Transparent,stretchable, and rapid-response humidity sensor for body-attachable wearable electronics

Stretchable and conformal humidity sensors that can be attached to the human body for continuously monitoring the humidity of the environment around the human body or the moisture level of the human skin can play an important role in electronic skin and personal healthcare applications.However,most stretchable humidity sensors are based on the geometric engineering of non-stretchable components and only a few detailed studies are available on stretchable humidity sensors under applied mechanical deformations.In this paper,we propose a transparent,stretchable humidity sensor with a simple fabrication process,having intrinsically stretchable components that provide high stretchability,sensitivity,and stability along with fast response and relaxation time.Composed of reduced graphene oxide-polyurethane composites and an elastomeric conductive electrode,this device exhibits impressive response and relaxation time as fast as 3.5 and 7 s,respectively.The responsivity and the response and relaxation time of the device in the presence of humidity remain almost unchanged under stretching up to a strain of 60％ and after 10,000 stretching cycles at a 40％ strain.Further,these stretchable humidity sensors can be easily and conformally attached to a finger for monitoring the humidity levels of the environment around the human body,wet objects,or human skin.     

Multiscale Hierarchical Design of a Flexible Piezoresistive Pressure Sensor with High Sensitivity and Wide Linearity Range

Flexible piezoresistive pressure sensors have been attracting wide attention for applications in health monitoring and human‐machine interfaces because of their simple device structure and easy‐readout signals. For practical applications, flexible pressure sensors with both high sensitivity and wide linearity range are highly desirable. Herein, a simple and low‐cost method for the fabrication of a flexible piezoresistive pressure sensor with a hierarchical structure over large areas is presented. The piezoresistive pressure sensor consists of arrays of microscale papillae with nanoscale roughness produced by replicating the lotus leaf's surface and spray‐coating of graphene ink. Finite element analysis (FEA) shows that the hierarchical structure governs the deformation behavior and pressure distribution at the contact interface, leading to a quick and steady increase in contact area with loads. As a result, the piezoresistive pressure sensor demonstrates a high sensitivity of 1.2 kPa⁻¹ and a wide linearity range from 0 to 25 kPa. The flexible pressure sensor is applied for sensitive monitoring of small vibrations, including wrist pulse and acoustic waves. Moreover, a piezoresistive pressure sensor array is fabricated for mapping the spatial distribution of pressure. These results highlight the potential applications of the flexible piezoresistive pressure sensor for health monitoring and electronic skin.     

All‐Carbon Pressure Sensors with High Performance and Excellent Chemical Resistance

An all‐carbon pressure sensor is designed and fabricated based on reduced graphene oxide (rGO) nanomaterials. By sandwiching one layer of superelastic rGO aerogel between two freestanding high‐conductive rGO thin papers, the sensor works based on the contact resistance at the aerogel–paper interfaces, getting rid of the alien materials such as polymers and metals adopted in traditional sensors. Without the limitation of alien materials, the all‐carbon sensors demonstrate an ultrawide detecting range (0.72 Pa–130 kPa), low energy consumption (≈0.58 µW), ultrahigh sensitivity (349–253 kPa^?1) at low‐pressure regime (<1.4 Pa), fast response time (8 ms at 1 kPa), high stability (10 000 unloading–loading cycles between 0 and 1 kPa), light weight (<10 mg), easily scalable fabrication process, and excellent chemical stability. These merits enable them to detect real‐time human physiological signals and monitor the weights of various droplets of not only water but also hazardous chemical reagents including strong acid, strong alkali, and organic solvents. This shows their great potential applications in real‐time health monitoring, sport performance detecting, harsh environment‐related robotics and industry, and so forth.     

A New Strategy for Humidity Independent Oxide Chemiresistors: Dynamic Self‐Refreshing of In2O3 Sensing Surface Assisted by Layer‐by‐Layer Coated CeO2 Nanoclusters

