Article

Nanostrip Flexible Microwave Enzymatic Biosensor for Noninvasive Epidermal Glucose Sensing

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Abstract

Microwave sensors based on microstrip antennas are promising as wearable devices because of their flexibility and wireless communication compatibility. However, their sensitivity is limited due to the reduced sensor size and the potential of biochemical monitoring need to be explored. In this work, we present a new concept to enhance the microwave signals using of nanostrip-based metamaterials. The introduction of the nanostrip structures were achieved by theory and simulations. Experiments proof their enhancement to the electric field and sensing response in the characteristic gigahertz (GHz) wave band. Ordered nanostrips were fabricated on plastic substrate through simple nanoscale printing approach. Glucose oxidase is directly doped into the nanostrips, which enables a flexible wearable enzymatic biosensor for glucose sensing. Sensing experiments demonstrated that the nanostrip biosensor gives excellent performance for glucose detection, including high sensitivity, fast response, low detection limit, high affinity, and low power consumption. The applicability of the nanostrip-based sensor as wearable epidermal device for real-time noninvasive monitoring of glucose in sweat is verified as well.

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In this paper, we propose a humidity sensor based on a negative resistance oscillator using conducting polymer (CP) PEDOT:PSS film at room temperature. The proposed humidity sensor basically consists of a microstrip line and a negative resistance circuit, which creates a negative resistance for high-frequency oscillation. The microstrip line has a circuit structure that is connected through a via hole between the ground plane and the signal line with a CP thin film. From our experimental results, we find that the oscillation frequency of the sensor gradually decreases as the relative humidity (RH) increases. Owing to the conductivity variation of the CP film with the RH value, the oscillation frequency of the sensor sensitively changes in real time. Therefore, we suggest that our microwave-oscillator-based sensor scheme is a good candidate for the design of a robust and stable humidity sensor.
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Profuse medical information about cardiovascular properties can be gathered from pulse waveforms. Therefore, it is desirable to design a smart pulse monitoring device to achieve noninvasive and real-time acquisition of cardiovascular parameters. The majority of current pulse sensors are usually bulky or insufficient in sensitivity. In this work, a graphene-based skin-like sensor is explored for pulse wave sensing with features of easy use and wearing comfort. Moreover, the adjustment of the substrate stiffness and interfacial bonding accomplish the optimal balance between sensor linearity and signal sensitivity, as well as measurement of the beat-to-beat radial arterial pulse. Compared with the existing bulky and nonportable clinical instruments, this highly sensitive and soft sensing patch not only provides primary sensor interface to human skin, but also can objectively and accurately detect the subtle pulse signal variations in a real-time fashion, such as pulse waveforms with different ages, pre-and post-exercise, thus presenting a promising solution to home-based pulse monitoring.
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Wearable, flexible healthcare devices, which can monitor health data to predict and diagnose disease in advance, benefit society. Toward this future, various flexible and stretchable sensors as well as other components are demonstrated by arranging materials, structures, and processes. Although there are many sensor demonstrations, the fundamental characteristics such as the dependence of a temperature sensor on film thickness and the impact of adhesive for an electrocardiogram (ECG) sensor are yet to be explored in detail. In this study, the effect of film thickness for skin temperature measurements, adhesive force, and reliability of gel-less ECG sensors as well as an integrated real-time demonstration is reported. Depending on the ambient conditions, film thickness strongly affects the precision of skin temperature measurements, resulting in a thin flexible film suitable for a temperature sensor in wearable device applications. Furthermore, by arranging the material composition, stable gel-less sticky ECG electrodes are realized. Finally, real-time simultaneous skin temperature and ECG signal recordings are demonstrated by attaching an optimized device onto a volunteer's chest.
