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Norovirus (NoV) is the predominant cause of foodborne illness globally; current detection methods are typically expensive, have inadequate sensitivities, and utilize biological receptors with poor stability. Therefore, accurate, cost-effective, and highly stable detection methods are needed to screen for NoV in foods. We developed molecularly imprinted polymer nanoparticles (nanoMIPs) to detect NoV using a small target epitope (12 amino acids) with a solid-phase synthesis approach. The performance of three batches of nanoMIPs with varying monomer compositions (nanoMIP-1, -2, and -3) were compared both experimentally and computationally. Surface plasmon resonance examined nanoMIP binding affinity to norovirus virus-like particles (NoV-LPs), whereby nanoMIP-1 had the lowest KD value of 0.512 µM. This is significant, as traditional targets for generation of norovirus ligands previously reported were generated against drastically larger norovirus capsid segments that have limitations in ease of production. Further, an electrochemical sensor was developed by covalently attaching the nanoMIPs to glassy carbon electrodes. In agreement with our predictions from density functional theory simulations, electrochemical impedance spectroscopy showed a sensitive response toward NoV-LPs for nanoMIP batches tested; however, nanoMIP-1 was optimal, with an excellent detection limit of 3.4 pg/mL (1.9 × 105 particles/mL). Due to its exceptional performance, nanoMIP-1 was immobilized to screen-printed electrodes and utilized within a thermal sensor, where it exhibited a low detection limit of 6.5 pg/mL (3.7 × 105 particles/mL). Crucially, we demonstrated that nanoMIP-1 could detect NoV in real food samples (romaine lettuce) by using electrochemical and thermal sensors. Consequently, the study highlights the exceptional potential of nanoMIPs to replace traditional biological materials (e.g., antibodies) as sensitive, versatile, and highly stable receptors within NoV sensors.

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A nonenzymatic redox-responsive sensor was put forward for the detection of methylparathion (MP) by designing globular nanostructures of molecularly imprinted polymers on graphene oxide (GO@MIPs) via surface-initiated reversible addition-fragmentation chain transfer polymerization (SI-RAFT). Fourier transform infrared (FTIR) spectroscopy, field emission scanning electron microscopy (FESEM), and small-angle X-ray scattering (SAXS) studies have confirmed the successful formation of receptor layers of MIPs on RAFT agent-functionalized GO sheets. The electrochemical signal with an amplified current response was attained because of the enhanced diffusion rate of ions at the interface provided by widening the pore size of the MIP film. The analytical response of GO@MIPs, validated by recording square-wave anodic stripping voltammetry (SWASV) at varying MP concentrations, followed the linear response between 0.2 and 200 ng/mL. Under optimized conditions, the sensor exhibited a limit of detection of 4.25 ng/mL with high selectivity over other interfering ions or molecules. The anti-interfering ability and good recovery (%) in food samples directed the use of the proposed sensor toward real-time monitoring and also toward future mimicking of surfaces.

