Self‐Organized Single‐Walled Carbon Nanotube Conducting Thin Films with Honeycomb Structures on Flexible Plastic Films

Complex 1, synthesized from anionic shortened single‐walled carbon nanotubes and cationic ammonium lipid dissolved in organic solvents, is cast on pretreated transparent flexible poly(ethylene terephthalate) (PET) films under a higher relative humidity to form thin films with self‐organized honeycomb structures. The cell sizes are controllable by changing the experimental conditions. The lipid, which is the cationic part of complex 1, is easily removed by a simple ion‐exchange method, while maintaining the basic honeycomb structures. After the ion exchange, the nanotube honeycomb films on PET with thinner skeletons exhibit a dramatic decrease in the surface resistivity from insulating to conducting. Carbon nanotubes with honeycomb structures formed by the self‐organization on flexible polymer films are useful in many areas of nanoscience and technology including nanomaterials, nanoelectronics, nanodevices, catalysts, sensors, and so on.     

Self‐Heating in Light‐Emitting Electrochemical Cells

Electroluminescent devices become warm during operation, and their performance can, therefore, be severely limited at high drive current density. Herein, the effects of this self‐heating on the operation of a light‐emitting electrochemical cell (LEC) are systematically studied. A drive current density of 50 mA cm^?2 can result in a local device temperature for a free‐standing LEC that exceeds 50 °C within a short period of operation, which in turn induces premature device degradation as manifested in the rapidly decreasing luminance and increasing voltage. Furthermore, this undesired self‐heating for a free‐standing thin‐film LEC can be suppressed by the employment of a device architecture featuring high thermal conductance and a small emission‐area fill factor, since the corresponding improved heat conduction to the nonemissive regions facilitates more efficient heat transfer to the ambient surroundings. In addition, the reported differences in performance between small‐area and large‐area LECs as well as between flexible‐plastic and rigid‐glass LECs are rationalized, culminating in insights that can be useful for the rational design of LEC devices with suppressed self‐heating and high performance.     

Room‐Temperature Self‐Healing and Recyclable Tough Polymer Composites Using Nitrogen‐Coordinated Boroxines

In this paper, nitrogen‐coordinated boroxines are exploited for the fabrication of self‐healing and recyclable polymer composites with enhanced mechanical properties. The 3D polymer networks cross‐linked with nitrogen‐coordinated boroxines are first synthesized through the trimerization of ortho‐aminomethyl‐phenylboronic acid groups at the terminals of poly(propylene glycol) (PPG) chains, and subsequently, the mechanically robust polymer composites are fabricated by utilizing the complexation of nitrogen‐coordinated boroxine‐containing PPG (N‐boroxine‐PPG) with poly(acrylic acid) (PAA) and hydrogen‐bonding interactions between them. The N‐boroxine‐PPG is soft with a tensile strength of 0.19 MPa, whereas the tensile strengths of N‐boroxine‐PPG/PAA composites can be tailored to range from 1.7 to 12.7 MPa by increasing the PAA contents in the polymer composites. It is revealed that the amine ligands can facilitate the formation and dissociation of nitrogen‐coordinated boroxines at room temperature. Moreover, the reversibility of nitrogen‐coordinated boroxines and hydrogen‐bonding interactions enable multiple cycles of healing and recycling of the damaged N‐boroxine‐PPG/PAA composites. The healed and recycled N‐boroxine‐PPG/PAA polymer composites regain most of their mechanical strength.     

