ACS Measurement Science Au最新文献

In this paper, we report on a printable glass-based manufacturing method and a new proof-of-concept colorimetric signal readout scheme for a dielectric barrier discharge (DBD)-type helium plasma photoionization detector. The sensor consists of a millimeter-sized glass chamber manufactured using a printable glass suspension. Plasma inside the chip is generated using a custom-built power supply (900 V and 83.6 kHz), and the detector uses ∼5 W of power. Our new detection scheme is based on detecting the change in the color of plasma after the introduction of target gases. The change in color is first captured by a smartphone camera as a video output. The recorded video is then processed and converted to an image light intensity vs retention time plot (gas chromatogram) using three standard color space models (red, green, blue (RGB), hue, saturation, lightness (HSL), and hue, saturation, value (HSV)) with RGB performing the best among the three models. We successfully detected three different categories of volatile organic compounds using our new detection scheme and a 30-m-long gas chromatography column: (1) straight-chain alkanes (n-pentane, n-hexane, n-heptane, n-octane, and n-nonane), (2) aromatics (benzene, toluene, and ethylbenzene), and (3) polar compounds (acetone, ethanol, and dichloromethane). The best limit of detection of 10 ng was achieved for benzene at room temperature. Additionally, the device showed excellent performance for different types of sample mixtures consisting of three and five compounds. Our new detector readout method combined with our ability to print complex glass structures provides a new research avenue to analyze complex gas mixtures and their components.

Online techniques for the quantitative analysis of reaction products have many advantages over offline methods. However, owing to the low product formation rates in electrochemical reactions, few of these techniques can be coupled to electrochemistry. An exception is differential electrochemical mass spectrometry (DEMS), which gains increasing popularity not least because of its high time resolution in the sub-second regime. DEMS is often combined with a dual thin-layer cell (a two-compartment flow cell), which helps to mitigate a number of problems that arise due to the existence of a vacuum|electrolyte interface. However, the efficiency with which this cell transfers volatile reaction products into the vacuum of the mass spectrometer is far below 100%. Therefore, a calibration constant that considers not only the sensitivity of the DEMS setup but also the transfer efficiency of the dual thin-layer cell is needed to translate the signals observed in the mass spectrometer into electrochemical product formation rates. However, it can be challenging or impossible to design an experiment that yields such a calibration constant. Here, we show that the transfer efficiency of the dual thin-layer cell depends on the diffusion coefficient of the analyte. Based on this observation, we suggest a two-point calibration method. That is, a plot of the logarithm of the transfer efficiencies determined for H₂ and O₂ versus the logarithm of their diffusion coefficients defines a straight line. Extrapolation of this line to the diffusion coefficient of another analyte yields a good estimate of its transfer efficiency. This is a versatile and easy calibration method, because the transfer efficiencies of H₂ and O₂ are readily accessible for a large range of electrode–electrolyte combinations.

Fluorescence-based single-molecule approaches have helped revolutionize our understanding of chemical and biological mechanisms. Unfortunately, these methods are only suitable at low concentrations of fluorescent molecules so that single fluorescent species of interest can be successfully resolved beyond background signal. The application of these techniques has therefore been limited to high-affinity interactions despite most biological and chemical processes occurring at much higher reactant concentrations. Fortunately, recent methodological advances have demonstrated that this concentration barrier can indeed be broken, with techniques reaching concentrations as high as 1 mM. The goal of this Review is to discuss the challenges in performing single-molecule fluorescence techniques at high-concentration, offer applications in both biology and chemistry, and highlight the major milestones that shatter the concentration barrier. We also hope to inspire the widespread use of these techniques so we can begin exploring the new physical phenomena lying beyond this barrier.

In this article, we present a toolset to fully leverage a previously developed transcutaneous oxygenation monitor (TCOM) wearable technology to accurately measure skin oxygenation values. We describe numerical models and experimental characterization techniques that allow for the extraction of precise tissue oxygenation measurements. The numerical model is based on an inverse boundary problem of the parabolic equation with Dirichlet boundary conditions. To validate this model and characterize the diffusion of oxygen through the oxygen sensing materials, we designed a series of control/calibration experiments modeled after the device’s clinical application using oxygenation values in the physiological range expected for healthy tissue. Our results demonstrate that it is possible to obtain accurate tissue pO₂ measurements without the need for long equilibration times with a small wearable device.