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Crevice corrosion in modular taper junctions of hip or knee replacements using cobalt-chrome-molybdenum (CoCrMo) alloys remains a clinical concern. Non-mechanically-driven corrosion has been less explored compared to mechanically assisted crevice corrosion. This study hypothesized that solution chemistry within crevices, inflammation, and cathodic electrode potential shifts during fretting result in low pH and generate reactive oxygen species (ROS), affecting oxide film behavior. This study investigated how resistance and capacitance of the CoCrMo oxide film (i.e., corrosion resistance) are modified in simulated in vivo crevice environments of modular taper junctions. Six solutions were evaluated (two pH levels: 1 and 7.4 and four hydrogen peroxide (H2O2) concentrations: 0, 0.001, 0.01 and 0.1 M). Rp versus voltage and Mott-Schottky plots were created from symmetry-based electrochemical impedance spectroscopy (sbEIS). At pH 1, the semiconductor transition to p-type occurs at more anodic potentials and higher flat band potentials were found. H2O2 decreased the flat band potential and slope in the Mott-Schottky plot. Higher H2O2 in pH 7.4 solution significantly modified the oxide film, leading to increased donor density (p = 0.0004) and a 150-fold reduction in Rp in the cathodic potential range at -1 V (p = 0.0005). The most unfavorable condition (0.1 M H2O2 pH 1) resulted in a 250-fold lower resistance compared to phosphate buffered saline (PBS) pH 7.4 at -1 V (p = 0.0013). This study highlights the corrosion susceptibility of CoCrMo under adverse chemical and potential conditions, identifying increased defects in the oxide film due to ROS, hydrogen ions and electrode potential. STATEMENT OF SIGNIFICANCE: Corrosion of cobalt chrome molybdenum alloy caused by direct chemical attack in the crevice region of hip replacements, such as modular taper junctions, remains a clinical concern. The junction environment contains adverse chemical compositions, including high acidity and reactive oxygen species (ROS) due to inflammatory responses against the corrosion products. We simulate inflammatory environments with different pH levels and hydrogen peroxide, representative of ROS. We employ electrochemical impedance spectroscopy and apply stepwise voltage over the range induced by tribocorrosion processes. We relate the effect of adverse chemical components on corrosion and semiconducting behavior of the oxide film using Mott-Schottky analysis. This study shows how pH and ROS concentration compromises the oxide film potentially leading to non-mechanically induced corrosion.

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This article reports on a bioanalytical sensor device that hosts three different transducer principles: impedance spectroscopy, quartz-crystal microbalance with dissipation monitoring, and the thermal-current-based heat-transfer method. These principles utilize a single chip, allowing one to perform either microbalance and heat transfer measurements in parallel or heat transfer and impedance measurements. When taking specific precautions, the three measurement modalities can even be used truly simultaneously. The probed parameters are distinctly different, so that one may speak about multiparametric or "orthogonal" sensing without crosstalk between the sensing circuits. Hence, this sensor allows one to identify which of these label-free sensing principles performs best for a given bioanalytical application in terms of a high signal amplitude and signal-to-noise ratio. As a proof-of-concept, the three-parameter sensor was validated by studying the spontaneous, collective detachment of eukaryotic cells in the presence of a temperature gradient between the QCM chip and the supernatant liquid. In addition to heat transfer, detachment can also be monitored by the impedance- and QCM-related signals. These features allow for the distinguishing between different yeast strains that differ in their flocculation genes, and the sensor device enables proliferation monitoring of yeast colonies over time.

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The combination of solid oxide fuel cells (SOFCs) and wood gasification has the potential to significantly increase renewable electricity production and decrease emissions. Depending on the quality of the wood gas, degradation processes have a significant impact on the reliability and lifetime of the SOFC. Using electrochemical impedance spectroscopy (EIS) and subsequent distribution of relaxation times (DRT) analysis, the impact on the degradation of coupling wood gasification with a commercial SOFC stack is determined in this study. The thermal behavior of the SOFC stack under various operating conditions, as well as various synthetic wood gas mixtures classified by their hydrogen-to-carbon (H/C) ratio, was assessed. The decrease in the H/C ratio from 8 to 1, observed during syngas and real wood gas operation, leads to a rightward shift in the Nyquist plots, suggesting an increase in the SOFC stack's impedance. Correlations between variations in the H/C ratio and their effects on anodic electrooxidation, ionic conduction, gas transport, and diffusion were identified using DRT analysis to interpret the EIS results. By incorporating an upstream desulfurization system and ensuring an H/C ratio greater than 2, the coupling of biomass gasification with the SOFC stack was stable to degradation issues.