Versatile,High‐Power,Flexible, Stretchable Carbon Nanotube Sheet Heating Elements Tolerant to Mechanical Damage and Severe Deformation

A macroscopic carbon nanotube (CNT) sheet‐based heating element having flexible, stretchable, and damage‐tolerant features, and wide applicability in harsh environments, is introduced. Because of the intrinsic connection of extremely flexible CNT bundles throughout the sample by van der Waals interactions without use of a binder, the electrical resistance variation of the CNT sheet on elastomer heating element as a function of strain is completely suppressed to some extent, even when stretched under up to 400% strain, which guarantees electrical stability under severe mechanical deformation. In addition, the spatial uniformity of the heat generated from the microaligned CNT bundles reduces the temperature variation inside the sample, which also guarantees thermal stability and operation at a higher average temperature. Such exceptional performance is achieved by the passivation of the elastomer layer on the CNT sheets. Furthermore, the mechanical robustness of this flexible, stretchable heating element is demonstrated by stable heater operation, even when the heating element is damaged. In addition, this design concept of CNT sheet on elastomer is extended to transparent flexible heaters and electric‐thermochromic windows.     

Photoconductive Hybrid Films via Directional Self‐Assembly of C60 on Aligned Carbon Nanotubes

Hybrid nanostructured materials can exhibit different properties than their constituent components, and can enable decoupled engineering of energy conversion and transport functions. Novel means of building hybrid assemblies of crystalline C₆₀ and carbon nanotubes (CNTs) are presented, wherein aligned CNT films direct the crystallization and orientation of C₆₀ rods from solution. In these hybrid films, the C₆₀ rods are oriented parallel to the direction of the CNTs throughout the thickness of the film. High‐resolution imaging shows that the crystals incorporate CNTs during growth, yet grazing‐incidence X‐ray diffraction (GIXD) shows that the crystal structure of the C₆₀ rods is not perturbed by the CNTs. Growth kinetics of the C₆₀ rods are enhanced 8‐fold on CNTs compared to bare Si, emphasizing the importance of the aligned, porous morphology of the CNT films as well as the selective surface interactions between C₆₀ and CNTs. Finally, it is shown how hybrid C₆₀–CNT films can be integrated electrically and employed as UV detectors with a high photoconductive gain and a responsivity of 10⁵ A W^?1 at low biases (± 0.5 V). The finding that CNTs can induce rapid, directional crystallization of molecules from solution may have broader implications to the science and applications of crystal growth, such as for inorganic nanocrystals, proteins, and synthetic polymers.     

Full Recovery of Fracture Toughness Using a Nontoxic Solvent‐Based Self‐Healing System

Two significant advances are reported for solvent‐based self‐healing of epoxy materials. First, an autonomic system yielding complete recovery of fracture toughness after crack propagation was achieved by embedding microcapsules containing a mixture of epoxy monomer and solvent into an epoxy matrix. Healing with epoxy‐solvent microcapsules is superior to capsules that contain solvent alone, and multiple healing events are reported for this system. Second, efficient healing is reported for new solvents, including aromatic esters, which are significantly less toxic than the previously employed solvent, chlorobenzene. Preliminary aging studies using either chlorobenzene or ethyl phenylacetate as the solvent demonstrate the stability of the epoxy‐solvent system under ambient conditions for at least one month.     

Self‐Healable and Recyclable Tactile Force Sensors with Post‐Tunable Sensitivity

It is challenging to post‐tune the sensitivity of a tactile force sensor. Herein, a facile method is reported to tailor the sensing properties of conductive polymer composites by utilizing the liquid‐like property of dynamic polymer matrix at low strain rates. The idea is demonstrated using dynamic polymer composites (CB/dPDMS) made via evaporation‐induced gelation of the suspending toluene solution of carbon black (CB) and acid‐catalyzed dynamic polydimethylsiloxane (dPDMS). The dPDMS matrices allow CB to redistribute to change the sensitivity of materials at the liquid‐like state, but exhibit typical solid‐like behavior and thus can be used as strain sensors at normal strain rates. It is shown that the gauge factor of the polymer composites can be easily post‐tuned from 1.4 to 51.5. In addition, the dynamic polymer matrices also endow the composites with interesting self‐healing ability and recyclability. Therefore, it is envisioned that this method can be useful in the design of various novel tactile sensing materials for many applications.     

