Charlie Tobias, Daniel López-Puertollano, Antonio Abad-Somovilla, Josep V. Mercader, Antonio Abad-Fuentes, Knut Rurack
{"title":"Development of Simple and Rapid Bead-Based Cytometric Immunoassays Using Superparamagnetic Hybrid Core–Shell Microparticles","authors":"Charlie Tobias, Daniel López-Puertollano, Antonio Abad-Somovilla, Josep V. Mercader, Antonio Abad-Fuentes, Knut Rurack","doi":"10.1021/acsmeasuresciau.4c00038","DOIUrl":"https://doi.org/10.1021/acsmeasuresciau.4c00038","url":null,"abstract":"Flow cytometry-based immunoassays are valuable in biomedical research and clinical applications due to their high throughput and multianalyte capability, but their adoption in areas such as food safety and environmental monitoring is limited by long assay times and complex workflows. Rapid, simplified bead-based cytometric immunoassays are needed to make these methods viable for point-of-need applications, especially with the increasing accessibility of miniaturized cytometers. This work introduces superparamagnetic hybrid polystyrene-silica core–shell microparticles as promising alternatives to conventional polymer beads in competitive cytometric immunoassays. These beads, featuring high specificity, sensitivity, and excellent handling capabilities via magnetic separation, were evaluated with three different antibodies and binding methods, showing variations in signal intensity based on the antibody and its attachment method. The optimal performance was achieved through a secondary antibody binding approach, providing strong and consistent signals with minimal uncertainty. The optimized protocol made it possible to achieve a detection limit of 0.025 nM in a total assay time of only 15 min and was successfully used to detect ochratoxin A (OTA) in raw flour samples. This work highlights the potential of these beads as versatile tools for flow cytometry-based immunoassays, with significant implications for food safety, animal health, environmental monitoring, and clinical diagnostics.","PeriodicalId":29800,"journal":{"name":"ACS Measurement Science Au","volume":"1 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-09-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142256997","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Zia ul Quasim Syed, Sathya Samaraweera, Zhuo Wang, James Kelby Schrader, Colton Scott, Joshua Schut, Dozier Johnson Smith, Joshua D. Ramsey, Sadagopan Krishnan
{"title":"Colorimetric Hybridization Sensor for DNA Mimic of a SARS-CoV-2 RNA Marker: Direct and Inverse Bioanalysis","authors":"Zia ul Quasim Syed, Sathya Samaraweera, Zhuo Wang, James Kelby Schrader, Colton Scott, Joshua Schut, Dozier Johnson Smith, Joshua D. Ramsey, Sadagopan Krishnan","doi":"10.1021/acsmeasuresciau.4c00043","DOIUrl":"https://doi.org/10.1021/acsmeasuresciau.4c00043","url":null,"abstract":"This article presents a colorimetric visual biosensor designed for direct application in undiluted biofluids, which holds significant promise for point-of-need applications. Unlike traditional biosensors that struggle with heavily diluted sample matrices, the presented biosensor does not require any instrumentation or trained personnel, making it highly practical. The sensor features an oligonucleotide probe covalently attached to magnetically separable magnetite (Fe<sub>3</sub>O<sub>4</sub>) particles. This probe selectively captures a DNA mimic of the SARS-CoV-2 RNA sequence via a base-pair hybridization. The DNA mimic oligomer sequence was tested in a buffer solution, undiluted serum, and undiluted salivary biofluids. A second complementary hybridization sequence with a biotin tag was used to bind the target oligomer already hybridized to the magnetic particle-conjugated capture probe. Subsequent detection of the target oligomer was accomplished through high-affinity selective binding of streptavidin-peroxidase labels with the detection probe biotin units for visual colorimetric detection in the presence of 3,3′,5,5′-tetramethylbenzidine and hydrogen peroxide. Inverse assaying of the unbound-free streptavidin-peroxidase labels left in the detection reagent solution offered a reverse trend to the target oligomer concentration, as anticipated. We obtained detection limits of 1 fM (buffer assay), 1 pM (undiluted serum assay), and 1 pM (undiluted saliva assay) and with the linear ranges of 1 fM–10 nM (buffer assay), 1 pM–1 nM (undiluted serum assay), and 1 pM–1 nM (undiluted saliva assay), respectively. The assays in different biofluids allowed for the estimation of the analytical performance and the effect of sample matrices on the detection limits and calibration sensitivity.","PeriodicalId":29800,"journal":{"name":"ACS Measurement Science Au","volume":"15 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-09-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142194453","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Arthur Langlard, Hassiba Smida, Romain Chevalet, Christine Thobie-Gautier, Mohammed Boujtita, Estelle Lebègue