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Electrochemical impedance spectroscopy (EIS), a conventional and alternating-current-(AC)-based technique for impedance measurement, is commonly used in battery diagnosis. However, it requires expensive equipment and demanding operating conditions and is complex and model-dependent in data analysis. Recently, novel direct current (DC) analytics have emerged as an alternative to EIS. They are simple yet powerful, being capable of revealing impedance information that traditionally could only be obtained through EIS and determining Li-ion diffusion coefficient. Besides, a complete EIS spectrum can be predicted based on constant current charging curves in the support of machine learning methods. This work highlights the similarities and discrepancies between DC techniques and EIS in the electrochemical analysis of Li-ion batteries. Looking ahead, DC techniques may be a promising substitute for EIS in future battery diagnosis, requiring simplified equipment while offering a deep understanding of battery impedance and its underlying electrochemical processes.

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Ammonia­nitrogen wastewater is one of the main pollutants in the current environment. Rapid detection of microorganisms resistant to ammonia­nitrogen provides a basis for bioremediation of ammonia­nitrogen contaminated sites. This study uses electrochemical analysis for efficiently detecting of ammonia-resistant bacteria, utilizing a commercially available, low-cost screen-printed electrode (SPE) modified with agarose-based hydrogel (gel) or graphene oxide (GO). At the same time, the study employed electrochemical impedance spectroscopy (EIS) and differential pulse voltammetry (DPV) to monitor bacterial growth, revealing Escherichia coli (E. coli) inhibition upon ammonia­nitrogen addition, while Raoultella terrigena (RN1) and Pseudomonas (RN2) exhibit tolerance. The method provides sensitivity results in <45 min, which is significantly faster than traditional methods. RN1 and RN2 exhibit promising ammonia­nitrogen removal rates, reaching up to 81 % and 92 %, respectively. This study aimed to develop an effective electrochemical method for rapidly detecting the sensitivity of microorganisms to ammonia­nitrogen. The method offers advantages such as high speed, efficiency, and cost-effectiveness, potentially providing valuable microbial resources for mitigating ammonia nitrogen wastewater pollution.

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A simple technique was utilized to fabricate pure hexagonal La2O3 nanorods by utilizing lanthanum(III) nitrate hexahydrate (La(NO3)3·6H2O) and ammonia (NH4OH). The La2O3 nanoparticles were analyzed using XRD, TGA, Raman, SEM, FTIR, TEM, PL spectroscopy, and Mott-Schottky techniques. The XRD analysis confirmed the production of La(OH)3 nanorods under appropriate conditions, which were then successfully converted into La2O2CO3 and finally into La2O3 nanorods through annealing. The TGA analysis showed that the total weight loss was due to water evaporation and the dissolution of minimal moisture present in the environment. The FTIR analysis confirmed the presence of functional groups. The SEM analysis revealed changes in morphology. The TEM analysis to determine the particle size. The PL findings showed three emission peaks at 390, 520, and 698 nm due to interband transitions and defects in the samples. The Mott-Schottky analysis demonstrated that the flatband potential and acceptor density varied with annealing temperature, ranging from 1 to 1.2 V and 2 × 1018 to 1.4 × 1019 cm-3, respectively. Annealing at 1000 °C resulted in the lowest resistance to charge transfer (Rct).

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Premature failure and degradation of layers are the main problems for transportation infrastructure. Addressing these issues necessitates implementing structural health monitoring (SHM) for pavement construction layers. To this end, this research investigated the stress/strain and damage detection capabilities of a self-sensing cementitious composite developed for potential utilization in the construction of an intelligent subgrade layer. The prepared self-sensing cementitious composite consisted of 10% cement and hybrid conductive fillers, including multiwalled carbon nanotubes (MWCNTs) and graphene nanoplatelets (GNPs) in sand. Initial findings reveal that the electrical resistivity of the composite is significantly affected by the concentration of MWCNTs/GNPs, with a minimum concentration of more than 0.5% needed to achieve a responsive cementitious composite. Moreover, the piezoresistive analysis indicates that an increase in the concentration of MWCNTs/GNPs and stress levels leads to an improvement in the stress/strain-sensing performance. When the self-sensing cementitious composite is subjected to equivalent stress levels, variations in the fractional changes in resistivity (FCR) exhibit an increasing trend with decreasing resilient modulus, stemming from a decrease in stiffness due to the increased concentration of MWCNTs/GNPs. Additionally, the electrochemical impedance spectroscopy (EIS) analysis demonstrates a contraction for the Nyquist plots under compressive ramp loading prior to failure, followed by the expansion of these curves post-failure. Scanning electron microscopy (SEM) images visually showcase the bridging effects of MWCNTs and the filling effects of GNPs within the composite structure.

