RBD-Modified Polyaniline-Based Label-Free Immunosensor for Sensitive Impedimetric Detection of Anti-SARS-CoV-2 Antibodies

The emergence of the SARS-CoV-2 virus and the associated pandemic has affected the entire human population. Human susceptibility to the virus has highlighted a tremendous need for affordable diagnostic systems to manage the pandemic and monitor the effectiveness of vaccination. We have developed a simple and label-free electrochemical immunosensor for the detection of human anti-SARS-CoV-2 IgG antibodies, which consists of a supporting screen-printed carbon electrode (SPCE) modified with an electrodeposited polyaniline film and glutaraldehyde, allowing effective immobilization of the SARS-CoV-2 spike glycoprotein receptor-binding domain (RBD) as a biorecognition element. The impedimetric immunosensor showed a linear response over a wide concentration range of 0.01–10 μg mL−1, that is, 67 pM–6.7 nM, with a low detection limit of 25.9 pM. A dual working electrode configuration with a built-in negative control unit was demonstrated for practical field applications. The immunosensor was successfully used in a real serum sample from an infected patient and showed good reproducibility and fair agreement with ELISA. An optional amplification step with secondary goat anti-human IgG antibodies was demonstrated, resulting in an extended linear range and a detection limit as low as 0.93 pM.

Automatic Analysis of Isothermal Amplification via Impedance Time-Constant-Domain Spectroscopy: A SARS-CoV-2 Case Study

The development of sensitive and affordable testing devices for infectious diseases is essential to preserve public health, especially in pandemic scenarios. In this work, we have developed an attractive analytical method to monitor products of genetic amplification, particularly the loop-mediated isothermal amplification reaction (RT-LAMP). The method is based on electrochemical impedance measurements and the distribution of relaxation times model, to provide the so-called time-constant-domain spectroscopy (TCDS). The proposed method is tested for the SARS-CoV-2 genome, since it has been of worldwide interest due to the COVID-19 pandemic. Particularly, once the method is calibrated, its performance is demonstrated using real wastewater samples. Moreover, we propose a simple classification algorithm based on TCDS data to discriminate among positive and negative samples. Results show how a TCDS-based method provides an alternative mechanism for label-free and automated assays, exhibiting robustness and specificity for genetic detection.

Customizable Fabrication Process for Flexible Carbon-Based Electrochemical Biosensors

In recent research, 3D printing has become a powerful technique and has been applied in the last few years to carbon-based materials. A new generation of 3D-printed electrodes, more affordable and easier to obtain due to rapid prototyping techniques, has emerged. We propose a customizable fabrication process for flexible (and rigid) carbon-based biosensors, from biosensor design to printable conductive inks. The electrochemical biosensors were obtained on a 50 µm Kapton® (polyimide) substrate and transferred to a 500 µm PDMS substrate, using a 3D-extrusion-based printing method. The main features of our fabrication process consist of short-time customization implementation, fast small-to-medium batch production, ease of electrochemical spectroscopy measurements, and very good resolution for an extrusion-based printing method (100 µm). The sensors were designed for future integration into a smart wound dressing for wound monitoring and other biomedical applications. We increased their sensibility with electro-deposited gold nanoparticles. To assess the biosensors' functionality, we performed surface functionalization with specific anti-N-protein antibodies for SARS-CoV 2 virus, with promising preliminary results.

Influence of Nitrogen-Doped Carbon Dot and Silver Nanoparticle Modified Carbon Paste Electrodes on the Potentiometric Determination of Tobramycin Sulfate: A Comparative Study

Two inexpensive and simple methods for synthesis of carbon nanodots were applied and compared to each other, namely a hydrothermal and microwave-assisted method. The synthesized carbon nanodots were characterized using transmission electron microscopy (TEM), ultraviolet-visible (UV-Vis), photoluminescence (PL), Fourier transform-infrared spectroscopy (FTIR), and X-ray diffraction (XRD). The synthesized microwave carbon nanodots had smaller particle size and were thus chosen for better electrochemical performance. Therefore, they were used for our modification process. The proposed electrodes performance characteristics were evaluated according to the IUPAC guidelines, showing linear response in the concentration range 10−6–10−2, 10−7–10−2, and 10−8–10−2 M of tobramycin with a Nernstian slope of 52.60, 58.34, and 57.32 mV/decade for the bare, silver nanoparticle and carbon nanodots modified carbon paste electrodes, respectively. This developed potentiometric method was used for quantification of tobramycin in its co-formulated dosage form and spiked human plasma with good recovery percentages and without interference of the co-formulated drug loteprednol etabonate and excipients.

