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The emerging two-dimensional (2D) materials have attracted explosive research interest, because of their unique properties and broad applications. However, the instability of typical 2D materials (...

Summary Electronic textile (E-textile) has drawn tremendous attention with the development of flexible and wearable electronics in recent years. Herein, we report the direct printing of E-textile composed of core-sheath fibers by employing a 3D printer equipped with a coaxial spinneret. Customer-designed core-sheath fiber-based patterns can be printed on textile for various purposes. For demonstration, we used carbon nanotubes (CNTs) as a conductive core and silk fibroin (SF) as a dielectric sheath, and fabricated a CNTs@SF core-sheath fiber-based smart pattern, which was further used as a triboelectricity nanogenerator textile. The smart textile could harvest biomechanical energy from human motion and achieve a power density as high as 18 mW/m2. We also demonstrated the printing of a supercapacitor textile for energy storage. The direct printing of smart patterns on textile may contribute to the large-scale production of self-sustainable E-textile with integrated electronics.

Protective clothing plays a vital role in safety and security. Traditional protective clothing can protect the human body from physical injury. It is highly desirable to integrate modern wearable electronics into a traditional protection suit to endow it with versatile smart functions. However, it is still challenging to integrate electronics into clothing through a practical approach while keeping the intrinsic flexibility and breathability of textiles. In this work, we realized the direct writing of laser-induced graphene (LIG) on a Kevlar textile in air and demonstrated the applications of the as-prepared Janus graphene/Kevlar textile in intelligent protective clothing. The C═O and N-C bonds in Kevlar were broken, and the remaining carbon atoms were reorganized into graphene, which can be ascribed to a photothermal effect induced by the laser irradiation. Proof-of-concept devices based on the prepared graphene/Kevlar textile, including flexible Zn-air batteries, electrocardiogram electrodes, and NO2 sensors, were demonstrated. Further, we fabricated self-powered and intelligent protective clothing based on the graphene/Kevlar textile. The laser-induced direct writing of graphene from commercial textiles in air conditions provides a versatile and rapid route for the fabrication of textile electronics.

Recently, wearable devices have been attracting significantly increased interest in human motion detection and human physiological signal monitoring. Currently, it is still a great challenge to fabricate strain sensors with high performance and good fit to the human body. In this work, we fabricated a close-fitting and wearable graphene textile strain sensor based on a graphene textile without polymer encapsulation. Graphene oxide acts as a colorant to dye the polyester fabric and is reduced at high temperature, which endows the graphene textile strain sensor with excellent performance. Compared with the previously reported strain sensors, our strain sensor exhibits a distinctive negative resistance variation with increasing strain. In addition, the sensor also demonstrates fascinating performance, including high sensitivity, long-term stability, and great comfort. Based on its superior performance, the graphene textile strain sensor can be knitted on clothing for detecting both subtle and large human motions, showing the tremendous potential for applications in wearable electronics.

Due to its excellent flexibility, graphene has an important application prospect in epidermal electronic sensors. However, there are drawbacks in current devices, such as sensitivity, range, lamination, and artistry. In this work, we have demonstrated a multilayer graphene epidermal electronic skin based on laser scribing graphene, whose patterns are programmable. A process has been developed to remove the unreduced graphene oxide. This method makes the epidermal electronic skin not only transferable to butterflies, human bodies, and any other objects inseparably and elegantly, merely with the assistance of water, but also have better sensitivity and stability. Therefore, pattern electronic skin could attach to every object like artwork. When packed in Ecoflex, electronic skin exhibits excellent performance, including ultrahigh sensitivity (gauge factor up to 673), large strain range (as high as 10%), and long-term stability. Therefore, many subtle physiological signals can be detected based on epidermal electronic skin with a single graphene line. Electronic skin with multiple graphene lines is employed to detect large-range human motion. To provide a deeper understanding of the resistance variation mechanism, a physical model is established to explain the relationship between the crack directions and electrical characteristics. These results show that graphene epidermal electronic skin has huge potential in health care and intelligent systems.