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SARS-CoV-2 emerged in late 2019 and quickly spread globally, resulting in significant morbidity, mortality, and socio-economic disruptions. As of now, collaborative global efforts in vaccination and the advent of novel diagnostic tools have considerably curbed the spread and impact of the virus in many regions. Despite this progress, the demand remains for low-cost, accurate, rapid and scalable diagnostic tools to reduce the influence of SARS-CoV-2. Herein, the angiotensin-converting enzyme 2 (ACE2), a receptor for SARS-CoV-2, was immobilized on two types of electrodes, a screen-printed gold electrode (SPGE) and a screen-printed carbon electrode (SPCE), to develop electrochemical biosensors for detecting SARS-CoV-2 with high sensitivity and selectivity. This was achieved by using 1H, 1H, 2H, 2H-perfluorodecanethiol (PFDT) and aryl diazonium salt serving as linkers for SPGEs and SPCEs, respectively. Once SARS-CoV-2 was anchored onto the ACE2, the interaction of the virus with the redox probe was analyzed using electrochemical impedance spectroscopy (EIS) and cyclic voltammetry (CV). Aryl diazonium salt was observed as a superior linker compared to PFDT due to its consistent performance in the modification of the SPCEs and effective ACE2 enzyme immobilization. A distinct pair of redox peaks in the cyclic voltammogram of the biosensor modified with aryl diazonium salt highlighted the redox reaction between the functional groups of SARS-CoV-2 and the redox probe. The sensor presented a linear relationship between the redox response and the logarithm of SARS-CoV-2 concentration, with a detection limit of 1.02 × 106 TCID50/mL (50% tissue culture infectious dose). Furthermore, the biosensor showed remarkable selectivity towards SARS-CoV-2 over H1N1virus.

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Oncostatin M (OSM) is an interleukin-6 (IL-6) member family cytokine implicated in the pathogenesis of chronic diseases including inflammatory bowel disease (IBD). OSM is a novel diagnostic biomarker over-expressed in the serum of IBD patients. This paper reports on the first electrochemical OSM immunosensor, developed using a multistep fabrication process aimed at covalently immobilizing OSM antibodies on a mixed self-assembled monolayer coated gold working electrode. Cyclic voltammetry, atomic force microscopy (AFM), IR spectroscopy and optical characterizations were used to validate the sensor functionalization protocol. Electrochemical impedance spectroscopy (EIS) measurements were performed to assess the reliability of the immunosensor preparation and to verify the antibody-antigen complexes formation. The label-free immunosensor showed high sensitivity identifying OSM at clinically relevant concentrations (37-1000 pg mL-1) with low detection limit of 2.86 pg mL-1. Both sensitivity and selectivity of the proposed immunosensor were also demonstrated in human serum in the presence of interfering biomarkers, making it an innovative potential platform for the OSM biomarker detection in IBD patients' serum.

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Nanofiber technology is leading the revolution of wearable technology and provides a unique capability to fabricate smart textiles. With the novel fabrication technique of electrospinning, nanofibers can be fabricated and then manufactured into a durable conductive string for the application of smart textiles. This paper presents an electrospun nanofiber mesh-based (NF-Felt) string electrode with a conducting polymer coating for an electrochemical enzymatic glucose sensor. The surface area of a nanofiber matrix is a key physical property for enhanced glucose oxidase (GOx) enzyme binding for the development of an electrochemical biosensor. A morphological characterization of the NF-Felt string electrode was performed using scanning electron microscopy (SEM) and compared with a commercially available cotton-polyester (Cot-Pol) string coated with the same conducting polymer. The results from stress-strain testing demonstrated high stretchability of the NF-Felt string. Also, the electrochemical characterization results showed that the NF-Felt string electrode was able to detect a glucose concentration in the range between 0.0 mM and 30.0 mM with a sensitivity of 37.4 µA/mM·g and a detection limit of 3.31 mM. Overall, with better electrochemical performance and incredible flexibility, the NF-Felt-based string electrode is potentially more suitable for designing wearable biosensors for the detection of glucose in sweat.

