Polyaromatic Hydrocarbon-Functionalized 2D MXene-Based 3D Porous Antifouling Nanocomposite with Long Shelf Life for High-Performance Electrochemical Immunosensor Applications.

Affinity-based electrochemical (AEC) biosensors have gained more attention in the field of point-of-care management. However, AEC sensing is hampered by biofouling of the electrode surface and degradation of the antifouling material. Therefore, a breakthrough in antifouling nanomaterials is crucial for the fabrication of reliable AEC biosensors. Herein, for the first time, we propose 1-pyrenebutyric acid-functionalized MXene to develop an antifouling nanocomposite to resist biofouling in the immunosensors. The nanocomposite consisted of a 3D porous network of bovine serum albumin cross-linked with glutaraldehyde with functionalized MXene as conductive nanofillers, where the inherited oxidation resistance property of functionalized MXene improved the electrochemical lifetime of the nanocomposite. On the other hand, the size-extruded porous structure of the nanocomposite inhibited the biofouling activity on the electrode surface for up to 90 days in real samples. As a proof of concept, the antifouling nanocomposite was utilized to fabricate a multiplexed immunosensor for the detection of C-reactive protein (CRP) and ferritin biomarkers. The fabricated sensor showed good selectivity over time and an excellent limit of detection for CRP and ferritin of 6.2 and 4.2 pg/mL, respectively. This research successfully demonstrated that functionalized MXene-based antifouling nanocomposites have great potential to develop high-performance and low-cost immunosensors.

Analyzing Subnational Immunization Coverage to Catch up and Reach the Unreached in Seven High-Priority Countries in the Eastern Mediterranean Region, 2019-2021.

Yearly national immunization coverage reporting does not measure performance at the subnational level throughout the year and conceals inequalities within countries. We analyzed subnational immunization coverage from seven high-priority countries in our region. We analyzed subnational, monthly immunization data from seven high-priority countries. Five were Gavi eligible (i.e., Afghanistan, Pakistan, Somalia, Syria, and Yemen); these are countries that according to their low income are eligible for support from the Global Alliance on Vaccine and Immunization, while Iraq and Jordan were included because of a recent decrease in immunization coverage and contribution to the regional number of under and unimmunized children. DTP3 coverage, which is considered as the main indicator for the routine immunization coverage as the essential component of the immunization program performance, varied monthly in 2019-2021 before reaching pre-pandemic coverage in the last two months of 2021. Somalia and Yemen had a net gain in DTP3 coverage at the end of 2021, as improvement in 2021 exceeded the regression in 2020. In Pakistan and Iraq, DTP3 improvement in 2021 equaled the 2020 regression. In Afghanistan, Syria and Jordan, the regression in DTP3 coverage continued in 2020 and 2021. The number of districts with at least 6000 zero-dose children improved moderately in Afghanistan and substantially in Somalia throughout the follow-up period. In Pakistan, the geographical distribution differed between 2020 and 2021.Of the three countries with the highest number of zero-dose children, DTP1 coverage reached 109% in Q4 of 2020 after a sharp drop to 69% in Q2 of 2020. However, in Pakistan, the number of zero-dose children decreased to 1/10 of its burden in Q4 of 2021. In Afghanistan, the number of zero-dose children more than a doubled. Among the even countries, adaptation of immunization service to the pandemic varied, depending on the agility of the health system and the performance of the components of the expanded program on immunization. We recommended monitoring administrative monthly immunization coverage data at the subnational level to detect low-performing districts, plan catchup, identify bottlenecks towards reaching unvaccinated children and customize strategies to improve the coverage in districts with zero-dose children throughout the year and monitor progress.

Technological Tools and Artificial Intelligence in Estrus Detection of Sows-A Comprehensive Review.

In animal farming, timely estrus detection and prediction of the best moment for insemination is crucial. Traditional sow estrus detection depends on the expertise of a farm attendant which can be inconsistent, time-consuming, and labor-intensive. Attempts and trials in developing and implementing technological tools to detect estrus have been explored by researchers. The objective of this review is to assess the automatic methods of estrus recognition in operation for sows and point out their strong and weak points to assist in developing new and improved detection systems. Real-time methods using body and vulvar temperature, posture recognition, and activity measurements show higher precision. Incorporating artificial intelligence with multiple estrus-related parameters is expected to enhance accuracy. Further development of new systems relies mostly upon the improved algorithm and accurate data provided. Future systems should be designed to minimize the misclassification rate, so better detection is achieved.