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This paper reports a surface functionalization strategy for protein detections based on biotin-derivatized poly(L-lysine)-grafted oligo-ethylene glycol (PLL-g-OEGx-Biotin) copolymers. Such strategy can be used to attach the biomolecule receptors in a reproducible way simply by incubation of the transducer element in a solution containing such copolymers which largely facilitated the sensor functionalization at an industrial scale. As the synthesized copolymers are cationic in physiology pH, surface biotinylation can be easily achieved via electrostatic adsorption on negatively charged sensor surface. Biotinylated receptors can be subsequently attached through well-defined biotin-streptavidin interaction. In this work, the bioactive sensor surfaces were applied for mouse IgG and prostate specific antigen (PSA) detections using quartz crystal microbalance (QCM), optical sensor (BioLayer Interferometry) and conventional ELISA test (colorimetry). A limit of detection (LOD) of 0.5 nM was achieved for PSA detections both in HEPES buffer and serum dilutions in ELISA tests. The synthesized PLL-g-OEGx-Biotin copolymers with different OEG chain length were also compared for their biosensing performance. Moreover, the surface regeneration was achieved by pH stimulation to remove the copolymers and the bonded analytes, while maintaining the sensor reusability as well. Thus, the developed PLL-g-OEGx-Biotin surface assembling strategy is believed to be a versatile surface coating method for protein detections with multi-sensor compatibility.
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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), <0.3 kPa), low detection limit (0.6 Pa), fast response time (<16.7 ms), low operating voltage (0.03 V), and excellent stability for more than 35 000 loading-unloading cycles, thus promising potential applications in wearable electronics.
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Composite nanofibers of Eu3+ doped poly(vinylidene fluoride-co-hexafluoropropylene) (P(VDFHFP))/graphene are prepared by the electrospinning technique for the fabrication of ultrasensitive wearable piezoelectric nanogenerators (WPNGs) where the post-poling technique is not necessary. It is found that the complete conversion of the piezoelectric β-phase and the improvement of the degree of crystallinity is governed by the incorporation of Eu3+ and graphene sheets into P(VDF-HFP) nanofibers. The flexible nanocomposite fibers are associated with a hypersensitive electronic transition that results in an intense red light emission, and WPNGs also have the capability of detecting external pressure as low as ~23 Pa with a higher degree of acoustic sensitivity, ~11 V Pa–1,than has ever been previously reported. This means that ultrasensitive WPNGs can be utilized to recognize human voices, which suggests they could be a potential tool in the biomedical and national security sectors. The capacitor’s ability to charge from abundant environmental vibrations, such as music, wind, body motion, etc, drives WPNGs as a power source for portable electronics. This fact may open up the prospect of using the Eu3+ doped P(VDF-HFP)/graphene composite electrospun nanofibers, with their multifunctional properties such as vibration sensitivity, wearability, red light emission capability and piezoelectric energy harvesting, for various promising applications in portable electronics,health care monitoring, noise detection and security monitoring.
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We demonstrate a wearable, flexible electrochemical biosensor for the combinatorial label-free detection of glucose in human sweat. The novel device comprises of stacked metal/metal-oxide (gold/zinc oxide) thin films within porous polyamide substrates for low-volume ultrasensitive impedance based detection of glucose and cortisol using non-faradaic electron-ionic charge transfer. In this work, we report the detection of glucose over a concentration range from 0.01–200 mg/dL spiked in synthetic and human sweat. Monoclonal antibodies specific to glucose oxidase were immobilized on thiolated ZnO sensing electrode surfaces resulting in the modulation of charge transfer within the electrical double layer (EDL). Non-Faradaic electrochemical impedance spectroscopy (EIS) was used to calibrate the sensor response with varying dose concentration through measurement of change in impedance. Reliable limit of detection (LOD) of 0.1 mg/dL in human sweat was demonstrated. Correlation of the sensor response with that of a commercial glucose meter TRUEresult™ Sensor (LOD of 20 mg/dL in blood) was found to be 0.9. Combinatorial detection of glucose and cortisol was demonstrated through frequency specific EIS measurements. Sensor variability was found to be within 15% of individual dynamic range for each molecule.
