Sensing-transducing coupled piezoelectric textiles for self-powered humidity detection and wearable biomonitoring.

The performance of chemical sensors is dominated by the perception of the target molecules via sensitive materials and the conduction of sensing signals through transducers. However, sensing and transduction are spatially and temporally independent in most chemical sensors, which poses a challenge for device miniaturization and integration. Herein, we proposed a sensing-transducing coupled strategy by embedding the high piezoresponse Sm-PMN-PT ceramic (d33 = ∼1500 pC N-1) into a moisture-sensitive polyetherimide (PEI) polymer matrix via electrospinning to conjugate the humidity perception and signal transduction synchronously and sympatrically. Through phase-field simulation and experimental characterization, we reveal the principle of design of the composition and topological structure of sensing-transducing coupled piezoelectric (STP) textiles in order to modulate the recognition, conversion, and sensitive component utilization ratio of the prepared active humidity sensors, achieving high sensitivity (0.9%/RH%) and fast response (20 s) toward ambient moisture. The prepared STP textile can be worn on the human body to realize emotion recognition, exercise status monitoring, and physiological stress identification. This work offers unprecedented insights into the coupling mechanism between chemisorption-related interfacial state and energy conversion efficiency and opens up a new paradigm for developing autonomous, multifunctional and highly sensitive flexible chemical sensors.

Biodegradable cotton fiber-based piezoresistive textiles for wearable biomonitoring.

Electronic textiles are fundamentally changing the way we live. However, the inability to effectively recycle them is a considerable burden to the environment. In this study, we developed a cotton fiber-based piezoresistive textile (CF p-textile) for biomonitoring which is biocompatible, biodegradable, and environmentally friendly. These CF p-textiles were fabricated using a scalable dip-coating method to adhere MXene flakes to porous cotton cellulose fibers. The adhesion is made stronger by strong hydrogen bonding between MXene flakes and hierarchically porous cotton cellulose fibers. This cotton-fiber system provides a high sensitivity of 17.73 kPa-1 in a wide pressure range (100 Pa-30 kPa), a 2 Pa subtle pressure detection limit, fast response/recovery time (80/40 ms), and good cycle stability (over 5, 000 cycles). With its compelling sensing performance, the CF p-textile can detect various human biomechanical activities, including pulsation, muscle movement, and swallowing, while still being comfortable to wear. Moreover, the cotton cellulose is decomposed into low-molecular weight cellulose or glucose as a result of the 1,4-glycosidic bond breakage when exposed to acid or during natural degradation, which allows the electronic textile to be biodegradable. This work offers an ecologically-benign, cost-effective and facile approach to fabricating high-performance wearable bioelectronics.

Degradable MXene-Doped Polylactic Acid Textiles for Wearable Biomonitoring.

Degradable wearable electronics offer a promising route to construct sustainable cities and reduced carbon society. However, the difficult functionalization and the poor stability of degradable sensitive materials dramatically restrict their application in personalized healthcare assessment. Herein, we developed a scalable, low-cost, and porosity degradable MXene-polylactic acid textile (DMPT) for on-body biomonitoring via electrospinning. A combination of polydimethylsiloxane templating and MXene flake impregnation methods endows the fabricated DMPT with a sensitivity of 5.37/kPa, a fast response time of 98 ms, and a good mechanical stability (over 6000 cycles). An efficient degradation of as-electrospun DMPTs was observed in 1 wt % sodium carbonate solution. It is found that the incorporation of MXene nanosheets boosts the hydrophilicity and degradation efficiency of active polylactic acid nanofibrous films in comparison with the pristine counterpart. Furthermore, the as-received DMPT demonstrates great capability in monitoring physiological activities of wrist pulse, knuckle bending, swallowing, and vocalization. This work opens up a new paradigm for developing and optimizing high-performance degradable on-body electronics.

High-performance piezoelectric composites via ß phase programming.