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Salmonella contamination is a major global health challenge, causing significant foodborne illness. However, current detection methods face limitations in sensitivity and time, which mostly rely on the culture-based detection techniques. Hence, there is an immediate and critical need to enhance early detection, reduce the incidence and impact of Salmonella contamination resulting in outbreaks. In this work, we demonstrate a portable non-faradaic, electrochemical sensing platform capable of detecting Salmonella in potable water with an assay turnaround time of ~ 9 min. We evaluated the effectiveness of this sensing platform by studying two sensor configurations: one utilizing pure gold (Au) and the other incorporating a semiconductor namely a zinc oxide thin film coated on the surface of the gold (Au/ZnO). The inclusion of zinc oxide was intended to enhance the sensing capabilities of the system. Through comprehensive experimentation and analysis, the LoD (limit of detection) values for the Au sensor and Au/ZnO sensor were 0.9 and 0.6 CFU/mL, respectively. In addition to sensitivity, we examined the sensing platform's precision and reproducibility. Both the Au sensor and Au/ZnO sensor exhibited remarkable consistency, with inter-study percentage coefficient of variation (%CV) and intra-study %CV consistently below 10%. The proposed sensing platform exhibits high sensitivity in detecting low concentrations of Salmonella in potable water. Its successful development demonstrates its potential as a rapid and on-site detection tool, offering portability and ease of use. This research opens new avenues for electrochemical-based sensors in food safety and public health, mitigating Salmonella outbreaks and improving water quality monitoring.

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In this study, we are reporting a novel electrochemical capacitance spectroscopy (ECS) platform designed for the sensitive and label-free detection of antibodies against severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2) virus spike protein (anti-rS) in diluted blood serum. The determination of anti-rS is crucial for identification individuals who have been infected by SARS-CoV-2 virus and may have acquired immunity. The rS protein was immobilized on a screen-printed carbon electrode, which was incubated in diluted blood serum containing anti-rS antibodies. Label-free ECS was applied for the determination of interaction between immobilized rS and free-standing anti-rS. Here reported bioanalytical platform demonstrated high sensitivity and specificity in detecting anti-rS, achieving a limit of detection of 4.38 nM. This versatile platform could be further enhanced by applying various electrode materials and adapting this platform to detect antibodies against some other proteins. Our findings have significant implications for the development of affordable, scalable biosensing platforms capable to provide rapid and accurate public health screening and monitoring, particularly in the context of the coronavirus disease 2019 (COVID-19) pandemic.

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Food allergies are an exceptional response of the immune system caused by the ingestion of specific foods. The main foods responsible for allergic reactions are milk, eggs, seafood, soy, peanuts, tree nuts, wheat, and their derived products. Chicken egg ovalbumin (OVA), a common allergen molecule, is often used for the clarification process of wine. Traces of OVA remain in the wine during the fining process, and they can cause significant allergic reactions in sensitive consumers. Consequently, the European Food Safety Authority (EFSA) and the American Food and Drug Administration (FDA) have shown the risks for allergic people to assume allergenic foods and food ingredients, including eggs. Commonly, OVA detection requires sophisticated and time-consuming analytical techniques. Intending to develop a faster assay, we designed a proof-of-concept non-Faradaic impedimetric immunosensor for monitoring the presence of OVA in wine. Polyclonal antibodies anti-OVA were covalently immobilised onto an 11-mercaptoundecanoic-acid (11-MUA)-modified gold surface. The developed immunosensor was able to detect OVA in diluted white wine without the need for an external probe or any pre-treatment step with a sensitivity of 0.20 µg/mL, complying with the limit established by the resolution OIV/COMEX 502-2012 for the quantification of allergens in wine.

