Highly Aligned,Anisotropic Carbon Nanofiber Films for Multidirectional Strain Sensors with Exceptional Selectivity

Realization of sensing multidirectional strains is essential to understanding the nature of complex motions. Traditional uniaxial strain sensors lack the capability to detect motions working in different directions, limiting their applications in unconventional sensing technology areas, like sophisticated human–machine interface and real‐time monitoring of dynamic body movements. Herein, a stretchable multidirectional strain sensor is developed using highly aligned, anisotropic carbon nanofiber (ACNF) films via a facile, low‐cost, and scalable electrospinning approach. The fabricated strain sensor exhibits semitransparency, good stretchability of over 30%, outstanding durability for over 2500 cycles, and remarkable anisotropic strain sensing performance with maximum gauge factors of 180 and 0.3 for loads applied parallel and perpendicular to fiber alignment, respectively. Cross‐plied ACNF strain sensors are fabricated by orthogonally stacking two single‐layer ACNFs, which present a unique capability to distinguish the directions and magnitudes of strains with a remarkable selectivity of 3.84, highest among all stretchable multidirectional strain sensors reported so far. Their unconventional applications are demonstrated by detecting multi‐degrees‐of‐freedom synovial joint movements of the human body and monitoring wrist movements for systematic improvement of golf performance. The potential applications of novel multidirectional sensors reported here may shed new light into future development of next‐generation soft, flexible electronics.     

A Skin‐Inspired Integrated Sensor for Synchronous Monitoring of Multiparameter Signals

Electronic skins, as the integration of multiple distinct sensors, have aroused broad interests owing to their great potential in sensing applications. However, problems including the interference between sensing components and the difficulty in synchronous monitoring are practically encountered when they are applied to mixed signals. In this work, efforts are devoted to trouble‐free technical strategies for laminating three sensors with different sensing abilities into a skin‐like electronic device. The use of ionic liquid, combined with particular circuit topologies, ensures the reliable stability against mechanical disturbance during the real‐time sensing tests. The intrinsic layered structure and three independent sensing functions of natural skins are successfully presented by this particular device in which three sensors with the ease of preparation are spatially integrated. The changes of temperature, pressure, and infrared light can be recorded simultaneously yet without mutual signal interference. The perfect integration of multiple functional sensors into a single skin‐like device without any signal interference makes an important progress for pursuing the goal of future electronic skins that can practically be used as skin.     

Sensory Arrays of Covalently Functionalized Single‐Walled Carbon Nanotubes for Explosive Detection

Chemiresistive sensor arrays for cyclohexanone and nitromethane are fabricated using single‐walled carbon nanotubes (SWCNTs) that are covalently functionalized with urea, thiourea, and squaramide containing selector units. Based on initial sensing results and ¹H NMR binding studies, the most promising selectors are chosen and further optimized. These optimized selectors are attached to SWCNTs and simultaneously tested in a sensor array. The sensors show a very high level of reproducibility between measurements with the same sensor and across different sensors of the same type. Furthermore, the sensors show promising long‐term stability, which renders them suitable for practical applications.     

Rational Design of Nanostructured Electrode Materials toward Multifunctional Supercapacitors

As an intermediate step during energy usage, supercapacitors with superior power density, long‐term cycling stability, and moderate energy density have attracted immense interest as a facile route to use energy in a clean, efficient, and versatile manner in smart grid applications, as well as portable devices and other applications. Currently, the major drawback of supercapacitors is the low energy density. Electrode materials are the key components determining the cell performance. Great research efforts are made to develop nanostructured electrode materials with high performance. On the other hand, integrating supercapacitors with other applications have led to the emergence of many new types of multifunctional supercapacitors, which are attractive for a myriad of applications. The current understanding on charge/discharge mechanisms of electric double layer capacitors and pseudo‐capacitors is discussed along with recent development in designing nanostructured electrode materials by structure/morphology engineering, doping, and crystal structure controlling. Achievements in multifunctional supercapacitors like flexible supercapacitors, all‐solid‐state supercapacitors, self‐healing supercapacitors, electrochromic supercapacitors, self‐chargeable supercapacitors, and supercapacitors integrated with sensors are illustrated. Finally, opportunities and challenges in developing high performance and multifunctional supercapacitors are proposed.     