Polymer-ceramic piezoelectric composites, combining high piezoelectricity and mechanical flexibility, have attracted increasing interest in both academia and industry. However, their piezoelectric activity is largely limited by intrinsically low crystallinity and weak spontaneous polarization. Here, we propose a Ti3C2Tx MXene anchoring method to manipulate the intermolecular interactions within the all-trans conformation of a polymer matrix. Employing phase-field simulation and molecular dynamics calculations, we show that OH surface terminations on the Ti3C2Tx nanosheets offer hydrogen bonding with the fluoropolymer matrix, leading to dipole alignment and enhanced net spontaneous polarization of the polymer-ceramic composites. We then translated this interfacial bonding strategy into electrospinning to boost the piezoelectric response of samarium doped Pb (Mg1/3Nb2/3)O3-PbTiO3/polyvinylidene fluoride composite nanofibers by 160% via Ti3C2Tx nanosheets inclusion. With excellent piezoelectric and mechanical attributes, the as-electrospun piezoelectric nanofibers can be easily integrated into the conventional shoe insoles to form a foot sensor network for all-around gait patterns monitoring, walking habits identification and Metatarsalgi prognosis. This work utilizes the interfacial coupling mechanism of intermolecular anchoring as a strategy to develop high-performance piezoelectric composites for wearable electronics.

Designing Cu2+ as a Partial Substitution of Protons in Polyaniline Emeraldine Salt: Room-Temperature-Recoverable H2S Sensing Properties and Mechanism Study.

Hydrogen sulfide (H2S) sensors are in urgent demand in the field of hermetic environment detection and metabolic disease diagnosis. However, most of the reported room-temperature (RT) H2S sensors based on transition metal oxides/salts unavoidably suffer from the poisoning effect, resulting in the unrecoverable behavior to restrain their application. Herein, copper(II) chloride-doped polyaniline emeraldine salt (PANI-CuCl2) was devised for RT-recoverable H2S detection, where the copper ion (Cu2+) was designed as a partial substitution of protons (H+) in PANI. The prepared gas sensor exhibited full recovery capability toward 0.25-10 ppm H2S, good repeatability, and long-term stability under 80% RH. Meanwhile, the changes of the PANI-CuCl2 during the H2S sensing period were analyzed via multiple analytical methods to reveal the reversible sensing behavior. Results showed that doping of Cu2+ not only promoted the PANI's response through the formation of conductive copper sulfide (CuS) and following H+ redoping in the PANI but also facilitated the sensor's recovery behavior because of the Cu2+ regeneration under the H+/oxygen environment. This work not only proves the changes of the interaction between the PANI and Cu2+ during the H2S sensing period but also sheds light on designing recoverable H2S sensors based on transition metal salts.

Optimizing Piezoelectric Nanocomposites by High-Throughput Phase-Field Simulation and Machine Learning.

Piezoelectric nanocomposites with oxide fillers in a polymer matrix combine the merit of high piezoelectric response of the oxides and flexibility as well as biocompatibility of the polymers. Understanding the role of the choice of materials and the filler-matrix architecture is critical to achieving desired functionality of a composite towards applications in flexible electronics and energy harvest devices. Herein, a high-throughput phase-field simulation is conducted to systematically reveal the influence of morphology and spatial orientation of an oxide filler on the piezoelectric, mechanical, and dielectric properties of the piezoelectric nanocomposites. It is discovered that with a constant filler volume fraction, a composite composed of vertical pillars exhibits superior piezoelectric response and electromechanical coupling coefficient as compared to the other geometric configurations. An analytical regression is established from a linear regression-based machine learning model, which can be employed to predict the performance of nanocomposites filled with oxides with a given set of piezoelectric coefficient, dielectric permittivity, and stiffness. This work not only sheds light on the fundamental mechanism of piezoelectric nanocomposites, but also offers a promising material design strategy for developing high-performance polymer/inorganic oxide composite-based wearable electronics.

MXene-Sponge Based High-Performance Piezoresistive Sensor for Wearable Biomonitoring and Real-Time Tactile Sensing.