The targeted screening and sequencing approaches for COVID-19 surveillance need to be adjusted to fit the evolving surveillance objectives which necessarily change over time. We present the development of variant screening assays that can be applied to new targets in a timely manner and enable multiplexing of targets for efficient implementation in the laboratory. By targeting the HV69/70 deletion for Alpha, K417N for Beta, K417T for Gamma, and HV69/70 deletion plus K417N for sub-variants BA.1, BA.3, BA.4, and BA.5 of Omicron, we achieved simultaneous detection and differentiation of Alpha, Beta, Gamma, and Omicron in a single assay. Targeting both T478K and P681R mutations enabled specific detection of the Delta variant. The multiplex assays used in combination, targeting K417N and T478K, specifically detected the Omicron sub-variant BA.2. The limits of detection for the five variants of concern were 4–16 copies of the viral RNA per reaction. Both assays achieved 100% clinical sensitivity and 100% specificity. Analyses of 377 clinical samples and 24 wastewater samples revealed the Delta variant in 100 clinical samples (nasopharyngeal and throat swab) collected in November 2021. Omicron BA.1 was detected in 79 nasopharyngeal swab samples collected in January 2022. Alpha, Beta, and Gamma variants were detected in 24 wastewater samples collected in May–June 2021 from two major cities of Alberta (Canada), and the results were consistent with the clinical cases of multiple variants reported in the community.

Non-invasive liquid biopsy assays for blood-circulating biomarkers of cancer allow both its early diagnosis and treatment monitoring. Here, we assessed serum levels of protein HER-2/neu, overexpressed in a number of aggressive cancers, by the cellulase-linked sandwich bioassay on magnetic beads. Instead of traditional antibodies we used inexpensive reporter and capture aptamer sequences, transforming the enzyme-linked immuno-sorbent assay (ELISA) into an enzyme-linked aptamer-sorbent assay (ELASA). The reporter aptamer was conjugated to cellulase, whose digestion of nitrocellulose film electrodes resulted in the electrochemical signal change. ELASA, optimized relative aptamer lengths (dimer vs monomer and trimer), and assay steps allowed 0.1 fM detection of HER-2/neu in the 10% human serum in 1.3 h. Urokinase plasminogen activator and thrombin as well as human serum albumin did not interfere, and liquid biopsy analysis of serum HER-2/neu was similarly robust but 4 times faster and 300 times cheaper than both electrochemical and optical ELISA. Simplicity and low cost of cellulase-linked ELASA makes it a perspective diagnostic tool for fast and accurate liquid biopsy detection of HER-2/neu and of other proteins for which aptamers are available.

The development and increase in the number of crops recently have led to the requirement for greater efficiency in world food production and greater consumption of pesticides. In this context, the widespread use of pesticides has affected the decrease in the population of pollinating insects and has caused food contamination. Therefore, simple, low-cost, and quick analytical methods can be interesting alternatives for checking the quality of foods such as honey. In this work, we propose a new additively manufactured (3D-printed) device inspired by a honeycomb cell, with 6 working electrodes for the direct electrochemical analysis of methyl parathion by reduction process monitoring in food and environmental samples. Under optimized parameters, the proposed sensor presented a linear range between 0.85 and 19.6 μmol L^–1, with a limit of detection of 0.20 μmol L^–1. The sensors were successfully applied in honey and tap water samples by using the standard addition method. The proposed honeycomb cell made of polylactic acid and commercial conductive filament is easy to construct, and there is no need for chemical treatments to be used. These devices based on 6 working electrodes array are versatile platforms for rapid, highly repeatable analysis in food and environment, capable of performing detection in low concentrations.

Lyme disease, caused by infection with pathogenic Borrelia bacteria, has emerged as a pervasive illness throughout North America and many other regions of the world in recent years, owing in part to climate-mediated habitat expansion of the tick vectors. Standard diagnostic testing has remained largely unchanged over the past several decades and is indirect, relying on detection of antibodies against the Borrelia pathogen, rather than detection of the pathogen itself. The development of new rapid, point-of-care tests for Lyme disease that directly detects the pathogen could drastically improve patient health by enabling faster and more frequent testing that could better inform patient treatment. Here, we describe a proof-of-concept electrochemical sensing approach to the detection of the Lyme disease-causing bacteria, which utilizes a biomimetic electrode to interact with the Borrelia bacteria that induce impedance alterations. In addition, the catch-bond mechanism between bacterial BBK32 protein and human fibronectin protein, which exhibits improved bond strength with increased tensile force, is tested within an electrochemical injection flow-cell to achieve Borrelia detection under shear stress.