Graphene Paper Doped with Chemically Compatible Prussian Blue Nanoparticles as Nanohybrid Electrocatalyst

Along with reduced graphene oxide (RGO), water soluble Prussian blue nanoparticles (PBNPs, around 6 nm) are synthesized and broadly characterized. These two types of highly stable, low‐cost and chemically compatible nanomaterials are exploited as building ingredients to prepare electrically enhanced and functionally endorsed nanohybrid electrocatalysts, which are further transformed into free‐standing graphene papers. PBNPs doped graphene papers show highly efficient electrocatalysis towards reduction of hydrogen peroxide and can be used alone as flexible chemical sensors for potential applications in detection of hydrogen peroxide or/and other organic peroxides. The as‐prepared PBNPs–RGO papers are further capable of biocompatible accommodation of enzymes for development of free‐standing enzyme based biosensors. In this regard, glucose oxidase is used as an example for electrocatalytic oxidation and detection of glucose. The present work demonstrates a facile and highly reproducible way to construct free‐standing and flexible graphene paper doped with electroactive catalyst. Thanks to high stability, low‐cost and efficient electrocatalytic characteristics, this kind of nanohybrid material has potential to be produced on a large scale, and offers a broad range of possible applications, particularly in the fabrication of flexible sensing devices and as a platform for electrocatalytic energy conversion.     

Nanostructuring Platinum Nanoparticles on Multilayered Graphene Petal Nanosheets for Electrochemical Biosensing

Hybridization of nanoscale metals and carbon nanotubes into composite nanomaterials has produced some of the best‐performing sensors to date. The challenge remains to develop scalable nanofabrication methods that are amenable to the development of sensors with broad sensing ranges. A scalable nanostructured biosensor based on multilayered graphene petal nanosheets (MGPNs), Pt nanoparticles, and a biorecognition element (glucose oxidase) is presented. The combination of zero‐dimensional nanoparticles on a two‐dimensional support that is arrayed in the third dimension creates a sensor platform with exceptional characteristics. The versatility of the biosensor platform is demonstrated by altering biosensor performance (i.e., sensitivity, detection limit, and linear sensing range) through changing the size, density, and morphology of electrodeposited Pt nanoparticles on the MGPNs. This work enables a robust sensor design that demonstrates exceptional performance with enhanced glucose sensitivity (0.3 µM detection limit, 0.01–50 mM linear sensing range), a long stable shelf‐life (>1 month), and a high selectivity over electroactive, interfering species commonly found in human serum samples.     

Tuning the Composition and Nanostructure of Pt/Ir Films via Anodized Aluminum Oxide Templated Atomic Layer Deposition

Nanostructured metal films have been widely studied for their roles in sensing, catalysis, and energy storage. In this work, the synthesis of compositionally controlled and nanostructured Pt/Ir films by atomic layer deposition (ALD) into porous anodized aluminum oxide templates is demonstrated. Templated ALD provides advantages over alternative synthesis techniques, including improved film uniformity and conformality as well as atomic‐scale control over morphology and composition. Nanostructured Pt ALD films are demonstrated with morphological control provided by the Pt precursor exposure time and the number of ALD cycles. With these approaches, Pt films with enhanced surface areas, as characterized by roughness factors as large as 310, are reproducibly synthesized. Additionally, nanostructured PtIr alloy films of controlled composition and morphology are demonstrated by templated ALD, with compositions varying systematically from pure Pt to pure Ir. Lastly, the application of nanostructured Pt films to electrochemical sensing applications is demonstrated by the non‐enzymatic sensing of glucose.     