Electrode microfabrication technologies such as lithography and deposition have been widely applied in wearable electronics to boost interfacial coupling efficiency and device performance. However, a majority of these approaches are restricted by expensive and complicated processing techniques, as well as waste discharge. Here, helium plasma irradiation is employed to yield a molybdenum microstructured electrode, which is constructed into a flexible piezoresistive pressure sensor based on a Ti3 C2 Tx nanosheet-immersed polyurethane sponge. This electrode engineering strategy enables the smooth transition between sponge deformation and MXene interlamellar displacement, giving rise to high sensitivity (1.52 kPa-1 ) and good linearity (r2  = 0.9985) in a wide sensing range (0-100 kPa) with a response time of 226 ms for pressure detection. In addition, both the experimental characterization and finite element simulation confirm that the hierarchical structures modulated by pore size, plasma bias, and MXene concentration play a crucial role in improving the sensing performance. Furthermore, the as-developed flexible pressure sensor is demonstrated to measure human radial pulse, detect finger tapping, foot stomping, and perform object identification, revealing great feasibility in wearable biomonitoring and health assessment.

Simultaneous Biomechanical and Biochemical Monitoring for Self-Powered Breath Analysis.

The high moisture level of exhaled gases unavoidably limits the sensitivity of breath analysis via wearable bioelectronics. Inspired by pulmonary lobe expansion/contraction observed during respiration, a respiration-driven triboelectric sensor (RTS) was devised for simultaneous respiratory biomechanical monitoring and exhaled acetone concentration analysis. A tin oxide-doped polyethyleneimine membrane was devised to play a dual role as both a triboelectric layer and an acetone sensing material. The prepared RTS exhibited excellent ability in measuring respiratory flow rate (2-8 L/min) and breath frequency (0.33-0.8 Hz). Furthermore, the RTS presented good performance in biochemical acetone sensing (2-10 ppm range at high moisture levels), which was validated via finite element analysis. This work has led to the development of a novel real-time active respiratory monitoring system and strengthened triboelectric-chemisorption coupling sensing mechanism.

NiWO4 Microflowers on Multi-Walled Carbon Nanotubes for High-Performance NH3 Detection.

NiWO4 microflowers with a large surface area up to 79.77 m2·g-1 are synthesized in situ via a facile coprecipitation method. The NiWO4 microflowers are further decorated with multi-walled carbon nanotubes (MWCNTs) and assembled to form composites for NH3 detection. The as-fabricated composite exhibits an excellent NH3 sensing response/recovery time (53 s/177 s) at a temperature of 460 °C, which is a 10-fold enhancement compared to that of pristine NiWO4. It also demonstrates a low detection limit of 50 ppm; the improved sensing performance is attributed to the porous structure of the material, the large specific surface area, and the p-n heterojunction formed between the MWNTs and NiWO4. The gas sensitivity of the sensor based on daisy-like NiWO4/MWCNTs shows that the sensor based on 10 mol % (MWN10) has the best gas sensitivity, with a sensitivity of 13.07 to 50 ppm NH3 at room temperature and a detection lower limit of 20 ppm. NH3, CO2, NO2, SO2, CO, and CH4 are used as typical target gases to construct the NiWO4/MWCNTs gas-sensitive material and study the research method combining density functional theory calculations and experiments. By calculating the morphology and structure of the gas-sensitive material NiWO4(110), the MWCNT load samples, the vacancy defects, and the influence law and internal mechanism of gas sensitivity were described.

Optimizing K0.5Na0.5NbO3 Single Crystal by Engineering Piezoelectric Anisotropy.

K0.5Na0.5NbO3 is considered as one of the most promising lead-free piezoelectric ceramics in the field of wearable electronics because of its excellent piezoelectric properties and environmental friendliness. In this work, the temperature-dependent longitudinal piezoelectric coefficient d33* was investigated in K0.5Na0.5NbO3 single crystals via the Landau-Ginzburg-Devonshire theory. Results show that the piezoelectric anisotropy varies with the temperature and the maximum of d33max* deviates from the polar direction of the ferroelectric phase. In the tetragonal phase, d33maxt* parallels with cubic polarization direction near the tetragonal-cubic transition region, and then gradually switches toward the nonpolar direction with decreasing temperatures. The maximum of d33o* in the orthorhombic phase reveals a distinct varying trend in different crystal planes. As for the rhombohedral phase, slight fluctuation of the maximum of d33r* was observed and delivered a more stable temperature-dependent maximum d33maxr* and its corresponding angle θmax in comparison with tetragonal and orthorhombic phases. This work not only sheds some light on the temperature-dependent phase transitions, but also paves the way for the optimization of piezoelectric properties in piezoelectric materials and devices.