Self‐Healing Materials for Energy‐Storage Devices

The booming development of electronics, electric vehicles, and grid storage stations has led to a high demand for advanced energy‐storage devices (ESDs) and accompanied attention to their reliability under various circumstances. Self‐healing is the ability of an organism to repair damage and restore function through its own internal vitality. Inspired by this, brilliant designs have emerged in recent years using self‐healing materials to significantly improve the lifespan, durability, and safety of ESDs. Extrinsic and intrinsic self‐healing materials and their working principles are first introduced. Then, the application of self‐healing materials in ESDs according to their self‐healing chemistry, including hydrogen bonds, electrostatic interactions, and borate ester bonds, are described in detail. Based on these, critical challenges and important future directions of self‐healing ESDs are discussed.     

Self‐Healing,Flexible, and Tailorable Triboelectric Nanogenerators for Self‐Powered Sensors based on Thermal Effect of Infrared Radiation

Self‐healing triboelectric nanogenerators (TENGs) with flexibility, robustness, and conformability are highly desirable for promising flexible and wearable devices, which can serve as a durable, stable, and renewable power supply, as well as a self‐powered sensor. Herein, an entirely self‐healing, flexible, and tailorable TENG is designed as a wearable sensor to monitor human motion, with infrared radiation from skin to promote self‐healing after being broken based on thermal effect of infrared radiation. Human skin is a natural infrared radiation emitter, providing favorable conditions for the device to function efficiently. The reversible imine bonds and quadruple hydrogen bonding (UPy) moieties are introduced into polymer networks to construct self‐healable electrification layer. UPy‐functionalized multiwalled carbon nanotubes are further incorporated into healable polymer to obtain conductive nanocomposite. Driven by the dynamic bonds, the designed and synthesized materials show excellent intrinsic self‐healing and shape‐tailorable features. Moreover, there is a robust interface bonding in the TENG devices due to the similar healable networks between electrification layer and electrode. The output electric performances of the self‐healable TENG devices can almost restore their original state when the damage of the devices occurs. This work presents a novel strategy for flexible devices, contributing to future sustainable energy and wearable electronics.     

Self‐Doping Fullerene Electrolyte‐Based Electron Transport Layer for All‐Room‐Temperature‐Processed High‐Performance Flexible Polymer Solar Cells

To achieve high‐performance large‐area flexible polymer solar cells (PSCs), one of the challenges is to develop new interface materials that possess a thermal‐annealing‐free process and thickness‐insensitive photovoltaic properties. Here, an n‐type self‐doping fullerene electrolyte, named PCBB‐3N‐3I, is developed as electron transporting layer (ETL) for the application in PSCs. PCBB‐3N‐3I ETL can be processed at room temperature, and shows excellent orthogonal solvent processability, substantially improved conductivity, and appropriate energy levels. PCBB‐3N‐3I ETL also functions as light‐harvesting acceptor in a bilayer solar cell, contributing to the overall device performance. As a result, the PCBB‐3N‐3I ETL‐based inverted PSCs with a PTB7‐Th:PC₇₁BM photoactive layer demonstrate an enhanced power conversion efficiency (PCE) of 10.62% for rigid and 10.04% for flexible devices. Moreover, the device avoids a thermal annealing process and the photovoltaic properties are insensitive to the thickness of PCBB‐3N‐3I ETL, yielding a PCE of 9.32% for the device with thick PCBB‐3N‐3I ETL (61 nm). To the best of one's knowledge, the above performance yields the highest efficiencies for the flexible PSCs and thick ETL‐based PSCs reported so far. Importantly, the flexible PSCs with PCBB‐3N‐3I ETL also show robust bending durability that could pave the way for the future development of high‐performance flexible solar cells.     