{"title":"Computer-Assisted Processing of Current Step Signals in Single Blocking Impact Electrochemistry","authors":"Arthur Langlard, Hassiba Smida, Romain Chevalet, Christine Thobie-Gautier, Mohammed Boujtita, Estelle Lebègue","doi":"10.1021/acsmeasuresciau.4c00046","DOIUrl":"https://doi.org/10.1021/acsmeasuresciau.4c00046","url":null,"abstract":"Current step signals related to single-entity collisions in blocking impact electrochemistry were analyzed by computer-assisted processing for estimating the size distributions of various particles. In this work, three different types of entities were studied by single blocking impact electrochemistry: polystyrene nanospheres (350 nm diameter) and microspheres (1 μm diameter), phospholipid liposomes (300 nm diameter) and two different strains of Gram-negative bacillus bacteria (<i>Escherichia coli</i> and <i>Shewanella oneidensis</i>). The size estimations of these different entities from the current step signal analysis were compared and discussed according to the shape and size of each entity. From the magnitude of the current step transient, the size distribution of each entity was calculated by a new computer program assisting in the detection and analysis of single impact events in chronoamperometry measurements. The data processing showed that the size distributions obtained from the electrochemical data agreed with the dynamic light scattering and atomic force microscopy data for nanospheres and liposomes. In contrast, the size estimation calculated from the electrochemical data was underestimated for microspheres and bacteria. We demonstrated that our computer program was efficient for detecting and analyzing the collision events in single blocking impact electrochemistry for various entities from spherical hard nanoparticles to micrometer-sized rod-shaped living bacteria.","PeriodicalId":29800,"journal":{"name":"ACS Measurement Science Au","volume":"107 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-09-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142227711","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Super-Resolution Microscopic Imaging of Lipid Droplets in Living Cells via Carbonized Polymer Dot-Based Polarity-Responsive Nanoprobe","authors":"Zepeng Huo, Zitong Yu, Weiqing Xu, Shuping Xu","doi":"10.1021/acsmeasuresciau.4c00049","DOIUrl":"https://doi.org/10.1021/acsmeasuresciau.4c00049","url":null,"abstract":"Lipid droplets (LDs) are dynamic subcellular organelles that participate in various physiological processes, and their abnormality can also lead to various diseases. Tracing the dynamics of LDs in living cells will be valuable for understanding cell physiological states. Here, we employed a structured light illumination super-resolution imaging assisted with a carbonized polymer dot (CPD)-based fluorescence nanoprobe to track the travel paths of LDs and other organelles. The CPDs we developed are highly biocompatible with living cells and exhibit a highly sensitive response to solvent polarity, allowing for high specificity in staining LDs in living cells. Aided by these nanoprobes, we successfully observed many real-time LD-involved dynamics in living cells, such as intracellular LD interactions, communications with other organelles, and dynamic behaviors under external stimuli (oxidative stress inducer). These studies deepen our comprehension of the physiological role of LDs and drive the advancement of super-resolution fluorescent probes.","PeriodicalId":29800,"journal":{"name":"ACS Measurement Science Au","volume":"24 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-09-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142225030","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Georg Schwendt, Andrey V. Kalinichev, Sergey M. Borisov, Klaus Koren
{"title":"Simultaneous Imaging of Temperature and Oxygen by Utilizing Thermally Activated Delayed Fluorescence and Phosphorescence of a Single Indicator","authors":"Georg Schwendt, Andrey V. Kalinichev, Sergey M. Borisov, Klaus Koren","doi":"10.1021/acsmeasuresciau.4c00040","DOIUrl":"https://doi.org/10.1021/acsmeasuresciau.4c00040","url":null,"abstract":"Chemical gradients are essential in biological systems, affecting processes like microbial activity in soils and nutrient cycling. Traditional tools, such as microsensors, offer high-resolution data but are limited to one-dimensional measurements. Planar optodes allow for two-dimensional (2D) and three-dimensional (3D) chemical imaging but are often sensitive to temperature changes. This study presents an advanced dual-emission optical sensor that simultaneously measures temperature and oxygen using a modified platinum(II) meso-tetrakis(3,5-di<i>tert</i>-butylphenyl)-tetra(2-<i>tert</i>-butyl-1,4-naphthoquinono)porphyrin. The ratio between thermally activated delayed fluorescence and phosphorescence was optimized by modifying platinum(II) naphthoquinonoporphyrin with <i>tert</i>-butyl groups which simultaneously improved solubility in apolar solvents and polymer matrix (polystyrene). This dual-function sensor enables two-parameter chemical imaging with a consumer-grade RGB camera or a hyperspectral camera. We demonstrated 2D visualization of temperature and oxygen distribution in a model soil system. The RGB camera provided rapid and cost-effective imaging, while the hyperspectral camera offered more detailed spectral information despite some limitations. Our findings revealed the formation of a stable temperature gradient and oxygen depletion, driven by water content and temperature-sensitive microbial activity. This dual O<sub>2</sub>/T sensor, with further potential improvements, shows considerable promise for advanced multiparameter sensing in complex biological and environmental studies, providing deeper insights into dynamic microenvironments.","PeriodicalId":29800,"journal":{"name":"ACS Measurement Science Au","volume":"14 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-09-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142194490","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Jian Wang, Donghui Hong, Jili Li, Linlin Wang, Yuqi Xie, Jun Da, Yanlan Liu