The humidity dependence of the gas sensing characteristics of metal oxide semiconductors has been one of the greatest obstacles for gas sensor applications during the last five decades because ambient humidity dynamically changes with the environmental conditions. Herein, a new and novel strategy is reported to eliminate the humidity dependence of the gas sensing characteristics of oxide chemiresistors via dynamic self‐refreshing of the sensing surface affected by water vapor chemisorption. The sensor resistance and gas response of pure In₂O₃ hollow spheres significantly change and deteriorate in humid atmospheres. In contrast, the humidity dependence becomes negligible when an optimal concentration of CeO₂ nanoclusters is uniformly loaded onto In₂O₃ hollow spheres via layer‐by‐layer (LBL) assembly. Moreover, In₂O₃ sensors LBL‐coated with CeO₂ nanoclusters show fast response/recovery, low detection limit (500 ppb), and high selectivity to acetone even in highly humid conditions (relative humidity 80%). The mechanism underlying the dynamic refreshing of the In₂O₃ sensing surfaces regardless of humidity variation is investigated in relation to the role of CeO₂ and the chemical interaction among CeO₂, In₂O₃, and water vapor. This strategy can be widely used to design high performance gas sensors including disease diagnosis via breath analysis and pollutant monitoring.     

Transparent and Flexible Cellulose Nanocrystal/Reduced Graphene Oxide Film for Proximity Sensing

The rapid development of touch screens as well as photoelectric sensors has stimulated the fabrication of reliable, convenient, and human‐friendly devices. Other than sensors that detect physical touch or are based on pressure sensing, proximity sensors offer controlled sensibility without physical contact. In this work we present a transparent and eco‐friendly sensor made through layer‐by‐layer spraying of modified graphene oxide filled cellulose nanocrystals on lithographic patterns of interdigitated electrodes on polymer substrates, which help to realize the precise location of approaching objects. Stable and reproducible signals generated by keeping the finger in close proximity to the sensor can be controlled by humidity, temperature, and the distance and number of sprayed layers. The chemical modification and reduction of the graphene oxide/cellulose crystal composite and its excellent nanostructure enable the development of proximity sensors with faster response and higher sensitivity, the integration of which resolves nearly all of the technological issues imposed on optoelectronic sensing devices.     

Hybrid Films of Graphene and Carbon Nanotubes for High Performance Chemical and Temperature Sensing Applications

A hybrid composite material of graphene and carbon nanotube (CNT) for high performance chemical and temperature sensors is reported. Integration of 1D and 2D carbon materials into hybrid carbon composites is achieved by coupling graphene and CNT through poly(ionic liquid) (PIL) mediated‐hybridization. The resulting CNT/PIL/graphene hybrid materials are explored as active materials in chemical and temperature sensors. For chemical sensing application, the hybrid composite is integrated into a chemo‐resistive sensor to detect a general class of volatile organic compounds. Compared with the graphene‐only devices, the hybrid film device showed an improved performance with high sensitivity at ppm level, low detection limit, and fast signal response/recovery. To further demonstrate the potential of the hybrid films, a temperature sensor is fabricated. The CNT/PIL/graphene hybrid materials are highly responsive to small temperature gradient with fast response, high sensitivity, and stability, which may offer a new platform for the thermoelectric temperature sensors.     

Graphene‐Coated Spandex Sensors Embedded into Silicone Sheath for Composites Health Monitoring and Wearable Applications

This study presents a low‐cost, tunable, and stretchable sensor fabricated based on spandex (SpX) yarns coated with graphene nanoplatelets (GnP) through a dip‐coating process. The SpX/GnP is wrapped into a stretchable silicone rubber (SR) sheath to protect the conductive layer against harsh conditions, which allows for fabricating washable wearable sensors. Dip‐coating parameters are optimized to obtain the maximum GnP coating rate. The covering sheath is tailored to achieve high stretchability beyond the sensing limit of 104% for SpX/GnP/SR sensors. Adjustable sensitivity is attained by manipulating SpX immersion times broadening its application for a wide range of strains: Gauge factors as high as two orders of magnitude are achieved at tensile strains greater than ≈40%. The fabricated sensors are tested for two applications: First, the SpX/GnP sensors are integrated into composite fabrics (with no negative impact on the structural integrity of the part) for screening the yarn displacements, resin flow, solidification during the hot press forming process, and structural health monitoring under mechanical loads with minimal cross‐sensitivity to temperature/humidity. Second, the capability of SpX/GnP/SP sensors in detection of a wide range of bodily motions (from the joint motion to arterial blood pressure) is demonstrated.     

Nitrogen‐Doped Single Graphene Fiber with Platinum Water Dissociation Catalyst for Wearable Humidity Sensor

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 H₂(4%)/N₂(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.     

