Pub Date : 2025-04-02DOI: 10.1021/acs.analchem.5c00373
Lingling Luo, Yuying Zhou, Yaqin Chai, Ruo Yuan, Hongyan Liu
The minor changes of miRNA levels due to various diseases and cancers bring great challenges for early diagnosis. Here we propose a “signal on-off-super on” PEC biosensor based on a homogeneous multicycle cascaded DNA circuit and a SnSe/CdS photoanode for sensitive detection of biomarker miRNA-222. Specifically, a Z-type SnSe/CdS heterojunction with greatly enhanced photoanodic performance was developed to provide the initial “on” signal. The target miRNA-222 was converted to a dendritic DNA structure through a cascade DNA circuit. The PEC signal can be switched off by the dendritic DNA structure and further switched super on by the loading of photosensitizer manganese porphyrin (MnPP). It is worth noting that the homogeneous multicycle cascaded DNA circuit not only improved the reaction kinetics but also avoided the leakage of signal. Compared with the traditional “signal-on” or “signal-off” readout, this “signal on-off-super on” strategy avoids the false response and background, thereby enhancing the sensitivity and accuracy of the PEC biosensor. The detection limit of the constructed PEC sensor is 0.3 fM in the linear range from 1 fM to 10 nM. The PEC biosensor with outstanding reproducibility, stability, and sensitivity provides a promising platform for biomarker detection and early disease diagnosis.
{"title":"Homogeneous Multicycle Cascaded DNA Circuit for Sensitive “Signal On-Off-Super On” PEC Biosensing","authors":"Lingling Luo, Yuying Zhou, Yaqin Chai, Ruo Yuan, Hongyan Liu","doi":"10.1021/acs.analchem.5c00373","DOIUrl":"https://doi.org/10.1021/acs.analchem.5c00373","url":null,"abstract":"The minor changes of miRNA levels due to various diseases and cancers bring great challenges for early diagnosis. Here we propose a “signal on-off-super on” PEC biosensor based on a homogeneous multicycle cascaded DNA circuit and a SnSe/CdS photoanode for sensitive detection of biomarker miRNA-222. Specifically, a Z-type SnSe/CdS heterojunction with greatly enhanced photoanodic performance was developed to provide the initial “on” signal. The target miRNA-222 was converted to a dendritic DNA structure through a cascade DNA circuit. The PEC signal can be switched off by the dendritic DNA structure and further switched super on by the loading of photosensitizer manganese porphyrin (MnPP). It is worth noting that the homogeneous multicycle cascaded DNA circuit not only improved the reaction kinetics but also avoided the leakage of signal. Compared with the traditional “signal-on” or “signal-off” readout, this “signal on-off-super on” strategy avoids the false response and background, thereby enhancing the sensitivity and accuracy of the PEC biosensor. The detection limit of the constructed PEC sensor is 0.3 fM in the linear range from 1 fM to 10 nM. The PEC biosensor with outstanding reproducibility, stability, and sensitivity provides a promising platform for biomarker detection and early disease diagnosis.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"128 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143766655","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-04-02DOI: 10.1021/acs.analchem.4c06305
Connor D. Flynn, Zhenwei Wu, Amy Bantle, Scott E. Isaacson, Dingran Chang, Alam Mahmud, Hanie Yousefi, Jagotamoy Das, Shana O. Kelley
The development of biomolecular sensing technologies with high sensitivity and specificity remains an important goal in modern analytical science. Molecular pendulum sensing has emerged as a new reagentless method capable of detecting a wide array of biomolecules directly in biological fluids. This sensing approach relies heavily on the modulation of hydrodynamic drag of molecular probes through solution, such that alterations in hydrodynamic diameter can transduce biomolecular interactions. Here, we explore the use of nanobodies as an alternative receptor in pendulum-based systems due to their small size and robust affinities. We compare the performance of nanobodies with that of aptamers and antibodies integrated into the molecular pendulum system by targeting the inflammatory indicator interleukin-6 (IL-6). Nanobody molecular pendulums demonstrate enhanced sensor response and sensitivity compared to those of the other receptors, enabling fine control over detection in the low physiological range of IL-6. In addition, we demonstrate the ability of nanobody sensors to function in complex biological matrices and at physiological temperature.