Microfluidic-Integrated Multimodal Wearable Hybrid Patch for Wireless and Continuous Physiological Monitoring.

Despite extensive advances in wearable monitoring systems, most designs focus on the detection of physical parameters or metabolites and do not consider the integration of microfluidic channels, miniaturization, and multimodality. In this study, a combination of multimodal (biochemical and electrophysiological) biosensing and microfluidic channel-integrated patch-based wireless systems is designed and fabricated using flexible materials for improved wearability, ease of operation, and real-time and continuous monitoring. The reduced graphene oxide-based microfluidic channel-integrated glucose biosensor exhibits a good sensitivity of 19.97 (44.56 without fluidic channels) µA mM-1 cm-2 within physiological levels (10 µM-0.4 mM) with good long-term and bending stability. All the sensors in the patch are initially validated using sauna gown sweat-based on-body and real-time tests with five separate individuals who perspired three times each. Multimodal glucose and electrocardiogram (ECG) sensing, along with their real-time adjustment based on sweat pH and temperature fluctuations, optimize sensing accuracy. Laser-burned hierarchical MXene-polyvinylidene fluoride-based conductive carbon nanofiber-based dry ECG electrodes exhibit low skin contact impedance (40.5 kΩ cm2) and high-quality electrophysiological signals (signal-to-noise ratios = 23.4-32.8 dB). The developed system is utilized to accurately and wirelessly monitor the sweat glucose and ECG of a human subject engaged in physical exercise in real time.

An oxygen-insensitive and minimally invasive polymeric microneedle sensor for continuous and wide-range transdermal glucose monitoring.

Despite significant advances in diabetes management, particularly with the introduction of the most recent continuous glucose monitoring devices (CGMDs) that can monitor glucose actively in the transdermal interstitial fluid (ISF) in vivo, CGMDs still have significant disadvantages in terms of accuracy, low interference effect, precision, and stability. This is mostly because they detect hydrogen peroxide at higher potentials and require an oxygen-rich environment. First in its class, we developed an oxygen-insensitive polymeric glucose microneedle (MN) that was functionalized using a new electron-transfer mediator, 3-(3'-phenylimino)-3H-phenothiazinesulfonic acid-based enzyme cocktail for the NAD-GDH system. The inclusion of reduced graphene oxide aided in the absorption of the cocktail via the π-π interaction and enhanced the conductivity and sensor performance. The MN exhibited a dynamic linear range (1-30 mM) with a low detection limit of 26 µM, high sensitivity (18.05 µAmM-1 cm-2), stability (up to 7 days), high selectivity (due to a low oxidation potential of 0.15 V), and a fast response time (∼3 s). In vivo, deployment of the MN in a rabbit model demonstrated that the ISF glucose concentrations measured with the MN for up to 24 h correlate very well with the blood glucose concentrations measured with a commercial glucometer.

A hybridized nano-porous carbon reinforced 3D graphene-based epidermal patch for precise sweat glucose and lactate analysis.

Wearable electrochemical biosensors for perspiration analysis offer a promising non-invasive biomarker monitoring method. Herein, a functionalized hybridized nanoporous carbon (H-NPC)-encapsulated flexible 3D porous graphene-based epidermal patch was firstly fabricated for monitoring sweat glucose, lactate, pH, and temperature using simple, cost-effective, laser-engraved, and spray-coating techniques. The fabricated H-NPC-modified electrode significantly increased electrochemical surface area and electrocatalytic activity. Within the physiological sweat range (0-1.5 mM), the second-generation glucose sensor exhibited an excellent sensitivity of 82.7 µAmM-1cm-2 with 0.025 µM LOD. Moreover, the lactate biosensor exhibited an extraordinary linear range (0-56 mM) response owing to the incorporation of an outer diffusion limiting layer (DLL) that controls the lactate flux reaching the enzyme with comparable sensitivity (204 nAmM-1cm-2) and LOD (4 µM). Finally, we employed an analytical correction approach incorporating pH and temperature adjustments during on-body tests. In addition to connecting various carbon-based materials to limitless metal-organic frameworks as a transduction material, our research also paves the way for enabling these sensors to operate on pH and T correction independently while delivering accurate results.