Flexible Smart Noncontact Control Systems with Ultrasensitive Humidity Sensors

The development of noncontact humidity sensors with high sensitivity, rapid response, and a facile fabrication process is urgently desired for advanced noncontact human–machine interaction (HMI) applications. Here, a flexible and transparent humidity sensor based on MoO₃ nanosheets is developed with a low‐cost and easily manufactured process. The designed humidity sensor exhibits ultrahigh sensitivity, fast response, great stability, and high selectivity, exceeding the state‐of‐the‐art humidity sensors. Furthermore, a wearable moisture analysis system is assembled for real‐time monitoring of ambient humidity and human breathing states. Benefiting from the sensitive and rapid response to fingertip humidity, the sensors are successfully applied to both a smart noncontact multistage switch and a novel flexible transparent noncontact screen for smart mobile devices, demonstrating the potential of the MoO₃ nanosheets‐based humidity sensors in future HMI systems.     

Direct Growth of Ultrafast Transparent Single‐Layer Graphene Defoggers

The idea flat surface, superb thermal conductivity and excellent optical transmittance of single‐layer graphene promise tremendous potential for graphene as a material for transparent defoggers. However, the resistance of defoggers made from conventional transferred graphene increases sharply once both sides of the film are covered by water molecules which, in turn, leads to a temperature drop that is inefficient for fog removal. Here, the direct growth of large‐area and continuous graphene films on quartz is reported, and the first practical single‐layer graphene defogger is fabricated. The advantages of this single‐layer graphene defogger lie in its ultrafast defogging time for relatively low input voltages and excellent defogging robustness. It can completely remove fog within 6 s when supplied a safe voltage of 32 V. No visible changes in the full defogging time after 50 defogging cycles are observed. This outstanding performance is attributed to the strong interaction forces between the graphene films and the substrates, which prevents the permeation of water molecules. These directly grown transparent graphene defoggers are expected to have excellent prospects in various applications such as anti‐fog glasses, auto window and mirror defogging.     

Microtopography‐Guided Conductive Patterns of Liquid‐Driven Graphene Nanoplatelet Networks for Stretchable and Skin‐Conformal Sensor Array

Flexible thin‐film sensors have been developed for practical uses in invasive or noninvasive cost‐effective healthcare devices, which requires high sensitivity, stretchability, biocompatibility, skin/organ‐conformity, and often transparency. Graphene nanoplatelets can be spontaneously assembled into transparent and conductive ultrathin coatings on micropatterned surfaces or planar substrates via a convective Marangoni force in a highly controlled manner. Based on this versatile graphene assembled film preparation, a thin, stretchable and skin‐conformal sensor array (144 pixels) is fabricated having microtopography‐guided, graphene‐based, conductive patterns embedded without any complicated processes. The electrically controlled sensor array for mapping spatial distributions (144 pixels) shows high sensitivity (maximum gauge factor ≈1697), skin‐like stretchability (<48%), high cyclic stability or durability (over 10⁵ cycles), and the signal amplification (≈5.25 times) via structure‐assisted intimate‐contacts between the device and rough skin. Furthermore, given the thin‐film programmable architecture and mechanical deformability of the sensor, a human skin‐conformal sensor is demonstrated with a wireless transmitter for expeditious diagnosis of cardiovascular and cardiac illnesses, which is capable of monitoring various amplified pulse‐waveforms and evolved into a mechanical/thermal‐sensitive electric rubber‐balloon and an electronic blood‐vessel. The microtopography‐guided and self‐assembled conductive patterns offer highly promising methodology and tool for next‐generation biomedical devices and various flexible/stretchable (wearable) devices.     

自供能柔性氧化石墨烯湿度传感器的喷墨印刷制备及性能研究

呼吸频率及呼吸模式检测可用于医疗诊断以及人体健康评估。传统的医学检测器件体积大、能耗高、使用不便捷。针对高性能、低成本、便携式电子产品的迫切需求, 本工作利用氧化石墨烯材料自发极化后对湿度敏感的特性, 通过喷墨印刷方法制备了一种可以实现自供能的平面型湿度传感器。所制备的传感器对湿度响应呈现为线性关系, 并且具有优异的灵敏度、快速响应和恢复特性、多次循环稳定性和长期老化稳定性等特性。基于该传感器可以实现对于人体呼吸频率和呼吸模式等的检测。制备的湿度传感器具有制作简单、成本低、不易受人体行动及外界环境干扰等优点, 适用于实时监测呼吸频率和呼吸模式。     

