Humidity sensors are essential components in wearable electronics for monitoring of environmental condition and physical state. In this work, a unique humidity sensing layer composed of nitrogen-doped reduced graphene oxide (nRGO) fiber on colorless polyimide film is proposed. Ultralong graphene oxide (GO) fibers are synthesized by solution assembly of large GO sheets assisted by lyotropic liquid crystal behavior. Chemical modification by nitrogen-doping is carried out under thermal annealing in H (4%)/N (96%) ambient to obtain highly conductive nRGO fiber. Very small (≈2 nm) Pt nanoparticles are tightly anchored on the surface of the nRGO fiber as water dissociation catalysts by an optical sintering process. As a result, nRGO fiber can effectively detect wide humidity levels in the range of 6.1-66.4% relative humidity (RH). Furthermore, a 1.36-fold higher sensitivity (4.51%) at 66.4% RH is achieved using a Pt functionalized nRGO fiber (i.e., Pt-nRGO fiber) compared with the sensitivity (3.53% at 66.4% RH) of pure nRGO fiber. Real-time and portable humidity sensing characteristics are successfully demonstrated toward exhaled breath using Pt-nRGO fiber integrated on a portable sensing module. The Pt-nRGO fiber with high sensitivity and wide range of humidity detection levels offers a new sensing platform for wearable humidity sensors.

Weavable sensing fibers with superior mechanical strength and sensing functionality are crucial for the realization of wearable textile sensors. However, in the fabrication of previously reported wearable sensing fibers, additional processes such as reduction, doping, and coating were essential to satisfy both requirements. The sensing fibers should be continuously synthesized in a scalable process for commercial applications with high reliability and productivity, which was challenging. In this study, we first synthesize mass-producible wearable sensing fibers with good mechanical properties and sensing functionality without additional processes by incorporating carbon nanotubes (CNTs) into distinct nanocellulose. Nanocellulose extracted from tunicate (TCNF) is homogeneously composited with single-walled CNTs, and composite fibers (TCNF/CNT) are continuously produced in aligned directions by wet spinning, facilitating liquid-crystal properties. The TCNF/CNT fibers exhibit a superior gas (NO 2 )-sensing performance with high selectivity and sensitivity (parts-per-billion detection). In addition, the TCNF/CNT fibers can endure complex and harsh distortions maintaining their intrinsic sensing properties and can be perfectly integrated with conventional fabrics using a direct weaving process. Our meter-scale scalable synthesis of functional composite fibers is expected to provide a mass production platform of versatile wearable sensors.

Inspired by mussel adhesive polydopamine (PDA), effective reinforcement of graphene-based liquid crystalline fibers to attain high mechanical and electrical properties simultaneously is presented. The two-step defect engineering, relying on bioinspired surface polymerization and subsequent solution infiltration of PDA, addresses the intrinsic limitation of graphene fibers arising from the folding and wrinkling of graphene layers during the fiber-spinning process. For a clear understanding of the mechanism of PDA-induced defect engineering, interfacial adhesion between graphene oxide sheets is straightforwardly analyzed by the atomic force microscopy pull-off test. Subsequently, PDA could be converted into an N-doped graphitic layer within the fiber structure by a mild thermal treatment such that mechanically strong fibers could be obtained without sacrificing electrical conductivity. Bioinspired graphene-based fiber holds great promise for a wide range of applications, including flexible electronics, multifunctional textiles, and wearable sensors.

Since carbon nanotube (CNT) fibers have a hierarchical structure, the specific strength of CNT fibers can be estimated to be much higher than its real value when the linear density of the fiber is measured using the vibroscopic method.

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The development of freestanding fiber-type chemiresistors, having high integration ability with various portable electronics including smart clothing systems, is highly demanding for the next-generation wearable sensing platforms. However, critical challenges stemming from the irreversible chemical sensing kinetics and weak reliability of the freestanding fiber-type chemiresistor hinder their practical use. In this work, for the first time, we report on the potential suitability of the freestanding and ultraporous reduced graphene oxide fiber functionalized with WO3 nanorods (porous WO3 NRs-RGO composite fiber) as a sensitive nitrogen dioxide (NO2) detector. By employing a tunicate cellulose nanofiber (TCNF), which is a unique animal-type cellulose, the numerous mesopores are formed on a wet-spun TCNF-GO composite fiber, unlike a bare GO fiber with dense surface structure. More interestingly, due to the superior wettability of TCNF, the aqueous tungsten precursor is uniformly adsorbed on an ultraporous TCNF-GO fiber, and subsequent heat treatment results in the thermal reduction of a TCNF-GO fiber and hierarchical growth of WO3 NRs perpendicular to the porous RGO fiber (porous WO3 NRs-RGO fiber). The freestanding porous WO3 NRs-RGO fiber shows a notable response to 1 ppm NO2. Furthermore, we successfully demonstrate reversible NO2 sensing characteristics of the porous WO3 NRs-RGO fiber, which is integrated on a wrist-type wearable sensing device.

Fiber-shaped supercapacitors (FSSCs) are the most state-of-the-art power supplies suitable for wearable devices, but the intrinsically limited cylindrical space of fibers restricts their high electrochemical performance, which must be overcome with a delicate and systematic architectural process. Here, a simple but effective 3D architectural strategy for fabricating FSSCs with high performance and flexibility is proposed. Highly conductive liquid crystal spun carbon nanotube fiber (CNTF) is an excellent 1D core fiber for the electrophoretic deposition of graphene oxide (GO). The deposited GO forms a vertical 3D structure on the CNTF (VG@CNTF), which can be successfully preserved by a consecutive coating of pseudocapacitive active materials onto the surface of VG. Notably, a solid-state asymmetric FSSC shows an outstanding performance of 65 Wh kg −1 at 100 kW kg −1 and exceptional stability and flexibility (capacitance retention of 98.60% at bending angles of 90° and 93.1% after 5000 bending cycles). This work can provide new insight into the development of high-performance FSSCs for practical wearable applications.