Continuous Glucose Monitoring in Hypoxic Environments Based on Water Splitting-Assisted Electrocatalysis

Conventional enzyme-based continuous glucose sensors in interstitial fluid usually rely on dissolved oxygen as the electron-transfer mediator to bring electrons from oxidase to electrode while generating hydrogen peroxide. This may lead to several problems. First, the sensor may provide biased detection results owing to fluctuation of oxygen in interstitial fluid. Second, the polymer coatings that regulate the glucose/oxygen ratio can affect the dynamic response of the sensor. Third, the glucose oxidation reaction continuously produces corrosive hydrogen peroxide, which may compromise the long-term stability of the sensor. Here, we introduce an oxygen-independent nonenzymatic glucose sensor based on water splitting-assisted electrocatalysis for continuous glucose monitoring. For the water splitting reaction (i.e., hydrogen evolution reaction), a negative pretreatment potential is applied to produce a localized alkaline condition at the surface of the working electrode for subsequent nonenzymatic electrocatalytic oxidation of glucose. The reaction process does not require the participation of oxygen;therefore, the problems caused by oxygen can be avoided. The nonenzymatic sensor exhibits acceptable sensitivity, reliability, and biocompatibility for continuous glucose monitoring in hypoxic environments, as shown by the in vitro and in vivo measurements. Therefore, we believe that it is a promising technique for continuous glucose monitoring, especially for clinically hypoxic patients.

Electrochemical Sensing Platform Based on Renewable Carbon Modified with Antimony Nanoparticles for Methylparaben Detection in Personal Care Products

This paper describes for the first time the surface modification of glassy carbon (GC) electrodes with bamboo-based renewable carbon (RC) and antimony nanoparticles (SbNPs) for the determination of methylparaben (MePa) in personal care products (PCPs). The synthesized RC-SbNP material was successfully characterized by scanning electron microcopy, energy-dispersive X-ray spectroscopy and cyclic voltammetry. The proposed sensor was applied in the detection of MePa using the optimized parameters by differential pulse voltammetry (DPV). The analytical range for detection of MePa was 0.2 to 9.0 µmol L−1, with limits of detection and quantification of 0.05 µmol L−1 and 0.16 µmol L−1, respectively. The determination of MePa in real PCP samples was performed using the proposed GC/RC-SbNP sensor by DPV and UV-vis spectrophotometry as comparative methodology. The use of RC-SbNP material for the development of electrochemical sensors brings a fresh approach to low-cost devices for MePa analysis.

Photocatalytic Degradation of Paracetamol under Simulated Sunlight by Four TiO2 Commercial Powders: An Insight into the Performance of Two Sub-Micrometric Anatase and Rutile Powders and a Nanometric Brookite Powder

The photocatalytic degradation of the emerging contaminant paracetamol in aqueous solution has been studied under 1 SUN (~1000 W m−2) in the presence of four commercial TiO2 powders, namely sub-micrometric anatase and rutile, and nanometric brookite and P25 (the popular anatase/rutile mixture used as a benchmark in most papers). The rutile powder showed low activity, whereas, interestingly, the anatase and the brookite powders outperformed P25 in terms of total paracetamol conversion to carboxylic acids, which, according to the literature, are the final products of its degradation. To explain such results, the physicochemical properties of the powders were studied by applying a multi-technique approach. Among the physicochemical properties usually affecting the photocatalytic performance of TiO2, the presence of some surface impurities likely deriving from K3PO4 (used as crystallization agent) was found to significantly affect the percentage of paracetamol degradation obtained with the sub-micrometric anatase powder. To confirm the role of phosphate, a sample of anatase, obtained by a lab synthesis procedure and having a "clean” surface, was used as a control, though characterized by nanometric particles and higher surface area. The sample was less active than the commercial anatase, but it was more active after impregnation with K3PO4. Conversely, the presence of Cl at the surface of the rutile did not sizably affect the (overall poor) photocatalytic activity of the powder. The remarkable photocatalytic activity of the brookite nanometric powder was ascribed to a combination of several physicochemical properties, including its band structure and nanoparticles size.