The Era of Digital Health: A Review of Portable and Wearable Affinity Biosensors

Digital health facilitated by wearable/portable electronics and big data analytics holds great potential in empowering patients with real‐time diagnostics tools and information. The detection of a majority of biomarkers at trace levels in body fluids using mobile health (mHealth) devices requires bioaffinity sensors that rely on “bioreceptors” for specific recognition. Portable point‐of‐care testing (POCT) bioaffinity sensors have demonstrated their broad utility for diverse applications ranging from health monitoring to disease diagnosis and management. In addition, flexible and stretchable electronics‐enabled wearable platforms have emerged in the past decade as an interesting approach in the ambulatory collection of real‐time data. Herein, the technological advancements of mHealth bioaffinity sensors evolved from laboratory assays to portable POCT devices, and to wearable electronics, are synthesized. The involved recognition events in the mHealth affinity biosensors enabled by bioreceptors (e.g., antibodies, DNAs, aptamers, and molecularly imprinted polymers) are discussed along with their transduction mechanisms (e.g., electrochemical and optical) and system‐level integration technologies. Finally, an outlook of the field is provided and key technological bottlenecks to overcome identified, in order to achieve a new sensing paradigm in wearable bioaffinity platforms.     

Synthesis and Characterization of a Composite Zeolite–Metglas Carbon Dioxide Sensor

The synthesis of a faujasite–Metglas composite material that can be used in gas‐sensing applications is presented. A continuous faujasite film was synthesized on a Metglas magnetoelastic strip using the secondary growth method. The ability of the new composite to remotely sense carbon dioxide in a nitrogen atmosphere at room temperature over a wide range of concentrations is demonstrated by monitoring the changes in the resonance frequency of the strip. The novel sensor combines the electromagnetic properties of the magnetoelastic material with the adsorption properties of the faujasite crystals. Experiments performed over a period of a few months showed that the composite sensor remained fully operational, thus indicating its long‐term stability. Furthermore, the present work demonstrates that a zeolite–Metglas composite can be used as a sensor of an analyte in a mixture as long as it adsorbs selectively larger amounts of the particular analyte than other compounds present in the mixture.     

Development of Film Sensors Based on Conjugated Polymers for Copper (II) Ion Detection

A fluorescent film sensor was prepared by chemical modification of a polyfluorene derivative on a glass‐plate surface. X‐ray photoelectron spectroscopy and ellipsometry measurements demonstrate the covalent attachment of the polyfluorene derivative to the glass‐plate surface. The sensor was used to detect Cu²⁺ ions in aqueous solution by a mechanism exploiting fluorescence quenching of conjugated polymers. Among the tested metal ions, the film sensor presents good selectivity towards Cu²⁺ ions. Further experiments show that the sensing process is reversible. Moreover, sensory microarrays based on conjugated polymers targeting Cu²⁺ ions are constructed, which display similar sensing performance to that of the film sensor. The structural motif in which conjugated polymers are covalently confined to a solid substrate surface offers several attractive advantages for sensing applications. First, in comparison with film sensors in which small fluorescent molecules are employed as sensing elements, the sensitivity of our new film sensor is enhanced due to the signal‐amplifying effect of the conjugated polymers. Second, the film sensors or microarrays can be used in aqueous environments, which is crucial for their potential use in a wide range of real‐world systems. Since the sensing process is reversible, the sensing materials can be reused. Third, unlike physically coated polymer chains, the covalent attachment of the grafted chains onto a material surface precludes desorption and imparts long‐term stability of the polymer chains.     