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We report on a bimetallic, bifunctional electrode where a platinum (Pt) surface was patterned with nanostructured gold (Au) fingers with different film thicknesses, which was functionalized with glucose oxidase (GOx) to yield a highly sensitive glucose biosensor. This was achieved by using selective adsorption of a self-assembled monolayer (SAM) onto Au fingers, which allowed GOx immobilization only onto the Au-SAM surface. This modified electrode was termed bifunctional because it allowed to simultaneously immobilize the biomolecule (GOx) on gold to catalyze glucose, and detect hydrogen peroxide on Pt sites. Optimized electrocatalytic activity was reached for the architecture Pt/Au-SAM/GOx with 50 nm thickness of Au, where synergy between Pt and Au allowed for detection of hydrogen peroxide (H2O2) at a low applied potential (0 V vs. Ag/AgCl). Detection was performed for H2O2 in the range between 4.7 and 102.7 nmol L–1, with detection limit of 3.4 × 10−9 mol L−1 (3.4 nmol L−1) and an apparent Michaelis-Menten rate constant of 3.2×10−6 mol L−1, which is considerably smaller than similar devices with monometallic electrodes. The methodology was validated by measuring glucose in artificial saliva, including in the presence of interferents. The synergy between Pt and Au was confirmed in electrochemical impedance spectroscopy measurements with an increased electron transfer, compared to bare Pt and Au electrodes. The approach for fabricating the reproducible bimetallic Pt/Au electrodes is entirely generic and may be explored for other types of biosensors and biodevices where advantage can be taken of the combination of the two metals.
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In this work, we present a clinical prototype with a wearable patient interface for microwave breast cancer detection. The long-term aim of the prototype is a breast health monitoring application. The system operates using multistatic time-domain pulsed radar, with 16 flexible antennas embedded into a bra. Unlike the previously reported, table-based prototype with a rigid cup-like holder, the wearable one requires no immersion medium and enables simple localization of breast surface. In comparison with the table-based prototype, the wearable one is also significantly more cost-effective and has a smaller footprint. To demonstrate the improved functionality of the wearable prototype, we here report the outcome of daily testing of the new, wearable prototype on a healthy volunteer over a 28-day period. The resulting data (both signals and reconstructed images) is compared to that obtained with our table-based prototype. We show that the use of the wearable prototype has improved the quality of collected volunteer data by every investigated measure. This work demonstrates the proof-of-concept for a wearable breast health monitoring array, which can be further optimized in the future for use with patients with various breast sizes and tissue densities.
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The generalized polynomial chaos theory is com-bined with a dedicated cavity model for curved textile antennas to statistically quantify variations in the antenna's resonance frequency under randomly varying bending conditions. The non-intrusive stochastic method solves the dispersion relation for the resonance frequencies of a set of radius of curvature realizations corresponding to the Gauss quadrature points belonging to the orthogonal polynomials having the probability density function of the random variable as a weighting function. The formalism is applied to different distributions for the radius of curvature, either using a priori known or on-the-fly constructed sets of orthogonal polynomials. Numerical and experimental validation shows that the new approach is at least as accurate as Monte Carlo simulations while being at least 100 times faster. This makes the method especially suited as a design tool to account for performance variability when textile antennas are deployed on persons with varying body morphology.
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In this study, a planar split-ring resonator (SRR)-based RF biosensor was developed for label-free detection of biomolecules such as the prostate cancer marker, prostate specific antigen (PSA), and cortisol stress hormone. The biosensor has a resonance-assisted transducer and is excited by a time-varying magnetic field component of a local high-impedance microstrip line. The resulting device exhibits an intrinsic S21 resonance with a quality-factor (or Q-factor) of 50. For the biomolecular interaction, anti-PSA and anti-cortisol were immobilized on the gold surface of the resonator by a protein-G mediated bioconjugation process and corresponding frequency shifts of Δf1p=30±2 MHz (for anti-PSA) and Δf1c=20±3 MHz (for anti-cortisol) were observed. The additional frequency shift of each PSA and cortisol antigen with a 100 pg/ml concentration was about 5 ± 1.5 MHz and 3 ± 1 MHz, respectively. From the experimental results, we confirmed that our device is very effective RF biosensor with a limit of detection (LOD) of 100 pg/ml and has sufficiently feasibility as a label-free biosensing scheme.
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Printed electronics promise various kinds of sensor circuit labels, for applications in distributed sensing and monitoring, which can be manufactured using traditional printing tools at very low cost. Elevated humidity levels or water leakages cause tremendous costs in our society, such as in construction industries and in transportations. Distributed monitoring and remote sensing of the humidity level inside walls of buildings and packages is therefore desired and urgently needed. Here, we report a wireless humidity sensor label that is manufactured using screen-printing and dry-phase patterning. The sensor label includes a planar antenna, a tuning capacitor and a printed sensor-capacitor head. Through electromagnetic coupling between a reader and the printed sensor label, changes in humidity level were remotely detected and read-out as a shift of the resonant frequency. The manufacturing process of the humidity sensor label is fully compatible with inexpensive, reel-to-reel processing technologies, thus enabling low cost production.