Stretchable and flexible supercapacitors are highly desired due to their many potential applications in wearable devices. However, it is challenging to fabricate supercapacitors that can withstand large tensile strain while maintaining high performance. Herein, we report an ultra-stretchable wire-shaped supercapacitor based on carbon nanotube@graphene@MnO2 fibers wound around a superelastic core fiber. The supercapacitor can sustain tensile strain up to 850%, which is the highest value reported for this type of device to date, while maintaining stable electrochemical performance. The energy density of the supercapacitor is 3.37 mWh·cm–3 at a power density of 54.0 mW·cm–3. The results show that 82% of the specific capacitance is retained after 1,000 stretch–release cycles with strains of 700%, demonstrating the superior durability of the elastic supercapacitor and showcasing its potential application in ultra-stretchable flexible electronics.

Natural energy haversting devices serve as an alternative candidate for power supply in many micro-/nano-systems. However, traditional nanogenerators based on piezoelectricity or triboelectric power generation face challenges in terms of biocompatibility and stability in various biological systems. The bacteriorhodopsin (bR) protein in Halobacterium halobium is an ideal biocompatible material for photoelectric conversion. Conventional bR systems based on ion transport or enhanced light absorption layers have a limited light power conversion speed. On the other hand, bR-based biohybrid devices have a great potential for sensitive light power conversion as compared to conventional nanogenerators. Herein, we present a biohybrid nanogenerator made of bR and horizontally aligned-long carbon nanotubes (CNTs) with electron–ion interaction for the first time for sensitive light power conversion. The bR layer serves as the proton pump, whereas CNTs are utilized to enhance the photocurrent; thus, the photocurrent frequency response improves significantly because of the effect of the electron–ion interaction. The photocurrent shows a linear relationship with the intensity of light and can still obtain a stable signal at a light intensity of 0.03 mW cm−2. With regard to the influence of the light on–off period, the photocurrent initially increases and then decreases with an increase in flickering frequency up to 360 Hz; this can be ascribed to the combinational influence of light switch speed and photocycle decay time. The photocurrent shows highest value (99 nA cm−2) at a frequency of about 50 Hz at a light intensity of 0.43 mW cm−2, which matches well with the frequency standard of the electrical power supply system. Moreover, we found that a higher density of CNTs contributed to improve performance of the nanogenerators. Furthermore, a H+ ion releasing model was proposed to interpret the operating mechanism of the biohybrid nanogenerator. The biohybrid nanogenerator shows great potential for applications as a power source for bio-nanosystems.

Flexible and wearable sensors have drawn extensive concern due to their wide potential applications in wearable electronics and intelligent robots. Flexible sensors with high sensitivity, good flexibility, and excellent stability are highly desirable for monitoring human biomedical signals, movements and the environment. The active materials and the device structures are the keys to achieve high performance. Carbon nanomaterials, including carbon nanotubes (CNTs), graphene, carbon black and carbon nanofibers, are one of the most commonly used active materials for the fabrication of high-performance flexible sensors due to their superior properties. Especially, CNTs and graphene can be assembled into various multi-scaled macroscopic structures, including one dimensional fibers, two dimensional films and three dimensional architectures, endowing the facile design of flexible sensors for wide practical applications. In addition, the hybrid structured carbon materials derived from natural bio-materials also showed a bright prospect for applications in flexible sensors. This review provides a comprehensive presentation of flexible and wearable sensors based on the above various carbon materials. Following a brief introduction of flexible sensors and carbon materials, the fundamentals of typical flexible sensors, such as strain sensors, pressure sensors, temperature sensors and humidity sensors, are presented. Then, the latest progress of flexible sensors based on carbon materials, including the fabrication processes, performance and applications, are summarized. Finally, the remaining major challenges of carbon-based flexible electronics are discussed and the future research directions are proposed.