Organic Light‐Emitting Diode Sensing Platform: Challenges and Solutions

The organic light‐emitting diode (OLED)‐based sensing platform is gaining momentum due to unique attributes of the compact OLEDs that are used as excitation sources. This paper, however, points to issues related to this sensing platform that will affect many (bio)chemical sensing applications, in particular in photoluminescence (PL)‐based sensors operated in the advantageous time domain, where pulsed OLEDs are utilized. The issues are related to the post‐pulse electroluminescence (EL) profile, i.e., transient EL, which depends on the OLED materials and structure, and to the long‐wavelength tail of the typically broad‐band EL spectrum. Depending on materials and device structure, the transient EL may exhibit spikes peaking at ～100–200 ns and μs‐long tails. As shown, these interfere with the determination of PL decay times (that are related to analyte concentrations) of sensing elements. The results also indicate that the long‐wavelength tail of the EL spectrum contributes to the interfering post‐pulse μs‐long EL tail. Hence, it is shown that the choice of OLED materials, the use of microcavity (μC) OLEDs with tunable, narrower EL bands, and the use of UV OLEDs alleviate these issues, resulting in more reliable data analysis. Furthermore, a 2‐D uniform 2 μm‐pitch microlens array that was previously used for improving light extraction from the OLEDs (J.‐M. Park et al., Optics Express 2011 , 19, A786) is used for directional PL scattering toward the photodetector, which leads to a ～2.1–3.8 fold enhancement of the PL signal. This behavior is shown for oxygen sensing, which is the basis for sensing of bioanalytes such as glucose, lactate, ethanol, cholesterol, and uric acid.     

Self‐Healable Multifunctional Electronic Tattoos Based on Silk and Graphene

Electronic tattoos (E‐tattoos), which can be intimately mounted on human skin for noninvasive and high‐fidelity sensing, have attracted the attention of researchers in the field of wearable electronics. However, fabricating E‐tattoos that are capable of self‐healing and sensing multistimuli, similar to the inherent attributes of human skin, is still challenging. Herein, a healable and multifunctional E‐tattoo based on a graphene/silk fibroin/Ca²⁺ (Gr/SF/Ca²⁺) combination is reported. The highly flexible E‐tattoos are prepared through printing or writing using Gr/SF/Ca²⁺ suspension. The graphene flakes distributed in the matrix form an electrically conductive path that is responsive to environmental changes, such as strain, humidity, and temperature variations, endowing the E‐tattoo with high sensitivity to multistimuli. The performance of the E‐tattoo is investigated as a strain, humidity, and temperature sensor that shows high sensitivity, a fast response, and long‐term stability. The E‐tattoo is remarkably healed after damage by water because of the reformation of hydrogen and coordination bonds at the fractured interface. The healing efficiency is 100% in only 0.3 s. Finally, as proof of concept, its applications for monitoring of electrocardiograms, breathing, and temperature are shown. Based on its unique properties and superior performance, the Gr/SF/Ca²⁺ E‐tattoo may be a promising candidate material for epidermal electronics.     

Silicon Nanowire Sensors for Bioanalytical Applications: Glucose and Hydrogen Peroxide Detection

Silicon nanowire films have been modified with boron and used as sensors to measure glucose in aqueous solution. These sensors have a wide linear range (0–10 mM glucose), high sensitivity (172 nA mmol^–1), good reproducibility, and long‐term stability. Silicon nanowire films have also been modified with magnesium and shown to perform as sensors for detecting hydrogen peroxide in aqueous solution.     

Carbonized Cotton Fabric for High‐Performance Wearable Strain Sensors

Recent years have witnessed the booming development of flexible strain sensors. To date, it is still a great challenge to fabricate strain sensors with both large workable strain range and high sensitivity. Cotton is an abundant supplied natural material composed of cellulose fibers and has been widely used for textiles and clothing. In this work, the fabrication of highly sensitive wearable strain sensors based on commercial plain weave cotton fabric, which is the most popular fabric for clothes, is demonstrated through a low‐cost and scalable process. The strain sensors based on carbonized cotton fabric exhibit fascinating performance, including large workable strain range (>140%), superior sensitivity (gauge factor of 25 in strain of 0%–80% and that of 64 in strain of 80%–140%), inconspicuous drift, and long‐term stability, simultaneously offering advantages of low cost and simplicity in device fabrication and versatility in applications. Notably, the strain sensor can detect a subtle strain of as low as 0.02%. Based on its superior performance, its applications in monitoring both vigorous and subtle human motions are demonstrated, showing its tremendous potential for applications in wearable electronics and intelligent robots.     