{"title":"Nanobody Receptors Enable High-Sensitivity Monitoring of IL-6 Using Molecular Pendulum Bioanalysis","authors":"Connor D. Flynn, Zhenwei Wu, Amy Bantle, Scott E. Isaacson, Dingran Chang, Alam Mahmud, Hanie Yousefi, Jagotamoy Das, Shana O. Kelley","doi":"10.1021/acs.analchem.4c06305","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c06305","url":null,"abstract":"The development of biomolecular sensing technologies with high sensitivity and specificity remains an important goal in modern analytical science. Molecular pendulum sensing has emerged as a new reagentless method capable of detecting a wide array of biomolecules directly in biological fluids. This sensing approach relies heavily on the modulation of hydrodynamic drag of molecular probes through solution, such that alterations in hydrodynamic diameter can transduce biomolecular interactions. Here, we explore the use of nanobodies as an alternative receptor in pendulum-based systems due to their small size and robust affinities. We compare the performance of nanobodies with that of aptamers and antibodies integrated into the molecular pendulum system by targeting the inflammatory indicator interleukin-6 (IL-6). Nanobody molecular pendulums demonstrate enhanced sensor response and sensitivity compared to those of the other receptors, enabling fine control over detection in the low physiological range of IL-6. In addition, we demonstrate the ability of nanobody sensors to function in complex biological matrices and at physiological temperature.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"38 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143766654","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-04-02DOI: 10.1021/acs.analchem.4c05228
Phuong T. Do, Bailey Richardson, Samuel C. Brydon, Therese M. Fulloon, Stephen J. Blanksby, Hendrik Frisch, Berwyck L. J. Poad
[2 + 2] Photocycloaddition reactions are powerful tools for synthetic chemistry. However, analysis of the head-to-head or head-to-tail conformation of the resulting cycloadducts is often challenging by conventional spectroscopic methods. Herein, we report the analysis of coumarin and styrylpyrene cycloadducts by cyclic ion-mobility tandem mass spectrometry (cIM-MS/MS) to characterize the regioisomeric products of this important class of photoresponsive groups. Photodissociation (PD) and collision-induced dissociation (CID) of the cycloadduct ions in the gas phase gave similar products to photodissociation in solution with regiospecific fragmentation of the core cyclobutane ring. The styrylpyrene cycloadduct ion was observed to be more stable than the coumarin analog under CID conditions, reflecting the impact of different substituents on the stability of the cyclobutane ring. Exploiting the difference in cyclobutane fragmentation for head-to-head and head-to-tail styrylpyrene cycloadduct isomers, ion mobility enabled CID-MS/MS was applied successfully to differentiate and identify these isomers. The developed method proved to be robust even to complex molecular structures and enabled the identification and separation of photocycloadducts resulting from styrylpyrene terminated peptides, providing access to a rapid analysis of challenging cycloadduct isomers.
{"title":"Mass Spectrometry Directed Structural Elucidation of Isomeric [2 + 2] Photocycloadducts","authors":"Phuong T. Do, Bailey Richardson, Samuel C. Brydon, Therese M. Fulloon, Stephen J. Blanksby, Hendrik Frisch, Berwyck L. J. Poad","doi":"10.1021/acs.analchem.4c05228","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c05228","url":null,"abstract":"[2 + 2] Photocycloaddition reactions are powerful tools for synthetic chemistry. However, analysis of the head-to-head or head-to-tail conformation of the resulting cycloadducts is often challenging by conventional spectroscopic methods. Herein, we report the analysis of coumarin and styrylpyrene cycloadducts by cyclic ion-mobility tandem mass spectrometry (cIM-MS/MS) to characterize the regioisomeric products of this important class of photoresponsive groups. Photodissociation (PD) and collision-induced dissociation (CID) of the cycloadduct ions in the gas phase gave similar products to photodissociation in solution with regiospecific fragmentation of the core cyclobutane ring. The styrylpyrene cycloadduct ion was observed to be more stable than the coumarin analog under CID conditions, reflecting the impact of different substituents on the stability of the cyclobutane ring. Exploiting the difference in cyclobutane fragmentation for head-to-head and head-to-tail styrylpyrene cycloadduct isomers, ion mobility enabled CID-MS/MS was applied successfully to differentiate and identify these isomers. The developed method proved to be robust even to complex molecular structures and enabled the identification and separation of photocycloadducts resulting from styrylpyrene terminated peptides, providing access to a rapid analysis of challenging cycloadduct isomers.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"89 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143758272","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-04-02DOI: 10.1021/acs.analchem.5c00302