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An ultrasensitive impedimetric immunosensor was developed to detect brain natriuretic peptide (BNP) for early diagnosis of heart failure. To construct this immunosensor, anti-BNP antibodies were immobilized covalently onto nanocomposite of chitosan-Au nanoparticles and reduced graphene oxide nanosheets (CHIT-Au@rGONs) electrodeposited onto pencil graphite electrode. This approach impedes charge transfer resistance (Rct) value proportionally to the BNP captured by antigen-antibody interactions. The observed Rct values by this immunosensor, were correlated with linear concentrations of BNP in the range, 1 × 10-2 to 1 × 103 pg/mL, with a limit of detection of 12 pg/mL and limit of quantification of 36.3 pg/mL. The immunosensor detected BNP in spiked human sera. The analytic recovery of added BNP in human sera was 97.04%. The present method was fairly consistent with commercial approach. The working electrode was stored for 2 months in cold. BSA-IgG had no interference in the electrode activity showing its high specificity for BNP. This novel approach provided a new POC-diagnostics, as direct sample measurements are easier and more efficient by this immunosensor compared to existing immunosensors. Supplementary Information: The online version contains supplementary material available at 10.1007/s13205-023-03704-x.

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Introduction: Fibro-calcific aortic valve disease has high prevalence and is associated with significant mortality. Fibrotic extracellular matrix (ECM) remodeling and calcific mineral deposition change the valvular microarchitecture and deteriorate valvular function. Valvular interstitial cells (VICs) in profibrotic or procalcifying environment are frequently used in vitro models. However, remodeling processes take several days to weeks to develop, even in vitro. Continuous monitoring by real-time impedance spectroscopy (EIS) may reveal new insights into this process. Methods: VIC-driven ECM remodeling stimulated by procalcifying (PM) or profibrotic medium (FM) was monitored by label-free EIS. Collagen secretion, matrix mineralization, viability, mitochondrial damage, myofibroblastic gene expression and cytoskeletal alterations were analyzed. Results and Discussion: EIS profiles of VICs in control medium (CM) and FM were comparable. PM reproducibly induced a specific, biphasic EIS profile. Phase 1 showed an initial impedance drop, which moderately correlated with decreasing collagen secretion (r = 0.67, p = 0.22), accompanied by mitochondrial membrane hyperpolarization and cell death. Phase 2 EIS signal increase was positively correlated with augmented ECM mineralization (r = 0.97, p = 0.008). VICs in PM decreased myofibroblastic gene expression (p < 0.001) and stress fiber assembly compared to CM. EIS revealed sex-specific differences. Male VICs showed higher proliferation and in PM EIS decrease in phase 1 was significantly pronounced compared to female VICs (male minimum: 7.4 ± 4.2%, female minimum: 26.5 ± 4.4%, p < 0.01). VICs in PM reproduced disease characteristics in vitro remarkably fast with significant impact of donor sex. PM suppressed myofibroblastogenesis and favored ECM mineralization. In summary, EIS represents an efficient, easy-to-use, high-content screening tool enabling patient-specific, subgroup- and temporal resolution.

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In order to advance the development of sensors fabricated with monofunctional sensation systems capable of a versatile response to tactile, thermal, gustatory, olfactory, and auditory sensations, mechanoreceptors fabricated as a single platform with an electric circuit require investigation. In addition, it is essential to resolve the complicated structure of the sensor. In order to realize the single platform, our proposed hybrid fluid (HF) rubber mechanoreceptors of free nerve endings, Merkel cells, Krause end bulbs, Meissner corpuscles, Ruffini endings, and Pacinian corpuscles mimicking the bio-inspired five senses are useful enough to facilitate the fabrication process for the resolution of the complicated structure. This study used electrochemical impedance spectroscopy (EIS) to elucidate the intrinsic structure of the single platform and the physical mechanisms of the firing rate such as slow adaption (SA) and fast adaption (FA), which were induced from the structure and involved the capacitance, inductance, reactance, etc. of the HF rubber mechanoreceptors. In addition, the relations among the firing rates of the various sensations were clarified. The adaption of the firing rate in the thermal sensation is the opposite of that in the tactile sensation. The firing rates in the gustation, olfaction, and auditory sensations at frequencies of less than 1 kHz have the same adaption as in the tactile sensation. The present findings are useful not only in the field of neurophysiology, to research the biochemical reactions of neurons and brain perceptions of stimuli, but also in the field of sensors, to advance salient developments in sensors mimicking bio-inspired sensations.