Hydrophobic ionic liquid-in-polymer composites for ultrafast,linear response and highly sensitive humidity sensing

Traditional ionic liquids are sensitive to humidity but with long response time and nonlinear response.Pure liquid-state ionic liquids are usually hard for dehydration which have ultralong response time for humidity sensing.The immobilization of ionic liquids provide a possible way for high performance humidity sensing.Hydrophobic materials and structures also promised faster response in humidity sensing,because of easier desorption of water.In this work,we prepared flexible humidity sensitive composites based on hydrophobic ionic liquid and polymer.The combination of hydrophobic ionic liquid with hydrophobic polymer realized linear response,high sensitivity with low hysteresis to humidity.By adjusting the ratio of ionic liquid,not only the impedance but also the hydrophobicity of composite could be modulated,which had a significant influence on the humidity sensing performance.The morphology and microstructure of the material also affected its interaction with water molecules.Due to the diverse processing methods of polymer,highly transparent film fabricated by spinning-coating and nanofibrous membrane fabricated by electrospinning could be prepared and exhibited different response time,which could be used for different application scenarios.Especially,the fibrous membrane made with electrospinning method showed an ultrafast response and could distinguish up to 120 Hz humidity change,due to its fibrous structure with high specific surface area.The humidity sensors with ultrafast,linear response and high sensitivity showed potential applications in human respiratory monitoring and flexible non-contact switch.To better show the multifunction of ionic liquid-polymer composite,as a proof of concept,we fabricated an integrated humidity sensitive color change device by utilizing lower ionic liquid content composite for sensing in the humidity sensing module and higher ionic liquid content composite as the electrolyte in the electrochromic module.     

Water Affinity to Epitaxial Graphene: The Impact of Layer Thickness

The sensitivity to water vapour of one‐, two‐, and three‐layer epitaxial graphene (1, 2, and 3LG) is examined in this study. It is unambiguously shown that graphene's response to water, as measured by changes in work function and carrier density, is dependent on its thickness, with 1LG being the most sensitive to water adsorption and environmental concentration changes. This is furthermore substantiated by surface adhesion measurements, which bring evidence that 1LG is less hydrophobic than 2LG. Yet, surprisingly, it is found that other contaminants commonly present in ambient air have a greater impact on graphene response than water vapor alone. This study indicates that graphene sensor design and calibration to minimize or discriminate the effect of the ambient, in which it is intended to operate, are necessary to insure the desired sensitivity and reliability of sensors. The present work will aid in developing models for realistic graphene sensors and establishing protocols for molecular sensor design and development.     

In-situ sugar-templated porous elastomer sensor with high sensitivity for wearables

Fabrication of elastic pressure sensors with low cost, high sensitivity, and mechanical durability is important for wearables, electronic skins and soft robotics. Here, we develop high-sensitivity porous elastomeric sensors for piezoresistive and capacitive pressure detection. Specifically, a porous polydimethylsiloxane (PDMS) sponge embedded with conductive fillers of carbon nanotubes (CNTs) or reduced graphene oxide (rGO) was fabricated by an in-situ sugar template strategy. The sensor demonstrates sensitive deformation to applied pressure, exhibiting large and fast response in resistance or capacitance for detection of a wide range of pressure (0‒5 kPa). PDMS, as a high-elasticity framework, enables creation of sensors with high sensitivity, excellent stability, and durability for long-term usage. The highest sensitivities of 22.1 and 68.3 kPa⁻¹ can be attained by devices with 5% CNTs and 4% rGO, respectively. The geometrics of the sponge sensor is tailorable using tableting technology for different applications. The sensors demonstrate finger motion detection and heart-rate monitoring in real-time, as well as a capacitive sensor array for identification of pressure and shape of placed objects, exhibiting good potential for wearables and human-machine interactions.     