Discovering a Dihydrofluorescein Analogue as a Promising Fluorescence Substrate to HRP

Horseradish peroxidase (HRP) combined with its fluorescence substrates is attracting increasing attention for biochemical analysis. Amplex red is the most widely used fluorescence substrate to HRP;however, it suffers from some drawbacks, such as nonspecific responsiveness toward carboxylesterases. Discovering a new small molecular fluorescence substrate with improved sensitivity and selectivity for HRP is thus desired. Herein, three dihydrofluorescein derivatives (DCFHs) are presented to serve as HRP substrates through fluorescence turn-on methods. The most promising one, 2,7-dichloro-9-(2-(hydroxymethyl)phenyl)-9H-xanthene-3,6-diol (DCFH-1), exhibited excellent sensitivity in the detection of HRP. Moreover, DCFH-1 does not respond to carboxylesterase, thus holding advantages over Amplex red. In the further study, the detection reagent in the commercial ELISA kits was replaced with DCFH-1 to establish a new fluorescence ELISA, which works very well in the quantification of inflammatory cytokine biomarkers from in vitro models.

Impact of Surface Area on Sensitivity in Autonomously Reporting Sensing Hydrogel Nanomaterials for the Detection of Bacterial Enzymes

The rapid and selective detection of bacterial contaminations and bacterial infections in a non-laboratory setting using advanced sensing materials holds the promise to enable robust point-of-care tests and rapid diagnostics for applications in the medical field as well as food safety. Among the various possible analytes, bacterial enzymes have been targeted successfully in various sensing formats. In this current work, we focus on the systematic investigation of the role of surface area on the sensitivity in micro- and nanostructured autonomously reporting sensing hydrogel materials for the detection of bacterial enzymes. The colorimetric sensing materials for the detection of β-glucuronidase (ß-GUS) from Escherichia coli (E. coli) were fabricated by template replication of crosslinked pullulan acetoacetate (PUAA) and by electrospinning chitosan/polyethylene oxide nanofibers (CS/PEO NFs), both equipped with the chromogenic substrate 5-bromo-4-chloro-3-indolyl-β-D-glucuronide. The investigation of the dependence of the initial reaction rates on surface area unveiled a linear relationship of rate and thereby time to observe a signal for a given concentration of bacterial enzyme. This knowledge was exploited in nanoscale sensing materials made of CS/PEO NFs with diameters of 295 ± 100 nm. Compared to bulk hydrogel slabs, the rate of hydrolysis was significantly enhanced in NFs when exposed to bacteria suspension cultures and thus ensuring a rapid detection of living E. coli that produces the enzyme β-GUS. The findings afford generalized design principles for the improvement of known and novel sensing materials towards rapid detection of bacteria by nanostructuring in medical and food related settings.

Rutile-TiO2/PtO2 Glass Coatings Disinfects Aquatic Legionella pneumophila via Morphology Change and Endotoxin Degradation under LED Irradiation

