets contributes to the remarkable electrochemical performance. The fiber shape also provides the aluminum–air batteries with unique advantages; for example, they are flexible and stretchable and can be woven into a variety of textiles for large‐scale applications.     

An All‐Solid‐State Fiber‐Shaped Aluminum–Air Battery with Flexibility,Stretchability, and High Electrochemical Performance

Owing to the high theoretical energy density of metal–air batteries, the aluminum–air battery has been proposed as a promising long‐term power supply for electronics. However, the available energy density from the aluminum–air battery is far from that anticipated and is limited by current electrode materials. Herein we described the creation of a new family of all‐solid‐state fiber‐shaped aluminum–air batteries with a specific capacity of 935 mAh g^?1 and an energy density of 1168 Wh kg^?1. The synthesis of an electrode composed of cross‐stacked aligned carbon‐nanotube/silver‐nanoparticle sheets contributes to the remarkable electrochemical performance. The fiber shape also provides the aluminum–air batteries with unique advantages; for example, they are flexible and stretchable and can be woven into a variety of textiles for large‐scale applications.     

Elastic and Wearable Wire‐Shaped Lithium‐Ion Battery with High Electrochemical Performance

A stretchable wire‐shaped lithium‐ion battery is produced from two aligned multi‐walled carbon nanotube/lithium oxide composite yarns as the anode and cathode without extra current collectors and binders. The two composite yarns can be well paired to obtain a safe battery with superior electrochemical properties, such as energy densities of 27 Wh kg^?1 or 17.7 mWh cm^?3 and power densities of 880 W kg^?1 or 0.56 W cm^?3, which are an order of magnitude higher than the densities reported for lithium thin‐film batteries. These wire‐shaped batteries are flexible and light, and 97 % of their capacity was maintained after 1000 bending cycles. They are also very elastic as they are based on a modified spring structure, and 84 % of the capacity was maintained after stretching for 200 cycles at a strain of 100 %. Furthermore, these novel wire‐shaped batteries have been woven into lightweight, flexible, and stretchable battery textiles, which reveals possible large‐scale applications.     

Flexible and Stretchable Lithium‐Ion Batteries and Supercapacitors Based on Electrically Conducting Carbon Nanotube Fiber Springs

The construction of lightweight, flexible and stretchable power systems for modern electronic devices without using elastic polymer substrates is critical but remains challenging. We have developed a new and general strategy to produce both freestanding, stretchable, and flexible supercapacitors and lithium‐ion batteries with remarkable electrochemical properties by designing novel carbon nanotube fiber springs as electrodes. These springlike electrodes can be stretched by over 300 %. In addition, the supercapacitors and lithium‐ion batteries have a flexible fiber shape that enables promising applications in electronic textiles.     

Hybrid Fibers Made of Molybdenum Disulfide,Reduced Graphene Oxide,and Multi‐Walled Carbon Nanotubes for Solid‐State,Flexible, Asymmetric Supercapacitors

One of challenges existing in fiber‐based supercapacitors is how to achieve high energy density without compromising their rate stability. Owing to their unique physical, electronic, and electrochemical properties, two‐dimensional (2D) nanomaterials, e.g., molybdenum disulfide (MoS₂) and graphene, have attracted increasing research interest and been utilized as electrode materials in energy‐related applications. Herein, by incorporating MoS₂ and reduced graphene oxide (rGO) nanosheets into a well‐aligned multi‐walled carbon nanotube (MWCNT) sheet followed by twisting, MoS₂‐rGO/MWCNT and rGO/MWCNT fibers are fabricated, which can be used as the anode and cathode, respectively, for solid‐state, flexible, asymmetric supercapacitors. This fiber‐based asymmetric supercapacitor can operate in a wide potential window of 1.4 V with high Coulombic efficiency, good rate and cycling stability, and improved energy density.     