Recent Advances in Sensing Applications of Graphene Assemblies and Their Composites

Development of next‐generation sensor devices is gaining tremendous attention in both academia and industry because of their broad applications in manufacturing processes, food and environment control, medicine, disease diagnostics, security and defense, aerospace, and so forth. Current challenges include the development of low‐cost, ultrahigh, and user‐friendly sensors, which have high selectivity, fast response and recovery times, and small dimensions. The critical demands of these new sensors are typically associated with advanced nanoscale sensing materials. Among them, graphene and its derivatives have demonstrated the ideal properties to overcome these challenges and have merged as one of the most popular sensing platforms for diverse applications. A broad range of graphene assemblies with different architectures, morphologies, and scales (from nano‐, micro‐, to macrosize) have been explored in recent years for designing new high‐performing sensing devices. Herein, this study presents and discusses recent advances in synthesis strategies of assembled graphene‐based superstructures of 1D, 2D, and 3D macroscopic shapes in the forms of fibers, thin films, and foams/aerogels. The fabricated state‐of‐the‐art applications of these materials in gas and vapor, biomedical, piezoresistive strain and pressure, heavy metal ion, and temperature sensors are also systematically reviewed and discussed, and their sensing performance is compared.     

Fully Flexible Electromagnetic Vibration Sensors with Annular Field Confinement Origami Magnetic Membranes

Sensing of mechanical motion based on flexible electromagnetic sensors is challenging due to the complexity of obtaining flexible magnetic membranes with confined and enhanced magnetic fields. A fully flexible electromechanical system (MEMS) sensor is developed to conduct wearable monitoring of mechanical displacement with excellent adaptability to complex surface morphology through a suspended flexible magnet enclosed within a novel setup formed by a multi‐layer flexible coil and annular origami magnetic membranes. The annular membranes not only regulate the overall distribution of the magnetic field and enhance the overall magnetism by 291%, but also greatly increase the range of the magnetic field to cover the entire region of the coil. The sensor offers a broad frequency response ranging from 1 Hz to 10 kHz and a sensitivity of 0.59 mV µm^?1 at 1.7 kHz. The fully flexible format of the sensor enables various applications demonstrated by biophysical sensing, motion detection, voice recognition, and machine diagnostics through direct attachment on soft and curvilinear surfaces. Similar sensors can combine multiple sensing and energy harvesting modalities to achieve battery‐less and self‐sustainable operation, and can be deployed in large numbers to conduct distributed sensing for machine status assessment, health monitoring, rehabilitation, and speech aid.     

Enhanced Performance of a ZnO Nanowire‐Based Self‐Powered Glucose Sensor by Piezotronic Effect

A self‐powered, piezotronic effect‐enhanced glucose sensor based on metal‐semiconductor‐metal (M–S–M) structured single ZnO nanowire device is demonstrated. A triboelectrical nanogenerator (TENG) is integrated to build a self‐powered glucose monitoring system (GMS) to realize the continuously monitoring of glucose concentrations. The performance of the glucose sensor is generally enhanced by the piezotronic effect when applying a –0.79% compressive strain on the device, and magnitude of the output signal is increased by more than 200%; the sensing resolution and sensitivity of sensors are improved by more than 200% and 300%, respectively. A theoretical model using energy band diagram is proposed to explain the observed results. This work demonstrates a promising approach to raise the sensitivity, improve the sensing resolution, and generally enhance the performance of glucose sensors, also providing a possible way to build up a self‐powered GMS.     