Legionella pneumophila (L. pneumophila) is the causative agent of Legionnaires’ disease and Pontiac fever, collectively known as legionellosis. L. pneumophila infection occurs through inhalation of contaminated aerosols from water systems in workplaces and institutions. The development of disinfectants that can eliminate L. pneumophila in such water systems without evacuating people is needed to prevent the spread of L. pneumophila. Photocatalysts are attractive disinfectants that do not harm human health. In particular, the TiO2 photocatalyst kills L. pneumophila under various conditions, but its mode of action is unknown. Here, we confirmed the high performance of TiO2 photocatalyst containing PtO2 via the degradation of methylene blue (half-value period: 19.2 min) and bactericidal activity against Escherichia coli (half-value period: 15.1 min) in water. Using transmission electron microscopy, we demonstrate that the disinfection of L. pneumophila (half-value period: 6.7 min) by TiO2 photocatalyst in water is accompanied by remarkable cellular membrane and internal damage to L. pneumophila. Assays with limulus amebocyte lysate and silver staining showed the release of endotoxin from L. pneumophila due to membrane damage and photocatalytic degradation of this endotoxin. This is the first study to demonstrate the disinfection mechanisms of TiO2 photocatalyst, namely, via morphological changes and membrane damage of L. pneumophila. Our results suggest that TiO2 photocatalyst might be effective in controlling the spread of L. pneumophila.

Environmental and Pharmacokinetic Aspects of Zeolite/Pharmaceuticals Systems—Two Facets of Adsorption Ability

Zeolites belong to aluminosilicate microporous solids, with strong and diverse catalytic activity, which makes them applicable in almost every kind of industrial process, particularly thanks to their eco-friendly profile. Another crucial characteristic of zeolites is their tremendous adsorption capability. Therefore, it is self-evident that the widespread use of zeolites is in environmental protection, based primarily on the adsorption capacity of substances potentially harmful to the environment, such as pharmaceuticals, pesticides, or other industry pollutants. On the other hand, zeolites are also recognized as drug delivery systems (DDS) carriers for numerous pharmacologically active agents. The enhanced bioactive ability of DDS zeolite as a drug carrying nanoplatform is confirmed, making this system more specific and efficient, compared to the drug itself. These two applications of zeolite, in fact, illustrate the importance of (ir)reversibility of the adsorption process. This review gives deep insight into the balance and dynamics that are established during that process, i.e., the interaction between zeolites and pharmaceuticals, helping scientists to expand their knowledge necessarily for a more effective application of the adsorption phenomenon of zeolites.

Antimicrobial Activity of a Titanium Dioxide Additivated Thermoset

The transmission of pathogens via surfaces poses a major health problem, particularly in hospital environments. Antimicrobial surfaces can interrupt the path of spread, while photocatalytically active titanium dioxide (TiO2) nanoparticles have emerged as an additive for creating antimicrobial materials. Irradiation of such particles with ultraviolet (UV) light leads to the formation of reactive oxygen species that can inactivate bacteria. The aim of this research was to incorporate TiO2 nanoparticles into a cellulose-reinforced melamine-formaldehyde resin (MF) to obtain a photocatalytic antimicrobial thermoset, to be used, for example, for device enclosures or tableware. To this end, composites of MF with 5, 10, 15, and 20 wt% TiO2 were produced by ultrasonication and hot pressing. The incorporation of TiO2 resulted in a small decrease in tensile strength and little to no decrease in Shore D hardness, but a statistically significant decrease in the water contact angle. After 48 h of UV irradiation, a statistically significant decrease in tensile strength for samples with 0 and 10 wt% TiO2 was measured but with no statistically significant differences in Shore D hardness, although a statistically significant increase in surface hydrophilicity was measured. Accelerated methylene blue (MB) degradation was measured during a further 2.5 h of UV irradiation and MB concentrations of 12% or less could be achieved. Samples containing 0, 10, and 20 wt% TiO2 were investigated for long-term UV stability and antimicrobial activity. Fourier-transform infrared spectroscopy revealed no changes in the chemical structure of the polymer, due to the incorporation of TiO2, but changes were detected after 500 h of irradiation, indicating material degradation. Specimens pre-irradiated with UV for 48 h showed a total reduction in Escherichia coli when exposed to UV irradiation.