Double‐Twisted Conductive Smart Threads Comprising a Homogeneously and a Gradient‐Coated Thread for Multidimensional Flexible Pressure‐Sensing Devices

Fiber‐based, flexible pressure‐sensing systems have attracted attention recently due to their promising application as electronic skins. Here, a new kind of flexible pressure‐sensing device based on a polydimethylsiloxane membrane instrumented with double‐twisted smart threads (DTSTs) is reported. DTSTs are made of two conductive threads obtained by coating cotton threads with carbon nanotubes. One thread is coated with a homogeneous thickness of single‐walled carbon nanotubes (SWCNTs) to detect the intensity of an applied load and the other is coated with a graded thickness of SWCNTs to identify the position of the load along the thread. The mechanism and capacity of DTSTs to accurately sense an applied load are systematically analyzed. Results demonstrate that the fabricated 1D, 2D, and 3D sensing devices can be used to predict both the intensity and the position of an applied load. The sensors feature high sensitivity (between ≈0.1% and 1.56% kPa) and tunable resolution, good cycling resilience (>104 cycles), and a short response time (minimum 2.5 Hz). The presented strategy is a viable alternative for the design of simple, low‐cost pressure sensors.     

Self‐Protective Room‐Temperature Phosphorescence of Fluorine and Nitrogen Codoped Carbon Dots

The unstable triplet excited state is a core problem when developing self‐protective room temperature phosphorescence (RTP) in carbon dots (CDs). Here, fluorine and nitrogen codoped carbon dots (FNCDs) with long‐lived triplet excited states, emitting pH‐stabilized blue fluorescence and pH‐responsive green self‐protective RTP, are reported for the first time. The self‐protective RTP of FNCDs arises from n–π * electron transitions for C? N/C?N bonds with a small energy gap between singlet and triplet states at room temperature. Moreover, the interdot/intradot hydrogen bonds and steric protection of C? F bonds reduce quenching of RTP by oxygen at room temperature. The RTP emission of FNCDs shows outstanding reversibility, while the blue fluorescence emission has good pH stability. Based on these FNCDs, a data encoding/reading strategy for advanced anticounterfeiting is proposed via time‐resolved luminescence imaging techniques, as well as steganography of complex patterns.     

Boosting Photocurrent via Heating BiFeO3 Materials for Enhanced Self‐Powered UV Photodetectors

BiFeO₃ (BFO) is a potentially important Pb‐free ferroelectric with a narrow bandgap and is expected to become a novel photodetector. The photocurrent in BFO₃ strongly depends on the temperature but only a few studies have investigated in detail the relationships between photocurrent and temperature. Here, the temperature‐dependent photocurrent and the corresponding photosensing properties of a Ag/BFO/indiumtin oxide (ITO) photodetector based on an optimized planar‐structured electrode configuration are investigated. The photocurrent and responsivity of the BFO₃‐based photodetector can first be increased and then be decreased with increasing temperature. The largest photocurrent and responsivity can reach 51.5 µA and 6.56 × 10^?4 A W^?1 at 66.1 °C, which is enhanced 126.3% as compared with that at room temperature. This may be caused by the temperature‐modulated bandgap and barrier height in Ag/BFO/ITO device. This study clarifies the relationship between photosensing performance and the operating temperature of BFO‐based photodetector and will push forward the application of ferroelectric materials in photoelectric field.     

Self‐Assembled Robust Dipeptide Nanotubes and Fabrication of Dipeptide‐Capped Gold Nanoparticles on the Surface of these Nanotubes

Three water‐soluble dipeptides containing N‐terminally located β‐alanine residue and C‐terminally located α‐amino acid residues (β‐Ala‐L ‐Xaa, Xaa = Val/Ile/Phe) form robust crystalline nanotubes. These dipeptide nanotubes contain a common motif, a hybrid of β,α‐amino acids, which are stable against heat up to 80 °C, a wide range of pH (2–10), and proteolytic degradation. These robust crystalline dipeptide nanotubes are used as a template for fabricating dipeptide‐capped gold nanoparticles on their outer surfaces. This is an easy way to develop nanotube/nanoparticle hybrid materials under mild conditions.     