The unique structure of a vertically aligned carbon nanotube (VACNT) array makes it behave most similarly to a blackbody. It is reported that the optical absorptivity of an extremely black VACNT array is about 0.98-0.99 over a large spectral range of 200 nm-200 μm, inspiring us to explore the performance of VACNT arrays in solar energy harvesting. In this work, we report the highly efficient steam generation simply by laminating a layer of VACNT array on the surface of water to harvest solar energy. It is found that under solar illumination the temperature of upper water can significantly increase with obvious water steam generated, indicating the efficient solar energy harvesting and local temperature rise by the thin layer of VACNTs. We found that the evaporation rate of water assisted by VACNT arrays is 10 times that of bare water, which is the highest ratio for solar-thermal-steam generation ever reported. Remarkably, the solar thermal conversion efficiency reached 90%. The excellent performance could be ascribed to the strong optical absorption and local temperature rise induced by the VACNT layer, as well as the ultrafast water transport through the VACNT layer due to the frictionless wall of CNTs. Based on the above, we further demonstrated the application of VACNT arrays in solar-driven desalination.

With the rapid development of wearable devices, flexible pressure sensors with high sensitivity and wide workable range are highly desired. In nature, there are many well-adapted structures developed through natural selection, which inspired us for the design of biomimetic materials or devices. Particularly, human fingertip skin, where many epidermal ridges amplify external stimulations, might be a good example to imitate for highly sensitive sensors. In this work, based on unique chemical vapor depositions (CVD)-grown 3D graphene films that mimic the morphology of fingertip skin, we fabricated flexible pressure sensing membranes, which simultaneously showed a high sensitivity of 110 (kPa)−1 for 0–0.2 kPa and wide workable pressure range (up to 75 kPa). Hierarchical structured PDMS films molded from natural leaves were used as the supporting elastic films for the graphene films, which also contribute to the superior performance of the pressure sensors. The pressure sensor showed a low detection limit (0.2 Pa), fast response (< 30 ms), and excellent stability for more than 10,000 loading/unloading cycles. Based on these features, we demonstrated its applications in detecting tiny objects, sound, and human physiological signals, showing its potential in wearable electronics for health monitoring and human/machine interfaces.

Graphene exhibits properties of atomic thickness, high transparency, and high carrier mobility, which is highly desirable for a flexible transparent conductive material. However, the electronic properties of large-area chemical vapor deposition grown graphene film suffer from insulated polymer contaminations introduced by the transfer process and the easily cracked nature. Here, we report a preparation method of a transfer-medium-free large-area nanofiber-reinforced graphene (a-PAN/G) film simply by annealing the electrostatically spun polyacrylonitrile (PAN) nanofibers on the graphene film. The film could be free-standing on water and suspended in air with high transparency and enhanced electrical and mechanical properties compared to that of a monolayer graphene film. The flexible transparent a-PAN/G films were demonstrated as active materials for sensitive pressure sensors. The obtained pressure sensors demonstrate high sensitivity (44.5 kPa-1 within 1.2 kPa), low operating voltage (0.01-0.5 V), and excellent stability for 5500 loading-unloading cycles, revealing promising potential applications in wearable electronics.

Silkworm silk is gaining significant attention from both the textile industry and research society because of its outstanding mechanical properties and lustrous appearance. The possibility of creating tougher silks attracts particular research interest. Carbon nanotubes and graphene are widely studied for their use as reinforcement. In this work, we report mechanically enhanced silk directly collected by feeding Bombyx mori larval silkworms with single-walled carbon nanotubes (SWNTs) and graphene. We found that parts of the fed carbon nanomaterials were incorporated into the as-spun silk fibers, whereas the others went into the excrement of silkworms. Spectroscopy study indicated that nanocarbon additions hindered the conformation transition of silk fibroin from random coil and α-helix to β-sheet, which may contribute to increased elongation at break and toughness modules. We further investigated the pyrolysis of modified silk, and a highly developed graphitic structure with obviously enhanced electrical conductivity was obtained through the introduction of SWNTs and graphene. The successful generation of these SWNT- or graphene-embedded silks by in vivo feeding is expected to open up possibilities for the large-scale production of high-strength silk fibers.