Phytochemicals As a Potential Inhibitor of COVID-19: An In-Silico Perspective

The current research has centered on the use of pharmacological and binding affinity methods to test the 36 compounds as bioactive constituents’ inhibitors for COVID-19. Six compounds out of 36 phytoconstituents (rutin, quercetin, catechin gallate, rhamnetin, campesterol and stigmasterol) have demonstrated outstanding molecular docking and drug-like properties as HIV inhibitors Lopinavir and Indinavir. Interestingly, the lowest binding energies (LBE) and the inhibition constant (Ki) have showed that these compounds are able to bind to the P-glycoprotein substrate of 3CLpro and Nsp15. Interestingly, rutin has been found to be an excellent potential inhibitor for COVID-19 proteins because it has the best LBE score and Ki value than those of other compounds, and of its ability to form strong H-bonds with COVID-19 proteins. The compounds that come next to the rutin compound are stigmasterol and campesterol. As a result, these compounds are considered possible novel inhibitors of COVID-19. In order to validate the computational results, more in vitro and in vivo investigations are required to support the findings of this research.

Analysis and Dynamic Monitoring of Indoor Air Quality Based on Laser-Induced Breakdown Spectroscopy and Machine Learning

The air quality of the living area influences human health to a certain extent. Therefore, it is particularly important to detect the quality of indoor air. However, traditional detection methods mainly depend on chemical analysis, which has long been criticized for its high time cost. In this research, a rapid air detection method for the indoor environment using laser-induced breakdown spectroscopy (LIBS) and machine learning was proposed. Four common scenes were simulated, including burning carbon, burning incense, spraying perfume and hot shower which often led to indoor air quality changes. Two steps of spectral measurements and algorithm analysis were used in the experiment. Moreover, the proposed method was found to be effective in distinguishing different kinds of aerosols and presenting sensitivity to the air compositions. In this paper, the signal was isolated by the forest, so the singular values were filtered out. Meanwhile, the spectra of different scenarios were analyzed via the principal component analysis (PCA), and the air environment was classified by K-Nearest Neighbor (KNN) algorithm with an accuracy of 99.2%. Moreover, based on the establishment of a high-precision quantitative detection model, a back propagation (BP) neural network was introduced to improve the robustness and accuracy of indoor environment. The results show that by taking this method, the dynamic prediction of elements concentration can be realized, and its recognition accuracy is 96.5%.

Hybrid Nanocomposites of Plasmonic Metal Nanostructures and 2D Nanomaterials for Improved Colorimetric Detection

Plasmonic phenomena and materials have been extensively investigated for a long time and gained popularity in the last few years, finding in the design of the biosensors platforms promising applications offering devices with excellent performances. Hybrid systems composed of graphene, or other 2D materials, and plasmonic metal nanostructures present extraordinary optical properties originated from the synergic connection between plasmonic optical effects and the unusual physicochemical properties of 2D materials, thus improving their application in a broad range of fields. In this work, firstly, an overview of the structures and properties of 2D nanomaterials will be provided along with the physics of surface plasmon resonance and localized surface plasmon resonance. In the second part of the work, some examples of colorimetric biosensors exploiting the outstanding properties of hybrids nanocomposites will be presented. Finally, concluding perspectives on the actual status, challenges, and future directions in plasmonic sensing biosensing will be provided. Special emphasis will be given to how this technology can be used to support digitalization and virtualization in pandemic handling.

CeO2-Based Heterogeneous Catalysts in Dry Reforming Methane and Steam Reforming Methane: A Short Review

Transitioning to lower carbon energy and environment sustainability requires a reduction in greenhouse gases such as carbon dioxide (CO2) and methane (CH4) that contribute to global warming. One of the most actively studied rare earth metal catalysts is cerium oxide (CeO2) which produces remarkable improvements in catalysts in dry reforming methane. This paper reviews the management of CO2 emissions and the recent advent and trends in bimetallic catalyst development utilizing CeO2 in dry reforming methane (DRM) and steam reforming methane (SRM) from 2015 to 2021 as a way to reduce greenhouse gas emissions. This paper focus on the identification of key trends in catalyst preparation using CeO2 and the effectiveness of the catalysts formulated.