Acylhydrazones as Reversible Covalent Crosslinkers for Self‐Healing Polymers

The utilization of dynamic covalent and noncovalent bonds in polymeric materials offers the possibility to regenerate mechanical damage, inflicted on the material, and is therefore of great interest in the field of self‐healing materials. For the design of a new class of self‐healing materials, methacrylate containing copolymers with acylhydrazones as reversible covalent crosslinkers are utilized. The self‐healing polymer networks are obtained by a bulk polymerization of an acylhydrazone crosslinker and commercially available methacrylates as comonomers to fine‐tune the T_g of the systems. The influence of the amount of acylhydrazone crosslinker and the self‐healing behavior of the polymers is studied in detail. Furthermore, the basic healing mechanism and the corresponding mechanical properties are analyzed.     

Self‐Assembly of DNA‐Templated Polypyrrole Nanowires: Spontaneous Formation of Conductive Nanoropes

Polypyrrole nanowires formed by polymerization of pyrrole on a DNA template self‐assemble into rope‐like structures. These ‘nanoropes’ may be quite smooth (diameters 5–30 nm) or may show frayed ends where individual strands are visible. A combination of electric force microscopy, conductive atomic force microscopy and two‐terminal current–voltage measurements show that they are conductive. Nanoropes adhere more weakly to hydrophobic surfaces prepared by silanization of SiO₂ than to the clean oxide; this effect can be used to aid the combing of the nanoropes across microelectrode devices for electrical characterization.     

High‐Energy Asymmetric Supercapacitor Yarns for Self‐Charging Power Textiles

Rapid growth of electronic textile increases the demand for textile‐based power sources, which should have comparable lightweight, flexibility, and comfort. In this work, a self‐charging power textile interwoven by all‐yarn‐based energy‐harvesting triboelectric nanogenerators (TENG) and energy‐storing yarn‐type asymmetric supercapacitors (Y‐ASC) is reported. Common polyester yarns with conformal Ni/Cu coating are utilized as 1D current collectors in Y‐ASCs and electrodes in TENGs. The solid‐state Y‐ASC achieves high areal energy density (≈78.1 µWh cm^?2), high power density (14 mW cm^?2), stable cycling performance (82.7% for 5000 cycles), and excellent flexibility (1000 cycles bending for 180°). The TENG yarn can be woven into common fabrics with desired stylish designs to harvest energy from human daily motions at high output (≈60 V open‐circuit voltage and ≈3 µA short‐circuit current). The integrated self‐charging power textile is demonstrated to power an electronic watch without extra recharging by other power sources, suggesting its promising applications in electronic textiles and wearable electronics.     

A Low‐Cost,Self‐Standing NiCo2O4@CNT/CNT Multilayer Electrode for Flexible Asymmetric Solid‐State Supercapacitors

The demand for a new generation of flexible, portable, and high‐capacity power sources increases rapidly with the development of advanced wearable electronic devices. Here we report a simple process for large‐scale fabrication of self‐standing composite film electrodes composed of NiCo₂O₄@carbon nanotube (CNT) for supercapacitors. Among all composite electrodes prepared, the one fired in air displays the best electrochemical behavior, achieving a specific capacitance of 1,590 F g^?1 at 0.5 A g^?1 while maintaining excellent stability. The NiCo₂O₄@CNT/CNT film electrodes are fabricated via stacking NiCo₂O₄@CNT and CNT alternately through vacuum filtration. Lightweight, flexible, and self‐standing film electrodes (≈24.3 µm thick) exhibit high volumetric capacitance of 873 F cm^?3 (with an areal mass of 2.5 mg cm^?2) at 0.5 A g^?1. An all‐solid‐state asymmetric supercapacitor consists of a composite film electrode and a treated carbon cloth electrode has not only high energy density (≈27.6 Wh kg^?1) at 0.55 kW kg^?1 (including the weight of the two electrodes) but also excellent cycling stability (retaining ≈95% of the initial capacitance after 5000 cycles), demonstrating the potential for practical application in wearable devices.