A nanocomposite-decorated laser-induced graphene-based multi-functional hybrid sensor for simultaneous detection of water contaminants.

Here, nanocomposite-decorated laser-induced graphene-based flexible hybrid sensor is newly developed for simultaneous detection of heavy metals, pesticides, and pH in freshwater. A series of deposition methods such as drop-casting, electroplating, and heating are adopted to modify and functionalize laser-induced graphene for engineering the high-performance detection at the individual sensor. A micro-dendritic structured bismuth@tin alloy inlaid on laser-induced graphene is prepared via a simple ex-situ electrodeposition method and thermal treatment for detecting heavy metals. The electrochemical performance is evaluated through the simultaneous determination of lead and cadmium ions at the optimized deposition potential of -1.2 V for 170 s, and a wide detection concentration range of 2-250 ppb and low detection limits (1.6 ppb and 0.9 ppb, respectively) are achieved. The pesticide sensor co-modified by zirconia nanoparticles and multilayered Ti3C2Tx-MXene is successfully implemented with a good linear performance for parathion after an optimal accumulation time of 120s. It realizes a low detection concentration range (0.1-5 ppb) with a detection limit of 0.06 ppb. Furthermore, a polyaniline/antimony/laser-induced graphene-based pH sensor is also integrated, showing an excellent sensitivity of -72.08 mV pH-1 in the pH range (2-9). They are also measured and characterized in different real water samples, exhibiting an acceptable detection performance, which provides promising applicability in the on-site monitoring of pollutants in the water environment.

Siloxene-Functionalized Laser-Induced Graphene via COSi Bonding for High-Performance Heavy Metal Sensing Patch Applications.

Here, 2D Siloxene nanosheets are newly applied to functionalize porous laser-induced graphene (LIG) on polydimethylsiloxane, modify the surface chemical properties of LIG, and improve the heterogeneous electron transfer rate. Meanwhile, the newly generated COSi crosslink boosts the binding of LIG and Siloxene. Thus, the Siloxene/LIG composite is used as the basic electrode material for the multifunctional detection of copper (Cu) ions, pH, and temperature in human perspiration. Moreover, to enhance the sensing performance of Cu ions, Siloxene/LIG is further modified by carbon nanotubes (CNTs). The fabricated Siloxene-CNT/LIG-based Cu-ion sensor shows linear response within a wide range of 10-500 ppb and a low detection limit of 1.55 ppb. In addition, a pH sensor is integrated to calibrate for determining the accurate concentration of Cu ions due to pH dependency of the Cu-ion sensor. The polyaniline-deposited pH sensor demonstrates a good sensitivity of -64.81 mV pH-1 over the pH range of 3-10. Furthermore, a temperature sensor for accurate skin temperature monitoring is also integrated and exhibits a stable linear resistance response with an excellent sensitivity of 9.147 Ω °C-1 (correlation coefficient of 0.139% °C-1 ). The flexible hybrid sensor is promising in applications of noninvasive heavy-metal ion detection and prediction of related diseases.

A highly selective and stable cationic polyelectrolyte encapsulated black phosphorene based impedimetric immunosensor for Interleukin-6 biomarker detection.

Due to the insufficiency of binding sites for the immobilized recognition biomolecules on the immunosensing platform, cancer detection becomes challenging. Whereas, the degradation of black phosphorene (BP) in the presence of the environmental factors becomes a concerning issue for use in electrochemical sensing. In this study, BP is successfully encapsulated by polyallylamine (PAMI) to increase its stability as well as to enhance its electrochemical performance. The successful encapsulation of BP is ensured through X-ray Photoelectron spectroscopy and Raman spectroscopy, whereas the stability of black phosphorus is ensured by Zeta potential measurements and cyclic voltammetry tests. The developed BP-PAMI composite showed high stability in the ambient environment and exhibited improved electrochemical performances. The impedimetric immunosensor was developed on a BP-PAMI modified laser burned graphene (LBG) to detect interleukin-6 biomarkers using electrochemical impedance spectroscopy (EIS). Under the optimized parameters, the fabricated immunosensor demonstrated a wide linear range of 0.003-75 ng/mL, limit of detection (LOD) of 1 pg/mL. Based on the experimental analysis, the developed sensing strategy can be employed as an easy, disposable, cost-effective and highly selective point-of-care cancer detection. In addition, the developed technique can be applied broadly for detecting other biomarkers after treating with suitable biomolecules.