{"title":"Activatable Multiplexed 19F NMR Probes for Dynamic Monitoring of Biomarkers Associated with Cellular Senescence","authors":"Jian Wang, Donghui Hong, Jili Li, Linlin Wang, Yuqi Xie, Jun Da, Yanlan Liu","doi":"10.1021/acsmeasuresciau.4c00045","DOIUrl":"https://doi.org/10.1021/acsmeasuresciau.4c00045","url":null,"abstract":"Simultaneous detection of multiple biomarkers is crucial to achieve specific and dynamic analysis of cellular senescence, given its intrinsic high heterogeneity. Current approaches for senescence detection largely rely on fluorescence imaging, but fluorescent probes inevitably suffer from issues including autofluorescence and spectral overlap when being applied for the simultaneous detection of multiple biomarkers. Herein, we report an alternative strategy and design activatable multiplexed senoprobes based on <sup>19</sup>F NMR for dynamic monitoring of cellular senescence. Differing from previous approaches, our strategy has two unique advantages. First, this strategy utilizes the changes in the <sup>19</sup>F chemical shift as the signal output, which features by its fingerprint and quantifiable characters, thereby significantly enhancing the detection throughput toward biomarkers with minimized spectral overlapping. Second, the background signal is minimized, benefiting from the extremely low abundance of F in biological samples, and the detection accuracy can thus be improved. As a proof of concept, two activatable <sup>19</sup>F NMR molecular probes are synthesized that specially respond to two key senescence-associated biomarkers (β-gal and ROS) and have been successfully demonstrated for dynamical and quantitative assessment of the changes of these biomarkers in different cellular models of senescence, without causing obvious cytotoxicity. Owing to the flexible molecular design, this work may offer a useful platform to create diversified <sup>19</sup>F NMR senoprobes for deep understanding of cellular senescence across a wide range of aging-related diseases.","PeriodicalId":29800,"journal":{"name":"ACS Measurement Science Au","volume":"22 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-08-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142194494","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Decoupling Variable Capacitance and Diffusive Components of Active Solid–Liquid Interfaces with Flex Points","authors":"Liam Deehan, Ajeet Kumar Kaushik, Ganga Ram Chaudhary, Pagona Papakonstantinou, Nikhil Bhalla","doi":"10.1021/acsmeasuresciau.4c00057","DOIUrl":"https://doi.org/10.1021/acsmeasuresciau.4c00057","url":null,"abstract":"Understanding the current transport characteristics of electrode interfaces is essential for optimizing device performance across a wide range of applications including bio-/chemical sensing and energy storage sectors. Cyclic voltammetry (CV) is a popular method for studying interfacial properties, particularly those involving redox systems. However, it remains challenging to differentiate between electron movements that contribute to capacitive and diffusive behaviors. In this study, we introduce a technique called flex point analysis, which uses a single differentiation step to separate capacitive and diffusive electron movements at the electrode interface during a redox reaction. Our results show that the variable capacitance at the electrode surface exhibited both positive and negative values on the order of 10<sup>–6</sup> (micro) Farad. This approach provides a clearer understanding of interfacial electron dynamics, enhancing the interpretation of CV data and potentially improving the design and optimization of related materials and devices.","PeriodicalId":29800,"journal":{"name":"ACS Measurement Science Au","volume":"38 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-08-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142194493","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Laíse Aparecida Fonseca Dinali, Anny Talita Maria da Silva, Keyller Bastos Borges