Article
We fabricated a series of gold nanowires/alumina composite films with different wire lengths. Optical transmission measurements confirmed that the composite films exhibit transverse and longitudinal surface plasmon resonances. We show that the wavelength of the longitudinal resonance is sensitive to nanowire length, while that of the transverse resonance is not. The experimental results are in agreement with the modeled results based on the Maxwell Garnett effective medium theory. Moreover, the window for negative refraction of the samples can be tuned in synchronism with the longitudinal resonance by the nanowire length.
Article
A novel microwave nondestructive evaluation (NDE) sensor was developed in an attempt to increase the sensitivity of the microwave NDE method for detection of material defects small relative to a wavelength. The sensor was designed on the basis of a negative index material (NIM) lens. Transmission at the resonant frequency through the 1-D lens was determined to be about 10 times higher than that with the 2-D lens. However, the focusing ability of the 1-D lens was found to be slightly lower to the 2-D lens (focus spot size for the 1-D lens was determined to be 0.7λ vs. 0.48λ for the 2-D lens). A fiberglass material sample with a 3mm (0.037λ) diameter through hole (perpendicular to the propagation direction of the wave) was tested with both lenses. The hole was successfully detected with an 8.2cm wavelength electromagnetic wave with both lenses, but the image obtained with a 2-D lens was much sharper. Therefore, the choice of the lens to be used in a sensor is prescribed by the specific requirements of the testing system. For example, a 1-D lens should be considered when the simplicity of the testing system is deemed more important than the quality of the image obtained from a defect. A 1-D lens also allows for a longer sample standoff distance and higher transmission.
Article
AZ series Mg alloys AZ31, AZ61, and AZ80 are widely applied in 3C (computer, communication, and consumer electronic) industry. Their corrosion characters in simulated sweat solution have been investigated by electrochemical technology, surface analysis, and pH measurements. Electrochemical test results showed that the three magnesium alloys revealed different corrosion resistance (Rt) in simulated sweat solution, Rt(AZ31)a<aR t(AZ61)a<aRt(AZ80). Three major components of simulated sweat solution played different roles during corrosion processes. Lactic acid was a kind of strong erosive medium for the magnesium alloys, and NaCl can induce pitting corrosion on alloys surface, while urea acted as a corrosion inhibitor. The corroded surface morphology of the three magnesium alloys was observed using scanning electron microscopy (SEM) and corrosion products were analyzed by X-ray diffraction (XRD). Result of pH measurement tests showed that there were differences in climbing speed and final values of pH for the three magnesium alloys in simulated sweat solution.
Article
A simple analytical model, based on reaction-diffusion theory, is developed to predict the trade-off between average response (settling) time (ts) and minimum detectable concentration (&rgr;0) for nanobiosensors and nanochemical sensors. The model predicts a scaling relationship &rgr;0tsMD∼kD, where MD and kD are dimensionality dependent constants for one, two, and three dimensional nanosensors. We explore the performance limits of nanosensors using this analytical model and support its conclusions using detailed numerical simulation. Our results have obvious and significant implications for analyte density and response time reported in the literature and for design consideration of nanobiosensors and nanochemical sensors.
Article
An extremely low operating electric field has been achieved on zinc oxide (ZnO) nanowire field emitters grown on carbon cloth. Thermal vaporization and condensation was used to grow the nanowires from a mixture source of ZnO and graphite powders in a tube furnace. An emission current density of 1 mA∕cm2 was obtained at an operating electric field of 0.7 V∕μm. Such low field results from an extremely high field enhancement factor of 4.11×104 due to a combined effect of the high intrinsic aspect ratio of ZnO nanowires and the woven geometry of carbon cloth.
Article
The specular reflectance from a hexagonal array of gold nanorods embedded in an alumina matrix supported on an aluminum substrate is reported. The rods were grown by electrodeposition of gold in an alumina template and were oriented with their long axis perpendicular to the film surface. Optical reflectance measurements performed with an incident light beam of S polarization only exhibited the transverse surface plasmon resonance whereas the measurements obtained with P polarization exhibited both transverse and longitudinal resonances. A model for the reflectance from a thin anisotropic film was developed and shown to be in agreement with the experimental data.