Hydrogen-Bond-Triggered Hybrid Nanofibrous Membrane-Based Wearable Pressure Sensor with Ultrahigh Sensitivity over a Broad Pressure Range.

Recently, flexible capacitive pressure sensors have received significant attention in the field of wearable electronics. The high sensitivity over a wide linear range combined with long-term durability is a critical requirement for the fabrication of reliable pressure sensors for versatile applications. Herein, we propose a special approach to enhance the sensitivity and linearity range of a capacitive pressure sensor by fabricating a hybrid ionic nanofibrous membrane as a sensing layer composed of Ti3C2Tx MXene and an ionic salt of lithium sulfonamides in a poly(vinyl alcohol) elastomer matrix. The reversible ion pumping triggered by a hydrogen bond in the hybrid sensing layer leads to high sensitivities of 5.5 and 1.5 kPa-1 in the wide linear ranges of 0-30 and 30-250 kPa, respectively, and a fast response time of 70.4 ms. In addition, the fabricated sensor exhibits a minimum detection limit of 2 Pa and high durability over 20 000 continuous cycles even under a high pressure of 45 kPa. These results indicate that the proposed sensor can be potentially used in mobile medical monitoring devices and next-generation artificial e-skin.

A wearable battery-free wireless and skin-interfaced microfluidics integrated electrochemical sensing patch for on-site biomarkers monitoring in human perspiration.

In this study, an ultra-high sensitive, flexible, wireless, battery-free, and fully integrated (no external analysis equipment) electrochemical sensing patch system, including a microfluidic-sweat collecting unit, was newly developed for the on-site monitoring of the [K+] concentration in human sweat. Multiwalled carbon nanotube (MWCNT) and MXene-Ti3C2TX based hybrid multi-dimensional networks were applied to obtain a high surface activation area and faster charge transfer rate, strongly adsorbing the valinomycin membrane to protect the ionophore for effective transshipment and immobilization of the [K+]. Furthermore, the controllable porosity of carbon-based materials can accelerate the kinetic process of ion diffusion. This hybrid nanonetwork structure effectively enhanced electrochemical stability and sensitivity, addressing the noise and signal drifting problems experienced with low concentration detection. The fabricated sensor exhibited a high ion concentration sensitivity of 63 mV/dec with excellent selectivity, amplified to 173 mV/dec with the integrated amplification system. The Near Field Communication (NFC) is used to transmit measurements to a smartphone wirelessly. A microfluidic channel was integrated with the electrochemical sensor patch to efficiently collect sweat on the human skin surface and mitigate the sensor surface contamination problem. Furthermore, the developed sensing patch can also be applied to other biomarkers on-site detection after modifying the working electrode with the corresponding selective membranes.

Smart bandage with integrated multifunctional sensors based on MXene-functionalized porous graphene scaffold for chronic wound care management.

Three-dimensional (3D) porous laser-guided graphene (LGG) electrodes on elastomeric substrates are of great significance for developing flexible functional electronics. However, the high sheet resistance and poor mechanical properties of LGG sheets obstruct their full exploitation as electrode materials. Herein, we applied 2D MXene nanosheets to functionalize 3D LGG sheets via a C-O-Ti covalent crosslink to obtain an LGG-MXene hybrid scaffold exhibited high conductivity and improved electrochemistry with fast heterogeneous electron transfer (HET) rate due to the synergistic effect between LGG and MXene. Then we transferred the obtained hybrid scaffold onto PDMS to engineer a smart, flexible, and stretchable multifunctional sensors-integrated wound bandage capable of assessing uric acid (UA), pH, and temperature at the wound site. The integrated UA sensor exhibited a rapid response toward UA in an extended wide range of 50-1200 µM with a high sensitivity of 422.5 µA mM-1 cm-2 and an ultralow detection limit of 50 µM. Additionally, the pH sensor demonstrated a linear Nernstian response (R2 = 0.998) with a high sensitivity of -57.03 mV pH-1 in the wound relevant pH range of 4-9. The temperature sensor exhibited a fast and stable linear resistive response to the temperature variations in the physiological range of 25-50 °C with an excellent sensitivity and correlation coefficient of 0.09% °C-1 and 0.999, respectively. We anticipate that this stretchable and flexible smart bandage could revolutionize wound care management and have profound impacts on the therapeutic outcomes.