Silk is a widely available, edible, biocompatible, and environmentally sustainable natural material. Particulate matter (PM) pollution has drawn considerable attention because it is a serious threat to public health. Herein, we report a human-friendly silk nanofiber air filter, which exhibits superior filtration efficiency for both PM2.5 and submicron particles with obviously low pressure drop and low basis weight compared to typical commercial microfiber air filters. Additionally, other functions such as antibacterial activity could be easily integrated into the silk nanofiber air filters, enabling the fabrication of multifunctional air filters. All the above characteristics, combined with the natural abundance and biocompatibility of silk, suggest a great potential for the use of silk nanofibers as air filters, especially as comfortable and personal air purifiers.

This work presents a highly efficient and reliable strategy to grow horizontally aligned carbon nanotube (CNT) arrays on surfaces via preliminarily loading catalysts into the reactor. With the heat treatment before the growth of CNTs, the catalysts would migrate from the inner surface of the reactor to the surface of the targeted substrate to induce the growth of aligned CNTs. With this “in-situ catalyst loading” approach, aligned CNTs could be grown on different bare substrates, such as silicon, quartz and sapphire. The growth of CNTs could be repeated up to 50 times with reliable results via only one-time catalyst preloading process, avoiding the deposition of catalysts before each round of growth and the related randomicity, and thus benefiting the mass production of aligned CNT arrays on surfaces.

The development of nanomaterials has put forward high requirements for characterization techniques. Optical microscopy (OM), with easy accessibility and open operating spaces as compared to scanning electron microscopy, is a good choice to quickly locate materials and to be integrated with other equipment. However, OM is limited by its low resolution. Herein, we present a facile and non-destructive approach for optical observation of nanomaterials under conventional OMs with the aid of volatile nanoparticles (NPs), which can be deposited and removed in a controlled manner. The NPs deposited on the surface of nanomaterials render strong light scattering to enable the nanomaterials to become optically visible. For example, this approach enables the observation of individual carbon nanotubes (CNTs) with OMs at low magnification or even with the naked eye. Both supported CNTs on various substrates and suspended CNTs can be observed with this approach. Most importantly, the NPs can be completely removed through moderate heat treatment or laser irradiation, avoiding potential influence on the properties or subsequent applications of nanomaterials. Furthermore, we systematically investigate the deposition of various volatile NPs (up to 14 kinds) for the optical observation of nanomaterials. We also demonstrated the application of this approach on other nanomaterials, including nanowires and graphene. We showed that this approach is facile, controllable, non-destructive, and contamination-free, indicating wide potential applications.

Natural materials are often compositionally and structurally heterogeneous for realizing particular functions. Inspired by nature, researchers have designed hybrid materials that possess properties beyond each of the components. Particularly, it remains a great challenge to realize site‐specific anisotropy, which widely exists in natural materials and is responsible for unique mechanical properties as well as physiological behaviors. Herein, the spontaneous formation of aligned graphene oxide (GO) flakes in sodium alginate (SA) matrix with locally controlled orientation via a direct‐ink‐writing printing process is reported. The GO flakes are spontaneously aligned in the SA matrix by shear force when being extruded and then arranged horizontally after drying on the substrate, forming a brick‐and‐mortar structure that could anisotropically contract or expand upon activation by heat, light, or water. By designing the printing pathways directed by finite element analysis, the orientation of GO flakes in the composite is locally controlled, which could further guide the composite to transform into versatile architectures. Particularly, the transformation is reversible when water vapor is applied as one of the stimuli. As a proof of concept, complex morphing architectures are experimentally demonstrated, which are in good consistency with the simulation results., A multistimuli‐responsive composite with locally controlled texture that can be printed into programmable shape‐morphing architectures is presented. The printed structures show fast, reversible, and multistimuli‐responsive shape‐morphing toward heat, light, and water (liquid and vapor).

Silk has outstanding mechanical properties and biocompatibility. It has been used to fabricate traditional textiles for thousands of years and can be produced in large scale. Silk materials are potentially attractive in modern textile electronics. However, silk is not electrically conductive, thus limiting its applications in electronics. Moreover, regenerated silk is generally rigid and brittle, which hinder post processing. Here we report the fabrication of conductive silk wire in which carbon nanotube (CNT) yarns are wrapped with fluffy and flexible silk nanofiber films. The silk nanofiber film was prepared by electrospinning and then wrapped around a rotating CNT yarn in situ. The obtained silk-sheathed CNT (CNT@Silk) wire has an insulating sheath, which protects the body against electrical shock. In addition, the fabricated wires exhibit a high electrical conductivity (3.1 × 104 S/m), good mechanical strength (16 cN/tex), excellent flexibility, and high durability. More importantly, the wires have an...