Yangxia Han, Haixia Zhang, Yan-Ping Shi
Distinguishing between D2O and H2O is crucial for the utilization of high-purity D2O in the nuclear industry, chemical analysis, biological pathway tracing, and other fields, as well as for ensuring the integrity of water quality and safeguarding human health, but challenging due to their highly analogous physical and chemical properties. On the basis of the fact that D2O exhibits superior hydrogen bond strength and deprotonation capacity for phenolic OH group compared to H2O, the red-emitting carbon dots (RCDs) with excellent optical properties, salt tolerance, photobleaching resistance, long-term storage stability, and biocompatibility were synthesized via a one-step strategy at room temperature. The RCDs demonstrated sensitivity for detecting D2O content in H2O and H2O content in D2O was found to be 0.060% and 0.15%, respectively. Collectively, this research expanded the potential applications of carbon nanomaterials and introduced a highly facile strategy for analyzing the isotopic purity of D2O.
{"title":"Highly Facile Strategy for the Ultrasensitive Differentiation of D2O and H2O by Red-Emitting Carbon Dots","authors":"Yangxia Han, Haixia Zhang, Yan-Ping Shi","doi":"10.1021/acs.analchem.5c00302","DOIUrl":"https://doi.org/10.1021/acs.analchem.5c00302","url":null,"abstract":"Distinguishing between D<sub>2</sub>O and H<sub>2</sub>O is crucial for the utilization of high-purity D<sub>2</sub>O in the nuclear industry, chemical analysis, biological pathway tracing, and other fields, as well as for ensuring the integrity of water quality and safeguarding human health, but challenging due to their highly analogous physical and chemical properties. On the basis of the fact that D<sub>2</sub>O exhibits superior hydrogen bond strength and deprotonation capacity for phenolic OH group compared to H<sub>2</sub>O, the red-emitting carbon dots (RCDs) with excellent optical properties, salt tolerance, photobleaching resistance, long-term storage stability, and biocompatibility were synthesized via a one-step strategy at room temperature. The RCDs demonstrated sensitivity for detecting D<sub>2</sub>O content in H<sub>2</sub>O and H<sub>2</sub>O content in D<sub>2</sub>O was found to be 0.060% and 0.15%, respectively. Collectively, this research expanded the potential applications of carbon nanomaterials and introduced a highly facile strategy for analyzing the isotopic purity of D<sub>2</sub>O.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"22 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143758449","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-04-02DOI: 10.1021/acs.analchem.4c07121
Xionghao Xu, Bo Zhao, Tao Jiang, Nan Yi, Chunhua Fan, Juyoung Yoon, Zhengliang Lu
Ferroptosis, a recently proposed form of regulated cell death, is characterized by a surge in reactive oxygen species and a subsequent depletion of glutathione. The mitochondria and nucleoli play pivotal roles in the process of ferroptosis. Therefore, monitoring the interactions between mitochondria and the nucleoli during ferroptosis is crucial for clarifying its physiological and pathological processes. In this study, we designed and synthesized the near-infrared fluorescence probe MINU, which exhibits excellent stability against biological ions and physiological pH environments. Due to its cationic structure and good DNA affinity, MINU can target both mitochondria and the nucleoli. Cell imaging demonstrates that MINU can reversibly migrate between the mitochondria and the nucleoli in response to changes in mitochondrial membrane potential. By detecting the localization and intensity of fluorescence signals, we can effectively distinguish between normal cell, apoptotic cell, and ferroptotic cell. Monitoring the interactions between mitochondria and the nucleoli allows us to more accurately appreciate the biological processes of ferroptosis.