Hybrid Fibers Made of Molybdenum Disulfide,Reduced Graphene Oxide,and Multi‐Walled Carbon Nanotubes for Solid‐State,Flexible, Asymmetric Supercapacitors

One of challenges existing in fiber‐based supercapacitors is how to achieve high energy density without compromising their rate stability. Owing to their unique physical, electronic, and electrochemical properties, two‐dimensional (2D) nanomaterials, e.g., molybdenum disulfide (MoS₂) and graphene, have attracted increasing research interest and been utilized as electrode materials in energy‐related applications. Herein, by incorporating MoS₂ and reduced graphene oxide (rGO) nanosheets into a well‐aligned multi‐walled carbon nanotube (MWCNT) sheet followed by twisting, MoS₂‐rGO/MWCNT and rGO/MWCNT fibers are fabricated, which can be used as the anode and cathode, respectively, for solid‐state, flexible, asymmetric supercapacitors. This fiber‐based asymmetric supercapacitor can operate in a wide potential window of 1.4 V with high Coulombic efficiency, good rate and cycling stability, and improved energy density.     

A Lightweight Polymer Solar Cell Textile that Functions when Illuminated from Either Side

An all‐solid‐state, lightweight, flexible, and wearable polymer solar cell (PSC) textile with reasonable photovoltaic performance has been developed. A metal textile electrode made from micrometer‐sized metal wires is used as the cathode, and the surfaces of the metal wires are dip‐coated with the photoactive layers. Two ultrathin, transparent, and aligned carbon nanotube sheets that exhibit remarkable electronic and mechanical properties were coated onto the modified metal textile at both sides as the anode to produce the desired PSC textile. Because of the designed sandwich structure, the PSC textile displays the same energy conversion efficiencies regardless of which side it is irradiated from. As expected, the PSC textiles are highly flexible, and their energy conversion efficiencies varied by less than 3 % after bending for more than 200 cycles. The PSC textile shows an areal density (5.9 mg cm^?2) that is lower than that of flexible film‐based PSCs (31.3 mg cm^?2).     

High‐Performance,Stretchable, Wire‐Shaped Supercapacitors

A general approach toward extremely stretchable and highly conductive electrodes was developed. The method involves wrapping a continuous carbon nanotube (CNT) thin film around pre‐stretched elastic wires, from which high‐performance, stretchable wire‐shaped supercapacitors were fabricated. The supercapacitors were made by twisting two such CNT‐wrapped elastic wires, pre‐coated with poly(vinyl alcohol)/H₃PO₄ hydrogel, as the electrolyte and separator. The resultant wire‐shaped supercapacitors exhibited an extremely high elasticity of up to 350 % strain with a high device capacitance up to 30.7 F g⁻¹, which is two times that of the state‐of‐the‐art stretchable supercapacitor under only 100 % strain. The wire‐shaped structure facilitated the integration of multiple supercapacitors into a single wire device to meet specific energy and power needs for various potential applications. These supercapacitors can be repeatedly stretched from 0 to 200 % strain for hundreds of cycles with no change in performance, thus outperforming all the reported state‐of‐the‐art stretchable electronics.     

Aligned MoOx/MoS2 Core–Shell Nanotubular Structures with a High Density of Reactive Sites Based on Self‐Ordered Anodic Molybdenum Oxide Nanotubes

The present work demonstrates the self‐organized formation of anodic molybdenum oxide nanotube arrays. The amorphous tubes can be crystallized to MoO₂ or MoO₃ and be converted fully or partially into molybdenum sulfide. Vertically aligned MoO_x/MoS₂ nanotubes can be formed when, under optimized conditions, defined MoS₂ sheets form in a layer by layer arrangement that provide a high density of reactive stacking misalignments (defects). These core–shell nanotube arrays consist of a conductive suboxide core and a functional high defect density MoS₂ coating. Such structures are highly promising for applications in electrocatalysis (hydrogen evolution) or ion insertion devices.     

High‐Performance,Stretchable, Wire‐Shaped Supercapacitors

A general approach toward extremely stretchable and highly conductive electrodes was developed. The method involves wrapping a continuous carbon nanotube (CNT) thin film around pre‐stretched elastic wires, from which high‐performance, stretchable wire‐shaped supercapacitors were fabricated. The supercapacitors were made by twisting two such CNT‐wrapped elastic wires, pre‐coated with poly(vinyl alcohol)/H₃PO₄ hydrogel, as the electrolyte and separator. The resultant wire‐shaped supercapacitors exhibited an extremely high elasticity of up to 350 % strain with a high device capacitance up to 30.7 F g^?1, which is two times that of the state‐of‐the‐art stretchable supercapacitor under only 100 % strain. The wire‐shaped structure facilitated the integration of multiple supercapacitors into a single wire device to meet specific energy and power needs for various potential applications. These supercapacitors can be repeatedly stretched from 0 to 200 % strain for hundreds of cycles with no change in performance, thus outperforming all the reported state‐of‐the‐art stretchable electronics.     