Determination of Ascorbic Acid in Pharmaceuticals and Food Supplements with the New Potassium Ferrocyanide-Doped Polypyrrole-Modified Platinum Electrode Sensor

This paper reports the results obtained from the determination of ascorbic acid with platinum-based voltammetric sensors modified with potassium hexacyanoferrate-doped polypyrrole. The preparation of the modified electrodes was carried out by electrochemical polymerization of pyrrole from aqueous solutions, using chronoamperometry. Polypyrrole films were deposited on the surface of the platinum electrode, by applying a constant potential of 0.8 V for 30 s. The thickness of the polymer film was calculated from the chronoamperometric data, and the value was 0.163 μm. Cyclic voltammetry was the method used for the Pt/PPy-FeCN electrode electrochemical characterization in several types of solution, including KCl, potassium ferrocyanide, and ascorbic acid. The thin doped polymer layer showed excellent sensitivity for ascorbic acid detection. From the voltammetric studies carried out in solutions of different concentrations of ascorbic acid, ranging from 1 to 100 × 10−6 M, a detection limit of 2.5 × 10−7 M was obtained. Validation of the analyses was performed using pharmaceutical products with different concentrations of ascorbic acid, from different manufacturers and presented in various pharmaceutical forms, i.e., intravascular administration ampoules, chewable tablets, and powder for oral suspension.

Welcome to Physchem: Status and Prospects

The field of physical chemistry has been gaining in importance;indeed, being an intrinsically multidisciplinary area focused, in particular, on studies of how matter behaves on a molecular and atomic level, it is a field of primary importance for the development of many novel technologies, from fuel cells to batteries to catalytic systems. With a scope including the nexus of underlying physics, chemistry, and computational mathematics as well as data-driven approaches including machine learning and artificial intelligence applied to problems of physical chemistry, PhysChem is well positioned to attract innovative papers and enjoy a sustained rise in impact in the near future. Institutional Review Board Statement Not applicable.

Plasmonic Nanomaterials for Colorimetric Biosensing: A Review

In the last few decades, plasmonic colorimetric biosensors raised increasing interest in bioanalytics thanks to their cost-effectiveness, responsiveness, and simplicity as compared to conventional laboratory techniques. Potential high-throughput screening and easy-to-use assay procedures make them also suitable for realizing point of care devices. Nevertheless, several challenges such as fabrication complexity, laborious biofunctionalization, and poor sensitivity compromise their technological transfer from research laboratories to industry and, hence, still hamper their adoption on large-scale. However, newly-developing plasmonic colorimetric biosensors boast impressive sensing performance in terms of sensitivity, dynamic range, limit of detection, reliability, and specificity thereby continuously encouraging further researches. In this review, recently reported plasmonic colorimetric biosensors are discussed with a focus on the following categories: (i) on-platform-based (localized surface plasmon resonance, coupled plasmon resonance and surface lattice resonance);(ii) colloid aggregation-based (label-based and label free);(iii) colloid non-aggregation-based (nanozyme, etching-based and growth-based).

Design and Characterization of a Microwave Transducer for Gas Sensing Applications

Gas sensors have wide applications in several fields, spanning diverse areas such as environmental monitoring, healthcare, defense, and the evaluation of personal and occupational exposure to hazardous chemicals. Different typologies of gas sensors have been proposed over the years, such as optical, electrochemical, and metal oxide gas sensors. In this paper, a relatively new typology of gas sensors is explored: the microwave gas sensor. It consists of a combination of a microwave transducer with a nanostructured sensing material deposited on an interdigitated capacitor (IDC). The device is designed and fabricated on a Rogers substrate (RO4003C) using microstrip technology, and investigated as a microwave transducer over the frequency range from 1 GHz to 6 GHz by measuring the scattering (S) parameters in response to gas adsorption and desorption. The sensing material is based on a nano-powder of barium titanate oxalate with a coating of urea (BaTiO(C2O4)2/CO(NH2)2). It is deposited on the IDC surface by drop coating, thus creating a sensing film. The developed prototype has been tested toward different oxygen (O2) concentrations and exhibits a sensitivity of 28 kHz/%O2. Special attention has been devoted to the measurement process. Besides the canonical short-open-load-thru (SOLT) calibration of the measured S-parameters, a thru-reflect-line (TRL) calibration has been performed in order to get rid of the parasitic electromagnetic (EM) contributions of the board connectors and the feedlines, thus moving the measurement reference planes to the edges of the IDC.