Self-Powered Respiration Monitoring Enabled By a Triboelectric Nanogenerator.

In mammals, physiological respiration involves respiratory cycles of inhaled and exhaled breaths, which has traditionally been an underutilized resource potentially encompassing a wealth of physiologically relevant information as well as clues to potential diseases. Recently, triboelectric nanogenerators (TENGs) have been widely adopted for self-powered respiration monitoring owing to their compelling features, such as decent biocompatibility, wearing comfort, low-cost, and high sensitivity to respiration activities in the aspect of low frequency and slight amplitude body motions. Physiological respiration behaviors and exhaled chemical regents can be precisely and continuously monitored by TENG-based respiration sensors for personalized health care. This article presents an overview of TENG enabled self-powered respiration monitoring, with a focus on the working principle, sensing materials, functional structures, and related applications in both physical respiration motion detection and chemical breath analysis. Concepts and approaches for acquisition of physical information associated with respiratory rate and depth are covered in the first part. Then the sensing mechanism, theoretical modeling, and applications related to detection of chemicals released from breathing gases are systemically summarized. Finally, the opportunities and challenges of triboelectric effect enabled self-powered respiration monitoring are comprehensively discussed and criticized.

Dual Resistance and Impedance Investigation: Ultrasensitive and Stable Humidity Detection of Molybdenum Disulfide Nanosheet-Polyethylene Oxide Hybrids.

There is an imperative demand for real-time relative humidity (RH) discrimination with excellent sensitivity and robust operation stability over a broad RH range at room temperature (22 °C). Of diverse two-dimensional (2D) materials, p-type molybdenum disulfide (MoS2) as a typical gas-sensing candidate has been rarely harnessed for humidity detection due to tiny response and undesirable stability induced by the conversion from electron to proton conduction with increasing RH. To overcome these issues, MoS2-polyethylene oxide (PEO) inorganic-organic nanocomposites as the sensing layer were facilely prepared in this work. The results showed that the composition-optimized composite film sensor surpassed the isolated MoS2 counterpart in terms of repeatability, response, hysteresis, stability, and selectivity. Both DC-resistance and AC-impedance analyses unveiled different roles of MoS2 and PEO components within composites. MoS2 strengthened the film structure, while hydrophilic PEO enlarged the water-adsorption capacity and thus improved the response and detection reliability via water-triggered ionic conductivity. This work afforded a feasible strategy via inorganic-organic combination to distinguish trace RH and improved the operation stability of 2D material-based sensors, simultaneously demonstrating realistic monitoring applications of exhaled gas detection and distance variation of moisture-emitting objects.

Walking energy harvesting and self-powered tracking system based on triboelectric nanogenerators.

Due to the extensive energy consumption and high population density in modern cities, the collection and use of scattered walking energy from the stream of people is crucial for the development of a green ecological city. Herein, a flexible undulated electrode-based triboelectric nanogenerator (u-TENG) was integrated to the floor to scavenge walking energy from pedestrians, promoting the ordered collection of disordered and scattered energy. Driven by the steps of human walking, the output of the as-fabricated u-TENG are an open-circuit voltage of 86 V and a short-circuit current of 6.2 µA, which are able to continuously light up 110 light-emitting diode bulbs. In addition, a self-powered location-tracking system was prepared for pedestrian volume counting and passenger tracing with the purpose of reducing energy consumption in public areas. The proposed walking energy harvesting device is flexible, feasible, and unaffected by season, climate, or location. This work not only proposes a strategy for mechanical energy harvesting in public areas, including subway stations, hospitals, shopping malls, and business streets, but also offers a novel solution for smart cities and low-carbon transportation alternatives.