Bioinspired Composite Microfibers for Skin Adhesion and Signal Amplification of Wearable Sensors

A facile approach is proposed for superior conformation and adhesion of wearable sensors to dry and wet skin. Bioinspired skin‐adhesive films are composed of elastomeric microfibers decorated with conformal and mushroom‐shaped vinylsiloxane tips. Strong skin adhesion is achieved by crosslinking the viscous vinylsiloxane tips directly on the skin surface. Furthermore, composite microfibrillar adhesive films possess a high adhesion strength of 18 kPa due to the excellent shape adaptation of the vinylsiloxane tips to the multiscale roughness of the skin. As a utility of the skin‐adhesive films in wearable‐device applications, they are integrated with wearable strain sensors for respiratory and heart‐rate monitoring. The signal‐to‐noise ratio of the strain sensor is significantly improved to 59.7 because of the considerable signal amplification of microfibrillar skin‐adhesive films.     

露点温度传感器发展趋势综述

介绍了目前露点温度传感器领域的研究现状,阐述了光学式、谐振式、电学式、热学式、重量式、化学式露点温度传感器的原理及构造,指出光学式露点温度传感器测量精度极高,其中冷镜式露点仪可作为湿度计量标准;谐振式露点温度传感器具有体积小、成本低、响应时间短、灵敏度高、可靠性好的特点;电学式露点温度传感器灵敏度高、功耗小,便于实现小型化、集成化;重量法是准确度最高的湿度绝对测量方法;化学法常用来测量低湿环境下的有机混合气体。探讨了露点温度传感器在环境监测、工业制造、医疗诊断等领域的应用情况,指出未来露点温度传感器将会向高精度、高稳定性、高响应的方向发展,且应用范围将进一步拓展,以满足极端环境下的测量需求。     

Palladium‐Decorated Silicon Nanomesh Fabricated by Nanosphere Lithography for High Performance,Room Temperature Hydrogen Sensing

A hydrogen (H₂) gas sensor based on a silicon (Si) nanomesh structure decorated with palladium (Pd) nanoparticles is fabricated via polystyrene nanosphere lithography and top‐down fabrication processes. The gas sensor shows dramatically improved H₂ gas sensitivity compared with an Si thin film sensor without nanopatterns. Furthermore, a buffered oxide etchant treatment of the Si nanomesh structure results in an additional performance improvement. The final sensor device shows fast H₂ response and high selectivity to H₂ gas among other gases. The sensing performance is stable and shows repeatable responses in both dry and high humidity ambient environments. The sensor also shows high stability without noticeable performance degradation after one month. This approach allows the facile fabrication of high performance H₂ sensors via a cost‐effective, complementary metal–oxide–semiconductor (CMOS) compatible, and scalable nanopatterning method.     

Extraordinarily Stretchable All‐Carbon Collaborative Nanoarchitectures for Epidermal Sensors

Multifunctional microelectronic components featuring large stretchability, high sensitivity, high signal‐to‐noise ratio (SNR), and broad sensing range have attracted a huge surge of interest with the fast developing epidermal electronic systems. Here, the epidermal sensors based on all‐carbon collaborative percolation network are demonstrated, which consist 3D graphene foam and carbon nanotubes (CNTs) obtained by two‐step chemical vapor deposition processes. The nanoscaled CNT networks largely enhance the stretchability and SNR of the 3D microarchitectural graphene foams, endowing the strain sensor with a gauge factor as high as 35, a wide reliable sensing range up to 85%, and excellent cyclic stability (>5000 cycles). The flexible and reversible strain sensor can be easily mounted on human skin as a wearable electronic device for real‐time and high accuracy detecting of electrophysiological stimuli and even for acoustic vibration recognition. The rationally designed all‐carbon nanoarchitectures are scalable, low cost, and promising in practical applications requiring extraordinary stretchability and ultrahigh SNRs.     

Chemical Preparation of Graphene‐Based Nanomaterials and Their Applications in Chemical and Biological Sensors

Graphene is a flat monolayer of carbon atoms packed tightly into a 2D honeycomb lattice that shows many intriguing properties meeting the key requirements for the implementation of highly excellent sensors, and all kinds of proof‐of‐concept sensors have been devised. To realize the potential sensor applications, the key is to synthesize graphene in a controlled way to achieve enhanced solution‐processing capabilities, and at the same time to maintain or even improve the intrinsic properties of graphene. Several production techniques for graphene‐based nanomaterials have been developed, ranging from the mechanical cleavage and chemical exfoliation of high‐quality graphene to direct growth onto different substrates and the chemical routes using graphite oxide as a precusor to the newly developed bottom‐up approach at the molecular level. The current review critically explores the recent progress on the chemical preparation of graphene‐based nanomaterials and their applications in sensors.