A Self‐Healing Aqueous Lithium‐Ion Battery

Flexible lithium‐ion batteries are critical for the next‐generation electronics. However, during the practical application, they may break under deformations such as twisting and cutting, causing their failure to work or even serious safety problems. A new family of all‐solid‐state and flexible aqueous lithium ion batteries that can self‐heal after breaking has been created by designing aligned carbon nanotube sheets loaded with LiMn₂O₄ and LiTi₂(PO₄)₃ nanoparticles on a self‐healing polymer substrate as electrodes, and a new kind of lithium sulfate/sodium carboxymethylcellulose serves as both gel electrolyte and separator. The specific capacity, rate capability, and cycling performance can be well maintained after repeated cutting and self‐healing. These self‐healing batteries are demonstrated to be promising for wearable devices.     

A One‐Dimensional Fluidic Nanogenerator with a High Power Conversion Efficiency

Electricity generation from flowing water has been developed for over a century and plays a critical role in our lives. Generally, heavy and complex facilities are required for electricity generation, while using these technologies for applications that require a small size and high flexibility is difficult. Here, we developed a fluidic nanogenerator fiber from an aligned carbon nanotube sheet to generate electricity from any flowing water source in the environment as well as in the human body. The power conversion efficiency reached 23.3 %. The fluidic nanogenerator fiber was flexible and stretchable, and the high performance was well‐maintained after deformation over 1 000 000 cycles. The fiber also offered unique and promising advantages, such as the ability to be woven into fabrics for large‐scale applications.     

Realizing both High Energy and High Power Densities by Twisting Three Carbon‐Nanotube‐Based Hybrid Fibers

Energy storage devices, such as lithium‐ion batteries and supercapacitors, are required for the modern electronics. However, the intrinsic characteristics of low power densities in batteries and low energy densities in supercapacitors have limited their applications. How to simultaneously realize high energy and power densities in one device remains a challenge. Herein a fiber‐shaped hybrid energy‐storage device (FESD) formed by twisting three carbon nanotube hybrid fibers demonstrates both high energy and power densities. For the FESD, the energy density (50 mWh cm^?3 or 90 Wh kg^?1) many times higher than for other forms of supercapacitors and approximately 3 times that of thin‐film batteries; the power density (1 W cm^?3 or 5970 W kg^?1) is approximately 140 times of thin‐film lithium‐ion battery. The FESD is flexible, weaveable and wearable, which offers promising advantages in the modern electronics.     

A Self‐Standing and Flexible Electrode of Yolk–Shell CoS2 Spheres Encapsulated with Nitrogen‐Doped Graphene for High‐Performance Lithium‐Ion Batteries

Flexible lithium‐ion batteries (LIBs) have recently attracted increasing attention with the fast development of bendable electronic systems. Herein, a facile and template‐free solvothermal method is presented for the fabrication of hybrid yolk–shell CoS₂ and nitrogen‐doped graphene (NG) sheets. The yolk–shell architecture of CoS₂ encapsulated with NG coating is designed for the dual protection of CoS₂ to address the structural and interfacial stability concerns facing the CoS₂ anode. The as‐prepared composite can be assembled into a film, which can be used as a binder‐free and flexible electrode for LIBs that does not require any carbon black conducting additives or current collectors. When evaluating lithium‐storage properties, such a flexible electrode exhibits a high specific capacity of 992 mAh g^?1 in the first reversible discharge capacity at a current rate of 100 mA g^?1 and high reversible capacity of 882 mAh g^?1 after 150 cycles with excellent capacity retention of 89.91 %. Furthermore, a reversible capacity as high as 655 mAh g^?1 is still achieved after 50 cycles even at a high rate of 5 C due to the yolk–shell structure and NG coating, which not only provide short Li‐ion and electron pathways, but also accommodate large volume variation.     