3D graphene networks have shown extraordinary promise for high-performance electrochemical devices. Herein, the chemical vapor deposition synthesis of a highly porous 3D graphene foam (3D-GF) using naturally abundant calcined Iceland crystal as the template is reported. Intriguingly, the Iceland crystal transforms to CaO monolith with evenly distributed micro/meso/macropores through the releasing of CO2 at high temperature. Meanwhile, the hierarchical structure of the calcined template could be easily tuned under different calcination conditions. By precisely inheriting fine structure from the templates, the as-prepared 3D-GF possesses a tunable hierarchical porosity and low density. Thus, the hierarchical pores offer space for guest hybridization and provide an efficient pathway for ion/charge transport in typical energy conversion/storage systems. The 3D-GF skeleton electrode hybridized with Ni(OH)2 /Co(OH)2 through an optimal electrodeposition condition exhibits a high specific capacitance of 2922.2 F g-1 at a scan rate of 10 mV s-1 , and 2138.4 F g-1 at a discharge current density of 3.1 A g-1 . The hybrid 3D-GF symmetry supercapacitor shows a high energy density of 83.0 Wh kg-1 at a power density of 1011.3 W kg-1 and 31.4 Wh kg-1 at a high power density of 18 845.2 W kg-1 . The facile fabrication process enables the mass production of hierarchical porous 3D-GF for high-performance supercapacitors.

Recently, wearable pressure sensors have attracted tremendous attention because of their potential applications in monitoring physiological signals for human healthcare. Sensitivity and linearity are the two most essential parameters for pressure sensors. Although various designed micro/nanostructure morphologies have been introduced, the trade-off between sensitivity and linearity has not been well balanced. Human skin, which contains force receptors in a reticular layer, has a high sensitivity even for large external stimuli. Herein, inspired by the skin epidermis with high-performance force sensing, we have proposed a special surface morphology with spinosum microstructure of random distribution via the combination of an abrasive paper template and reduced graphene oxide. The sensitivity of the graphene pressure sensor with random distribution spinosum (RDS) microstructure is as high as 25.1 kPa–1 in a wide linearity range of 0–2.6 kPa. Our pressure sensor exhibits superior comprehensive properties com...

A three-dimensional carbon nanotube (CNT)/graphene hybrid material was synthesized by a two-step chemical vapor deposition (CVD) process. Due to the separated CVD processes for graphene and CNTs, the structures of the hybrid materials could be easily controlled. It is revealed that graphene film was tightly connected with one end of the CNT arrays, forming “jellyfish” structures. Moreover, our results indicate that the presence of graphene influenced the precipitation and growth rate of CNTs. The precipitation of CNTs was postponed due to the existence of graphene. However, the average growth rate of CNTs in the graphene region for the whole process was faster than that in the region without graphene.

There is a growing demand for flexible electronic devices. In particular, strain sensors with high performance have attracted more and more attention, because they can be attached on clothing or human skin for applications in the real-time monitoring of human activities. However, monitoring human-body motions that include both subtle and intensive motions, and many strain sensors cannot meet the diverse demands simultaneously. In this work, a silver nanoparticles (Ag NPs) bridged graphene strain sensor is developed for simultaneously detecting subtle and intensive human motions. Ag NPs serve as many bridges to connect the self-overlapping graphene sheets, which endows the strain sensor with many excellent performances. Because of the high sensitivity, with a large gauge factor (GF) of 475 and a strain range of >14.5%, high durability of the sensor has been achieved. Besides, the excellent consistency and repeatability of the fabrication process is verified. Furthermore, the model for explaining the working mechanism of the strain sensor is proposed. Most importantly, the designed wearable strain sensor can be applied in human motion detection, including large-scale motions and small-scale motions.