{"title":"Monitoring Ferroptosis with NIR Fluorescence Probe Capable of Reversible Mitochondria Nucleus Translocation","authors":"Xionghao Xu, Bo Zhao, Tao Jiang, Nan Yi, Chunhua Fan, Juyoung Yoon, Zhengliang Lu","doi":"10.1021/acs.analchem.4c07121","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c07121","url":null,"abstract":"Ferroptosis, a recently proposed form of regulated cell death, is characterized by a surge in reactive oxygen species and a subsequent depletion of glutathione. The mitochondria and nucleoli play pivotal roles in the process of ferroptosis. Therefore, monitoring the interactions between mitochondria and the nucleoli during ferroptosis is crucial for clarifying its physiological and pathological processes. In this study, we designed and synthesized the near-infrared fluorescence probe <b>MINU</b>, which exhibits excellent stability against biological ions and physiological pH environments. Due to its cationic structure and good DNA affinity, <b>MINU</b> can target both mitochondria and the nucleoli. Cell imaging demonstrates that <b>MINU</b> can reversibly migrate between the mitochondria and the nucleoli in response to changes in mitochondrial membrane potential. By detecting the localization and intensity of fluorescence signals, we can effectively distinguish between normal cell, apoptotic cell, and ferroptotic cell. Monitoring the interactions between mitochondria and the nucleoli allows us to more accurately appreciate the biological processes of ferroptosis.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"3 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143766367","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
The 190Pt–186Os and 187Re–187Os isotopic systems are powerful tools for researching the evolution of the Earth and the Solar System. However, high-precision 186Os/188Os analyses remain challenging. In this study, the preconcentration of osmium (Os) has been achieved by the adoption and decomposition of large amounts of geological materials (over 20 g) with the novel use of the antimony (Sb) fire assay. This enables high-precision 186Os/188Os and 187Os/188Os ratio measurements. The total procedural blanks of Os have been reduced to less than 10 pg for samples of 20 g through the purification procedures for fire assay collector Sb2O3 and the use of quartz crucibles. This study also applies multicollector inductively coupled plasma mass spectrometry (MC-ICPMS) for the Os isotope compositions, which is simple and fast and saves the complex polyatomic interferences and oxygen corrections of the traditional negative thermal ionization mass spectrometry (N-TIMS) method. Three Os standard solutions (DROsS, GSB, and HPS) and six rock reference materials were measured with this analytical protocol. The 186Os/188Os and 187Os/188Os ratios of the DROsS are consistent with previously published values within errors including precision and accuracy. Repeated measurements of the DROsS Os standard solution on MC-ICPMS exhibit fine external reproducibility of better than 53 ppm (2 RSD) for 186Os/188Os, which is sufficient to identify subtle 186Os/188Os variations of geological samples. This study is the first to report the 186Os/188Os and 187Os/188Os ratios of GSB and HPS, which are consistent with the N-TIMS values. Furthermore, the 186Os/188Os and 187Os/188Os ratios of six geological reference materials are in good agreement with N-TIMS values, and the results of WPR-1a and GPt-5 are within measurement uncertainty of the previously published N-TIMS results, confirming the validity of our new analytical procedure for the accurate determination of 186Os/188Os and 187Os/188Os ratios of geological samples.