Surface Engineering of a 3D Topological Network for Ultrasensitive Piezoresistive Pressure Sensors.

Polypyrrole (PPy) is a good candidate material for piezoresistive pressure sensors owing to its excellent electrical conductivity and good biocompatibility. However, it remains challenging to fabricate PPy-based flexible piezoresistive pressure sensors with high sensitivity because of the intrinsic rigidity and brittleness of the film composed of dense PPy particles. Here, a rational structure, that is, 3D-conductive and elastic topological film composed of coaxial nanofiber networks, is reported to dramatically improve the sensitivity of flexible PPy-based sensors. The film is prepared through surface modification of electrospun polyvinylidene fluoride (PVDF) nanofibers by polydopamine (PDA), in order to homogeneously deposit PPy particles on the nanofiber networks with strong interfacial adhesion (PVDF/PDA/PPy, PPP). This unique structure has a high surface area and abundant contact sites, leading to superb sensitivity against a subtle pressure. The as-developed piezoresistive pressure sensor delivers a low limit of detection (0.9 Pa), high sensitivity (139.9 kPa-1), fast response (22 ms), good cycling stability (over 10,000 cycles), and reliability, thereby showing a promising value for applications in the fields of health monitoring and artificial intelligence.

Alveolus-Inspired Active Membrane Sensors for Self-Powered Wearable Chemical Sensing and Breath Analysis.

Fossil fuel internal combustion engines generate and release a huge amount of nitrogen dioxide, leading to respiratory and allergic diseases such as asthma, pneumonia, and possibly tuberculosis. Here we develop an alveolus-inspired membrane sensor (AIMS) for self-powered wearable nitrogen dioxide detection and personal physiological assessment. The bionic AIMS exhibits an excellent sensitivity up to 452.44%, a good linearity of 0.976, and superior selectivity under a NO2 concentration of 50 ppm. Furthermore, the AIMS can also be employed to diagnose human breath behaviors for breath analysis. The fundamental sensing mechanism is established using a combination of thermodynamic analysis, finite-element analysis, and phase-field simulations. It is found that the depolarization field inside the sensitive materials plays a crucial role in the self-powered gas-sensing performance. This work not only provides an efficient, low-cost, portable, and environmentally friendly means for active environmental assessment and personal biomonitoring but also provides a deep understanding of the gas-sensing mechanisms.

Enhanced Room Temperature NO2 Sensing Performance of RGO Nanosheets by Building RGO/SnO2 Nanocomposite System.

RGO/SnO 2 nanocomposites were prepared by a simple blending method and then airbrushed on interdigitated electrodes to obtain the corresponding gas sensors. The characterizations of SEM, TEM, Raman, XRD and FTIR were used to characterize the microstructures, morphologies and surface chemical compositions of the nanocomposites, indicating that the two materials coexist in the composite films and the concentration of surface defects is affected by the amount of SnO 2 nanoparticles. It is also found that the room temperature sensing performance of RGO to NO 2 can be improved by introducing appropriate amount of SnO 2 nanoparticles. The enhanced NO 2 sensing properties are attributed to the rough surface structure and increased surface area and surface defects of the nanocomposite films. Since further reduction of RGO, heat treating the sensing films resulted in a decrease in the response and recovery times of the sensors. Furthermore, the sensor annealed at 200 ∘ C exhibited a small baseline drift, wide detection range, good linearity, high stability and better selectivity.

Two-Sided Topological Architecture on a Monolithic Flexible Substrate for Ultrasensitive Strain Sensors.