High-Performance Flexible Electrochemical Heavy Metal Sensor Based on Layer-by-Layer Assembly of Ti3C2Tx/MWNTs Nanocomposites for Noninvasive Detection of Copper and Zinc Ions in Human Biofluids.

A flexible electrochemical heavy metal sensor based on a gold (Au) electrode modified with layer-by-layer (LBL) assembly of titanium carbide (Ti3C2Tx) and multiwalled carbon nanotubes (MWNTs) nanocomposites was successfully fabricated for the detection of copper (Cu) and zinc (Zn) ions. An LBL drop-coating process was adopted to modify the surface of Au electrodes with Ti3C2Tx/MWNTs treated via ultrasonication to fabricate this novel nanocomposite electrode. In addition, an in situ simultaneous deposition of "green metal" antimony (Sb) and target analytes was performed to improve the detection performance further. The electrochemical measurement was realized using square wave anodic stripping voltammetry (SWASV). Moreover, the fabricated sensor exhibited excellent detection performance under the optimal experimental conditions. The detection limits for Cu and Zn are as low as 0.1 and 1.5 ppb, respectively. Furthermore, Cu and Zn ions were successfully detected in biofluids, that is, urine and sweat, in a wide range of concentration (urine Cu: 10-500 ppb; urine Zn: 200-600 ppb; sweat Cu: 300-1500 ppb; and sweat Zn: 500-1500 ppb). The fabricated flexible sensor also possesses other advantages of ultra-repeatability and excellent stability. Thus, these advantages provide a great possibility for the noninvasive smart monitoring of heavy metals in the future.

An Electrodeposited MXene-Ti3C2Tx Nanosheets Functionalized by Task-Specific Ionic Liquid for Simultaneous and Multiplexed Detection of Bladder Cancer Biomarkers.

Controlled deposition of 2D multilayered nanomaterials onto different electrodes to design a highly sensitive biosensing platform utilizing their active inherent electrochemistry is extremely challenging. Herein, a green, facile, and cost-effective one-pot deposition mechanism of 2D MXene-Ti3C2Tx nanosheets (MXNSs) onto conductive electrodes within few minutes via electroplating (termed electroMXenition) is reported for the first time. The redox reaction in the colloidal MXNS solution under the effect of a constant applied potential generates an electric field, which drives the nanoparticles toward a specific electrode interface such that they are cathodically electroplated. A task-specific ionic liquid, that is, 4-amino-1-(4-formyl-benzyl) pyridinium bromide (AFBPB), is exploited as a multiplex host arena for the substantial immobilization of MXNSs and covalent binding of antibodies. A miniaturized, single-masked gold dual interdigitated microelectrode (DIDµE) is microfabricated and presented by investigating the benefit of AFBPB coated on MXNSs. The resulting MXNSs-AFBPB-film-modified DIDµE biosensor exhibited a 7× higher redox current than bare electrodes owing to the uniform deposition. Using Apo-A1 and NMP 22 as model bladder cancer analytes, this newly developed dual immunosensor demonstrated precise and large linear ranges over five orders of significance with limit of detection values as low as 0.3 and 0.7 pg mL-1, respectively.

Wearable Capacitive Pressure Sensor Based on MXene Composite Nanofibrous Scaffolds for Reliable Human Physiological Signal Acquisition.