{"title":"Silver Core Coated with Molecularly Imprinted Polymer as Adsorbent in Pipet-Tip Solid Phase Extraction for Neonicotinoids Determination from Coconut Water","authors":"Laíse Aparecida Fonseca Dinali, Anny Talita Maria da Silva, Keyller Bastos Borges","doi":"10.1021/acsmeasuresciau.4c00036","DOIUrl":"https://doi.org/10.1021/acsmeasuresciau.4c00036","url":null,"abstract":"In this work, we report an innovative adsorbent named Ag-MPS@MIP that has a core@shell structure, i.e., silver nanoparticles modified with 3-methacryloxypropyltrimethoxysilane as the core and molecularly imprinted polymer based on methacrylic acid as its shell. Thiamethoxam, imidacloprid, and acetamiprid were extracted from coconut water samples using Ag-MPS@MIP in pipet-tip solid phase, prior to high-performance liquid chromatography analysis. The separation was carried out on isocratic mode using a mobile phase consisting of C18 column (Phenomenex, 150 mm × 4.6 mm, 5 μm), ultrapure water acidified with 0.3% phosphoric acid:acetonitrile (78:22, v/v), flow rate at 1.0 mL min<sup>–1</sup>, injection volume of 10 μL, temperature of 25 °C, and wavelength at 260 nm. The adsorbent and precursor materials were properly characterized by different instrumental techniques. The main factors affecting the recovery of analytes from coconut water samples by pipet-tip solid phase were optimized, such as sample volume (250 μL), sample pH (pH = 5.0), ionic strength (1%, m/v), washing solvent (300 μL ultrapure water), volume and type of eluent (500 μL methanol), amount of adsorbent (15 mg), cycle of percolation–dispensing (1×), and reuse (5×). Thereby, the neonicotinoids presented extraction recoveries between 82.80 and 96.36%, enrichment factor of 5, linearity ranged from 15 to 4000 ng mL<sup>–1</sup>, correlation coefficient (<i>r</i>) > 0.99, limit of detection of 5 ng mL<sup>–1</sup>, satisfactory selectivity, stability, and proper precision (RSD%: 0.52–9.64%) and accuracy (RE%: −5.19–6.45%). The method was successfully applied to real samples of coconut water.","PeriodicalId":29800,"journal":{"name":"ACS Measurement Science Au","volume":"25 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-08-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142194491","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Mushfeqa Iqfath, Syeda Nazifa Wali, Sara Amer, Emerson Hernly, Julia Laskin
{"title":"Nanospray Desorption Electrospray Ionization Mass Spectrometry Imaging (nano-DESI MSI): A Tutorial Review","authors":"Mushfeqa Iqfath, Syeda Nazifa Wali, Sara Amer, Emerson Hernly, Julia Laskin","doi":"10.1021/acsmeasuresciau.4c00028","DOIUrl":"https://doi.org/10.1021/acsmeasuresciau.4c00028","url":null,"abstract":"Nanospray desorption electrospray ionization (nano-DESI) is a liquid-based ambient mass spectrometry imaging (MSI) technique that enables visualization of analyte distributions in biological samples down to cellular-level spatial resolution. Since its inception, significant advancements have been made to the nano-DESI experimental platform to facilitate molecular imaging with high throughput, deep molecular coverage, and spatial resolution better than 10 μm. The molecular selectivity of nano-DESI MSI has been enhanced using new data acquisition strategies, the development of separation and online derivatization approaches for isobar separation and isomer-selective imaging, and the optimization of the working solvent composition to improve analyte extraction and ionization efficiency. Furthermore, nano-DESI MSI research has underscored the importance of matrix effects and established normalization methods for accurately measuring concentration gradients in complex biological samples. This tutorial offers a comprehensive guide to nano-DESI experiments, detailing fundamental principles and data acquisition and processing methods and discussing essential operational parameters.","PeriodicalId":29800,"journal":{"name":"ACS Measurement Science Au","volume":"25 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-08-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142194492","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Achiral Plasmonic Antennas Enhance Differential Absorption To Increase Preferential Detection of Chiral Single Molecules","authors":"Saaj Chattopadhyay, Julie S. Biteen","doi":"10.1021/acsmeasuresciau.4c00026","DOIUrl":"https://doi.org/10.1021/acsmeasuresciau.4c00026","url":null,"abstract":"Plasmonic antennas increase the photon flux in their vicinity, which can lead to plasmon-enhanced fluorescence for molecules near these nanostructures. Here, we combine plasmon-coupled fluorescence and fluorescence-detected circular dichroism to build a specific and sensitive detection strategy for chiral single molecules. Electromagnetic simulations indicate that a two-dimensional gold nanoparticle dimer antenna enhances the electric field and optical chirality of a plane wave in its near field. Furthermore, this optical chirality enhancement can be tuned based on the polarization of the incident electric field, such that enhancing the optical chirality via these antennas will increase the differential absorption of parity-inverted fields. We measured the fluorescence from single molecules of chiral absorbers─Cy5 J-dimers assembled in double-stranded DNA backbones─and achieved increased detectability of these right-handed molecules near achiral gold nanoparticle dimer antennas under right circularly polarized illumination. This strategy offers a new approach to distinguishing weakly fluorescent enantiomers.","PeriodicalId":29800,"journal":{"name":"ACS Measurement Science Au","volume":"116 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2024-08-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141931243","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}