Tremendous progress has been made in the research of carbon nanotubes (CNTs) in the past 25 years, which has facilitated the progress and development of fundamental research and industrial applications. However, challenges and opportunities remain. At the same time, the discovery and development of graphene in 2004 has had an obvious impact on the applications of CNTs. The progress and development of CNTs provide valuable references for graphene, ranging from synthesis and characterization to applications. Promising materials combining CNTs and graphene are on the rise. The popularity of CNT/graphene hybrids has expanded research and application of carbon nanomaterials. In this chapter, we summarize the challenges and opportunities that exist in the synthesis and application of CNTs and describe the synthesis and application of CNT/graphene hybrid materials.

We report a facile graphene/graphite sheet assisted CVD process for the synthesis of high-areal-density HACNT arrays. Besides, some metal nanoparticles could eat the graphene/graphite sheets, forming serpentine holes on the sheets in the early stage, and finally leading to the precipitation of CNTs without an additional carbon source.

The rational design of high-performance flexible pressure sensors attracts attention because of the potential applications in wearable electronics and human–machine interfacing. For practical applications, pressure sensors with high sensitivity and low detection limit are desired. Here, ta simple process to fabricate high-performance pressure sensors based on biomimetic hierarchical structures and highly conductive active membranes is presented. Aligned carbon nanotubes/graphene (ACNT/G) is used as the active material and microstructured polydimethylsiloxane (m-PDMS) molded from natural leaves is used as the flexible matrix. The highly conductive ACNT/G films with unique coalescent structures, which are directly grown using chemical vapor deposition, can be conformably coated on the m-PDMS films with hierarchical protuberances. Flexible ACNT/G pressure sensors are then constructed by putting two ACNT/G/PDMS films face to face with the orientation of the ACNTs in the two films perpendicular to each other. Due to the unique hierarchical structures of both the ACNT/G and m-PDMS films, the obtained pressure sensors demonstrate high sensitivity (19.8 kPa−1

We report a systematic study of large-scale growth of high-quality WSe2 atomic layers directly on SiO2/Si substrates using a convenient method. Various parameters, especially growth temperatures, flow rate of carrier gas and tube pressure, are investigated in affecting the properties of as-grown WSe2 flakes in terms of their sizes, shapes and thickness. The pre-annealing step is demonstrated to be a key role in achieving the large-scale growth. Under an optimized condition, the lateral size of triangular single-crystal monolayer WSe2 is up to 30 [Formula: see text]m and the area of the monolayer thin film can be up to 0.25 mm2. And some other interesting features, such as nanoflowers, are observed, which are a promising for catalyzing research. Raman spectrum and microphotoluminescence indicate distinct layer dependent efficiency. Auger electron spectroscopy (AES) studies demonstrate the atomic concentration of the as-grown WSe2. Electrical transport further shows that the [Formula: see text]-type WSe2 field-effect transistors exhibit excellent electrical properties with carrier mobility of [Formula: see text][Formula: see text]64 cm[Formula: see text]V[Formula: see text]s[Formula: see text] and current on/off ratio over 105. These results are comparable to the exfoliated materials.

Graphene has unique water wetting properties, which have drawn great research interests recently. On the other side, water condensation and evaporation is a natural phenomenon in our daily life. Here, by combining the wetting properties of graphene and water condensation, a facile optical visualization approach is developed for graphene on a variety of substrates simply with the assistance of water vapor. Monolayer graphene becomes optically visible in several seconds with bellowing of water vapor. The wetting properties of monolayer graphene-covered surface and uncovered surface on various substrates, including copper, pristine silicon (Si), HF-treated Si, SiO2/Si, quartz, glass, polyethylene terephthalate (PET), polydimethylsiloxane (PDMS), and micropatterned PDMS, are studied. It is shown that graphene is visible when it is not fully transparent to wetting for the underlying substrates. The different wetting behavior of graphene-covered and uncovered surface leads to the difference in the distribution and morphology of water droplets, also gives rise to the interesting confining wall effect of the graphene edge, contributing to the observation of graphene. Moreover, this approach also enables distinguishing the monolayer and nonmonolayer graphene. This simple but powerful method is green, convenient, and repeatable, promising its great potential applications for graphene or other 2D materials.