In recent years, highly sensitive pressure sensors that are flexible, biocompatible, and stretchable have attracted significant research attention in the fields of wearable electronics and smart skin. However, there has been a considerable challenge to simultaneously achieve highly sensitive, low-cost sensors coupled with optimum mechanical stability and an ultralow detection limit for subtle physiological signal monitoring devices. Targeting aforementioned issues, herein, we report the facile fabrication of a highly sensitive and reliable capacitive pressure sensor for ultralow-pressure measurement by sandwiching MXene (Ti3C2Tx)/poly(vinylidene fluoride-trifluoroethylene) (PVDF-TrFE) composite nanofibrous scaffolds as a dielectric layer between biocompatible poly-(3,4-ethylenedioxythiophene) polystyrene sulfonate /polydimethylsiloxane electrodes. The fabricated sensor exhibits a high sensitivity of 0.51 kPa-1 and a minimum detection limit of 1.5 Pa. In addition, it also enables linear sensing over a broad pressure range (0-400 kPa) and high reliability over 10,000 cycles even at extremely high pressure (>167 kPa). The sensitivity of the nanofiber-based sensor is enhanced by MXene loading, thereby increasing the dielectric constant up to 40 and reducing the compression modulus to 58% compared with pristine PVDF-TrFE nanofiber scaffolds. The proposed sensor can be used to determine the health condition of patients by monitoring physiological signals (pulse rate, respiration, muscle movements, and eye twitching) and also represents a good candidate for a next generation human-machine interfacing device.

Highly flexible and conductive poly (3, 4-ethylene dioxythiophene)-poly (styrene sulfonate) anchored 3-dimensional porous graphene network-based electrochemical biosensor for glucose and pH detection in human perspiration.

The patterned LIG flakes are generally not interconnected due to the line gap of the laser ray, leading to lower uniform conductivity and fragile graphene. Thus, the fabrication of a highly conductive and mechanically robust LIG-based biosensing platform remains challenging. In this study, the fabrication of a flexible electrochemical biosensor is reported based on poly (3, 4-ethylene dioxythiophene)-poly (styrene sulfonate) (PEDOT:PSS) modified 3-dimensional (3D) stable porous laser-induced graphene (LIG) for the detection of glucose and pH. PEDOT:PSS was spray-coated on the LIG to improve electrode robustness and deliver uniform electrical conductivity. The as-prepared PEDOT:PSS modified LIG (PP/LIG) was characterized using field-emission scanning electron microscopy (FESEM), x-ray photoelectron spectroscopy (XPS), Raman spectroscopy, and Fourier-transform infrared spectroscopy (FTIR). Platinum and palladium nanoparticles (Pt@Pd) were successfully electrodeposited on PP/LIG, markedly enhancing the electrocatalytic activity for glucose detection. The fabricated biosensor exhibited an excellent amperometric response to glucose with a wide linear range of 10 µM - 9.2 mM, a high sensitivity of 247.3 µAmM-1cm-2, and a low detection limit (LOD) of 3 µM, with high selectivity. In addition, the pH sensor was functionalized by the polyaniline (PANI) on PP/LIG, and it also exhibited excellent potentiometric response with a high sensitivity of 75.06 mV/pH in the linear range of pH 4 - 7. Ultimately, the feasibility of the biosensor was confirmed by the analysis of human perspiration collected during physical exercise. This approach validates the utility of the novel fabrication procedure, and the potential of the LIG-conductive polymer composite for biosensing applications.

MoS2-Decorated Laser-Induced Graphene for a Highly Sensitive, Hysteresis-free, and Reliable Piezoresistive Strain Sensor.

Advancement of sensing systems, soft robotics, and point-of-care testing requires the development of highly efficient, scalable, and cost-effective physical sensors with competitive and attractive features such as high sensitivity, reliability, and preferably reversible sensing behaviors. This study reports a highly sensitive and reliable piezoresistive strain sensor fabricated by one-step carbonization of the MoS2-coated polyimide film to obtain MoS2-decorated laser-induced graphene. The resulting three-dimensional porous graphene nanoflakes decorated with MoS2 exhibit stable electrical properties yielding a reliable output for longer strain/release cycles. The sensor demonstrates high sensitivity (i.e., gauge factor, GF ≈1242), is hysteresis-free (∼2.75%), and has a wide working range (up to 37.5%), ultralow detection limit (0.025%), fast relaxation time (∼0.17 s), and a highly stable and reproducible response over multiple test cycles (>12 000) with excellent switching response. Owing to the outstanding performances of the sensor, it is possible to successfully detect various subtle movements ranging from phonation, eye-blinking, and wrist pulse to large human-motion-induced deformations.