A Mediator‐Free Electroenzymatic Sensing Methodology to Mitigate Ionic and Electroactive Interferents' Effects for Reliable Wearable Metabolite and Nutrient Monitoring

Wearable electroenzymatic sensors enable monitoring of clinically informative biomolecules in epidermally retrievable biofluids. Conventional wearable enzymatic sensors utilize Prussian Blue (a redox mediator) to achieve selectivity against electroactive interferents. However, the use of Prussian Blue presents fundamental challenges including: 1) the susceptibility of the sensor response to dynamic concentration variation of ionic species and 2) the poor operational stability due to the degradation of its framework. As an alternative wearable electroenzymatic sensor development methodology to bypass the aforementioned limitations, a mediator‐free sensing interface is devised, comprising of a coupled platinum nanoparticle/multiwall carbon nanotube layer and a permselective membrane. The interface is adapted to develop sensors targeting glucose, lactate, and choline (as examples of informative metabolites and nutrients), showing high degrees of sensitivity, selectivity (against a wide panel of naturally present and diverse interfering species), stability (<6.5% signal drift over 20 h operation), and reliability of sensing operation in sweat samples. By integration within a readout board, a wireless sample‐to‐answer system is realized for on‐body sweat biomarker analysis. This methodology can be adapted to target a wide panel of biomarkers in various biofluids, introducing a new sensor development direction for personal health monitoring.     

Nanosensor Design Packages: A Smart and Compact Development for Metal Ions Sensing Responses

With recent advances in mesostructured materials and nanotechnologies, new methods are emerging to design optical sensors and biosensors, and to develop highly sensitive solid sensors. Here, highly sensitive, low cost, simple nanosensor designs for naked‐eye detection of toxic metal ions are successfully developed by the immobilization of commercially available α,β,γ,δ‐tetrakis(1‐methylpyridinium‐4‐yl)porphine p‐toluenesulfonate (TMPyP) and diphenylcarbazide (DPC), and chemically synthesized 4‐n‐dodecyl‐6‐(2‐thiazolylazo) resorcinol (DTAR) and 4‐n‐dodecyl‐6‐(2‐pyridylazo) phenol (DPAP) chromophore molecules into spherical nanosized cavities and surfaces. A rational strategy was crucial to develop optical nanosensors that can be used to control accurate recognition and signaling abilities of analyte species for ion‐sensing purposes. This is the first reported evidence of the significant key factors of the development of receptors as ‘indicator dyes' and surface‐confinement materials as ‘carriers' to broadening the applicability of optical chemical sensors for selective discrimination of trace levels of toxic analytes. In all the nanosensor design techniques presented here, a dense pattern of immobilized hydrophobic ‘neutral' and hydrophilic ‘charged' chromophores with intrinsic mobility, as a result of extremely robust constructed sequences on nanoscale structures, is a key to enhancing the sensing functionality of optical nanosensors. These nanosensor designs can be used as cage probe sinks with reliable control, for the first time, over the colorimetric recognition of cadmium ions to low levels of concentration in the range of 10^–9 to 10^–10 M . Optimization of control sensing conditions is established to achieve enhanced signal response and color intensities. These chemical nanosensors are reversible and have the potential to serve effectively in on‐site field analysis of environmental samples, which eliminates the necessity for instrument‐dependent analysis. Moreover, these new classes of optical cage sensors exhibit long‐term stability of signaling and recognition functionalities that in general provide extraordinary sensitivity, selectivity, reusability, and fast kinetic detection and quantification of various deleterious metal ions in our environment.     

Conducting‐Polymer Nanomaterials for High‐Performance Sensor Applications: Issues and Challenges

Owing to their promising applications in electronic and optoelectronic devices, conducting polymers have been continuously studied during the past few decades. Nevertheless, only limited progress had been made in conducting‐polymer‐based sensors until nanostructured conducting polymers were demonstrated for high‐performance signal transducers. Significant advances in the synthesis of conducting‐polymer nanomaterials have been recently reported, with enhanced sensitivity relative to their bulk counterparts. Today, conducting‐polymer nanomaterials rival metal and inorganic semiconductor nanomaterials in sensing capability. However, there are still several technological challenges to be solved for practical sensor applications of conducting‐polymer nanomaterials. Here, the key issues on conducting‐polymer nanomaterials in the development of state‐of‐the‐art sensors are discussed. Furthermore, a perspective on next‐generation sensor technology from a materials point of view is also given.