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Alzheimer's disease (AD) is a neurodegenerative disease with only late-stage detection; thus, diagnosis is made when it is no longer possible to treat the disease, only its symptoms. Consequently, this often leads to caregivers who are the patient's relatives, which adversely impacts the workforce along with severely diminishing the quality of life for all involved. It is, therefore, highly desirable to develop a fast, effective and reliable sensor to enable early-stage detection in an attempt to reverse disease progression. This research validates the detection of amyloid-beta 42 (Aß42) using a Silicon Carbide (SiC) electrode, a fact that is unprecedented in the literature. Aß42 is considered a reliable biomarker for AD detection, as reported in previous studies. To validate the detection with a SiC-based electrochemical sensor, a gold (Au) electrode-based electrochemical sensor was used as a control. The same cleaning, functionalization and Aß1-28 antibody immobilization steps were used on both electrodes. Sensor validation was carried out by means of Cyclic Voltammetry (CV) and Electrochemical Impedance Spectroscopy (EIS) aiming to detect an 0.5 µg·mL-1 Aß42 concentration in 0.1 M buffer solution as a proof of concept. A repeatable peak directly related to the presence of Aß42 was observed, indicating that a fast SiC-based electrochemical sensor was constructed and may prove to be a useful approach for the early detection of AD.

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Graphene sponge anode functionalized with two-dimensional (2D) boron, i.e., borophene, was applied for electrochemical oxidation of C4-C8 per- and polyfluoroalkyl substances (PFASs). Borophene-doped graphene sponge outperformed boron-doped graphene sponge anode in terms of PFASs removal efficiencies and their electrochemical degradation; whereas at the boron-doped graphene sponge anode up to 35% of the removed PFASs was recovered after the current was switched off, the switch to a 2D boron enabled further degradation of the electrosorbed PFASs. Borophene-doped graphene sponge anode achieved 32-77% removal of C4-C8 PFASs in one-pass flow-through mode from a 10 mM phosphate buffer at 230 A m-2 of anodic current density. Higher molarity phosphate buffer (100 mM) resulted in lower PFASs removal efficiencies (11-60%) due to the higher resistance of the graphene sponge electrode in the presence of phosphate ions, as demonstrated by the electrochemical impedance spectroscopy (EIS) analyses. Electro-oxidation of PFASs was more efficient in landfill leachate despite its high organic loading, with up to 95% and 75% removal obtained for perfluorooctane sulfonate (PFOS) and perfluorooctanoic acid (PFOA), versus 77% and 57% removal in the 10 mM phosphate buffer, respectively. Defluorination efficiencies as determined relative to the electrooxidized fraction of PFASs indicated up to 69% and 82% of defluorination of PFOS and PFOA in 10 mM phosphate buffer, which was decreased to 16 and 29% defluorination, respectively, for higher buffer molarity (100 mM) due to the worsened electrochemical performance of the sponge. In landfill leachate, relative defluorination efficiencies of PFOS and PFOA were 33% and 45%, respectively, indicating the inhibiting effect of complex organic and inorganic matrix of landfill leachate on the C-F bond breakage. This study demonstrates that electrochemical degradation of PFASs is possible to achieve in complex and brackish streams using a low-cost graphene sponge anode, without forming toxic chlorinated byproducts even in the presence of >7 g L-1 of chloride.

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