Low‐cost Nickel Complex Dye‐sensitized Titania Nanoparticle/nanotube Composites for Solar Cells

In this work, high‐performance dye‐sensitized solar cells (DSSCs) based on new low‐cost visible nickel complex dye (VisDye), TiO₂ nanoparticle/nanotube composites electrodes, carbon nanoparticles counter electrodes, and ionic liquids electrolytes have been fabricated. The electronic structure, optical spectroscopy, and electrochemical properties of the VisDye were studied. Experimental results indicate that it is beneficial to improve the electron transport and power conversion efficiency using the nickel complex VisDye and TiO₂ nanoparticle/nanotube composites. Under optimized conditions, the solar energy conversion efficiencies were measured. The short‐circuit current density (J_SC), the open‐circuit voltage (V_OC), the fill factor (FF), and the overall efficiency (η) of the DSSCs are 10.01 mA/cm², 516 mV, 0.68, and 3.52%, respectively. This study demonstrates that the combination of new VisDye with TiO₂ nanoparticle/nanotube composites electrodes and carbon nanoparticles counter electrodes provide a way to fabricate highly efficient dye‐sensitized solar cells in low‐cost production.     

Photo‐aligning of polyimide layers for liquid crystals

A series of soluble and highly transparent semi‐alicyclic polyimides (PIs) with designed flexible linkages have been synthesized derived from an alicyclic aromatic dianhydride (1,2,3,4‐cyclobutanetetracarboxylic dianhydride, CBDA) and various aromatic ether‐bridged diamines. The semi‐alicyclic PIs were evaluated as the photo‐alignment layers of liquid crystal (LC) molecules in liquid crystal display (LCD). Experimental results indicate that the photo‐alignment characteristics of LC molecules induced by the photo‐aligned PI layers and the electro‐optical (EO) properties of the LC cell devices are closely related with PI backbone structures. The retardation of the photo‐aligned PI layers is correlated with the ultraviolet (UV) absorption intensity of PI at 220 to approximately 330 nm. The higher UV absorption intensity PI has, the higher retardation and lower pre‐tilt angle the photo‐aligned PI layer exhibits. The defect‐free and photo‐aligned PI layer could result into the uniform LC texture, which is highly desired for in‐plane switching (IPS) mode LCD devices. In comparison, PI layer containing trifluoromethyl moiety shows poor photo‐aligning performance because of the strong electronic withdrawing effect of the fluorinated linkage.     

Highly Stretchable Supercapacitors Based on Aligned Carbon Nanotube/Molybdenum Disulfide Composites

Stretchable supercapacitors that can sustain their performance under unpredictable tensile force are important elements for practical applications of various portable and wearable electronics. However, the stretchability of most reported supercapacitors was often lower than 100 % because of the limitation of the electrodes used. Herein we developed all‐solid‐state supercapacitors with a stretchability as high as 240 % by using aligned carbon nanotube composites with compact structure as electrodes. By combined with pseudocapacitive molybdenum disulfide nanosheets, the newly developed supercapacitor showed a specific capacitance of 13.16 F cm^?3, and also showed excellent cycling retention (98 %) after 10 000 charge–discharge cycles. This work also presents a general and effective approach in developing high‐performance electrodes for flexible and stretchable electronics.     

Integrating Perovskite Solar Cells into a Flexible Fiber

Perovskite solar cells have triggered a rapid development of new photovoltaic devices because of high energy conversion efficiencies and their all‐solid‐state structures. To this end, they are particularly useful for various wearable and portable electronic devices. Perovskite solar cells with a flexible fiber structure were now prepared for the first time by continuously winding an aligned multiwalled carbon nanotube sheet electrode onto a fiber electrode; photoactive perovskite materials were incorporated in between them through a solution process. The fiber‐shaped perovskite solar cell exhibits an energy conversion efficiency of 3.3 %, which remained stable on bending. The perovskite solar cell fibers may be woven into electronic textiles for large‐scale application by well‐developed textile technologies.     

Transparent Electrodes Printed with Nanocrystal Inks for Flexible Smart Devices

Transparent electrodes (TEs) are crucial in a wide range of modern electronic and optoelectronic devices. However, traditional TEs cannot meet the requirements of smart devices under development in unique fields, such as electronic skins, wearable electronics, robotic skins, flexible and stretchable displays, and solar cells. Emerging TEs printed with nanocrystal (NC) inks are inexpensive and compatible with solution processes, and have huge potential in flexible, stretchable, and wearable devices. Every development in ink‐based electrodes makes them more competitive for practical applications in various smart devices. Herein, we provide an overview of emergent ink‐based electrodes, such as transparent conducting oxides, metal nanowires, graphene, and carbon nanotubes, and their application in solution‐based flexible and stretchable devices.