Flexible ultrasensitive strain sensors are highly desirable in view of their widespread applications in wearable electronics, health monitoring systems, and smart robots, where subtle strain detection is required. However, traditional fabrication of such sensors was done to prepare sensitive layers on bare or single-sided structural substrates, leading to limited sensitivity. Herein, a stretchable resistive-type strain sensor was demonstrated by self-assembling conductive networks onto a monolithic polydimethylsiloxane substrate with a two-sided topological design, for example, a sinusoid/auxetic binary architecture. The sensitivity of the obtained sensor was greatly improved by 22-fold as compared to the traditional counterpart with a bare substrate. The remarkably good agreement between the experimental results and finite element analysis predictions confirmed that the superior sensitivity is a synergistic effect of local strain enhancement derived from the topological structure on the foreside and an additional strain concentration and a reduced Poisson's ratio from the auxetic arrays on the backside. Furthermore, this sensor can withstand an extreme mechanical force (>750 N) because of the shear stiffening characteristic of the auxetic structure. Benefiting from the characteristics of ultrahigh sensitivity (gauge factor ∼1744 at 5%), low detection limit (<0.05%), and long-term durability (>500 loading cycles), this as-prepared sensor shows promise in practical applications of high-performance wearable electronics.

Facile, Flexible, Cost-Saving, and Environment-Friendly Paper-Based Humidity Sensor for Multifunctional Applications.

Developing a facile, cost-saving, and environment-friendly method for fabricating a multifunctional humidity sensor is of great significance to expand its practical applications. However, most humidity sensors involve a complex fabrication process, resulting in their high cost and narrow application fields. Herein, a multifunctional paper-based humidity sensor with many advantages is proposed. This humidity sensor is fabricated using conventional printing paper and flexible conductive adhesive tape by a facile pasting method, in which the paper is used as both the humidity-sensing material and the substrate of the sensor. Owing to the moderate hydrophilicity of the paper and the rational structure design of the paper-based humidity sensor, the sensor exhibits an excellent humidity-sensing response of more than 103 as well as good linearity ( R2 = 0.9549) within the humidity range from 41.1 to 91.5% relative humidity. Furthermore, the paper-based humidity sensor has good flexibility and compatibility, endowing it with multifunctional applications for breath rate, baby diaper wetting, noncontact switch, skin humidity, and spatial localization monitoring. Although the resistance of the paper-based humidity sensor is relatively large, the humidity-sensing response signals of the sensor can be conveniently processed by the designed signal processing system. The readily available starting materials and facile fabrication technique provide useful strategies for the development of multifunctional humidity sensors.

A New Model and Its Application for the Dynamic Response of RGO Resistive Gas Sensor.

An reduced graphene oxide (RGO) resistive gas sensor was prepared to detect ammonia at room temperature, the result indicated that the desorption of gas (NH 3 ) molecules from a graphene-based sensor was difficult, which lead to a baseline drift. The responses of different concentrations were compared and studied. It was found that both the response rate and its acceleration were affected by the gas concentration. An Intermolecular Forces Based Model was established to explain the adsorption and desorption dynamic response curves. A new method was proposed based on this model. The first and second derivative extrema (FSDE) of the response curve can be attained quickly to calibrate the gas concentrations. The experiment results demonstrated that this new method could eliminate the baseline drift and was capable of increasing the efficiency of gas calibration significantly.

Ammonia gas sensors based on poly (3-hexylthiophene)-molybdenum disulfide film transistors.

In this work, in order to enhance the recovery performance of organic thin film transistors (OTFTs) ammonia (NH3) sensors, poly (3-hexylthiophene) (P3HT) and molybdenum disulfide (MoS2) were combined as sensitive materials. Different sensitive film structures as active layers of OTFTs, i.e., P3HT-MoS2 composite film, P3HT/MoS2 bilayer film and MoS2/P3HT bilayer film were fabricated by spray technology. OTFT gas sensors based on P3HT-MoS2 composite film showed a shorter recovery time than others when the ammonia concentration changed from 4 to 20 ppm. Specifically, x-ray diffraction (XRD), Raman and UV-visible absorption were employed to explore the interface properties between P3HT and single-layer MoS2. Through the complementary characterization, a mechanism based on charge transfer is proposed to explain the physical originality of these OTFT gas sensors: closer interlayer d-spacing and better π-π stacking of the P3HT chains in composite film have ensured a short recovery time of OTFT gas sensors. Moreover, sensing mechanisms of OTFTs were further studied by comparing the device performance in the presence of nitrogen or dry air as a carrier gas. This work not only strengthens the fundamental understanding of the sensing mechanism, but provides a promising approach to optimizing the OTFT gas sensors.