{"title":"High-Precision Determination of 186Os/188Os and 187Os/188Os Isotope Ratios via an Antimony Fire Assay and Multi-collector ICP–MS","authors":"Hou-yin Bao, Jie Li, Wen-shan Ni, Tian-tian Wang, Neng-ping Shen, Gao-bin Chu, Jin-gao Liu, Jun-jie Liu, Ji-feng Xu","doi":"10.1021/acs.analchem.5c00563","DOIUrl":"https://doi.org/10.1021/acs.analchem.5c00563","url":null,"abstract":"The <sup>190</sup>Pt–<sup>186</sup>Os and <sup>187</sup>Re–<sup>187</sup>Os isotopic systems are powerful tools for researching the evolution of the Earth and the Solar System. However, high-precision <sup>186</sup>Os/<sup>188</sup>Os analyses remain challenging. In this study, the preconcentration of osmium (Os) has been achieved by the adoption and decomposition of large amounts of geological materials (over 20 g) with the novel use of the antimony (Sb) fire assay. This enables high-precision <sup>186</sup>Os/<sup>188</sup>Os and <sup>187</sup>Os/<sup>188</sup>Os ratio measurements. The total procedural blanks of Os have been reduced to less than 10 pg for samples of 20 g through the purification procedures for fire assay collector Sb<sub>2</sub>O<sub>3</sub> and the use of quartz crucibles. This study also applies multicollector inductively coupled plasma mass spectrometry (MC-ICPMS) for the Os isotope compositions, which is simple and fast and saves the complex polyatomic interferences and oxygen corrections of the traditional negative thermal ionization mass spectrometry (N-TIMS) method. Three Os standard solutions (DROsS, GSB, and HPS) and six rock reference materials were measured with this analytical protocol. The <sup>186</sup>Os/<sup>188</sup>Os and <sup>187</sup>Os/<sup>188</sup>Os ratios of the DROsS are consistent with previously published values within errors including precision and accuracy. Repeated measurements of the DROsS Os standard solution on MC-ICPMS exhibit fine external reproducibility of better than 53 ppm (2 RSD) for <sup>186</sup>Os/<sup>188</sup>Os, which is sufficient to identify subtle <sup>186</sup>Os/<sup>188</sup>Os variations of geological samples. This study is the first to report the <sup>186</sup>Os/<sup>188</sup>Os and <sup>187</sup>Os/<sup>188</sup>Os ratios of GSB and HPS, which are consistent with the N-TIMS values. Furthermore, the <sup>186</sup>Os/<sup>188</sup>Os and <sup>187</sup>Os/<sup>188</sup>Os ratios of six geological reference materials are in good agreement with N-TIMS values, and the results of WPR-1a and GPt-5 are within measurement uncertainty of the previously published N-TIMS results, confirming the validity of our new analytical procedure for the accurate determination of <sup>186</sup>Os/<sup>188</sup>Os and <sup>187</sup>Os/<sup>188</sup>Os ratios of geological samples.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"183 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143766657","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-04-02DOI: 10.1021/acs.analchem.4c05063
J. Carlos Sanchez, Ingrid H. Robertson, Victoria A. M. Shinkawa, Xiaojing Su, Wan-chen Tu, Timothy R. Robinson, Megan M. Chang, Andrea Blom, Elena Alfaro, Daniel B. Hatchett, Ayokunle O. Olanrewaju, Ellen R. Wald, Gregory P. DeMuri, Erwin Berthier, Sanitta Thongpang, Ashleigh B. Theberge
The CandyCollect is a lollipop-inspired open-fluidic oral sampling device designed to provide a comfortable user sampling experience. We demonstrate that the CandyCollect device can be coupled to a rapid antigen detection test (RADT) kit designed for Group A Streptococcus (GAS). Through in vitro experiments with pooled saliva spiked with Streptococcus pyogenes, we tested various reagents and elution volumes to optimize the RADT readout from CandyCollect device samples. The resulting optimized protocol uses the kit-provided reagents and lateral flow assay (LFA) while replacing the kit’s pharyngeal swab with the CandyCollect device, reducing the elution solution volume, and substituting the tube used for elution to accommodate the CandyCollect device. Positive test results were detected by eye with bacterial concentrations as low as the manufacturer’s “minimal detection limit” of 1.5 × 105 CFU/mL. LFA strips were also scanned and semiquantified with image analysis software to determine the signal-to-baseline ratio (SBR) and categorize positive test results without human bias. We tested our optimized protocol for integrating CandyCollect and RADT using CandyCollect clinical samples from pediatric patients (n = 6) who were previously diagnosed with GAS pharyngitis via pharyngeal swabs tested with RADT as part of their clinical care. The LFA results of these CandyCollect devices and interspersed negative controls were determined by independent observers with positive results obtained in four of the six participants on at least one LFA replicate. Taken together, our results show that CandyCollect devices from children with GAS pharyngitis can be tested by using LFA rapid tests.
{"title":"Integration of Group A Streptococcus Rapid Tests with the Open Fluidic CandyCollect Device","authors":"J. Carlos Sanchez, Ingrid H. Robertson, Victoria A. M. Shinkawa, Xiaojing Su, Wan-chen Tu, Timothy R. Robinson, Megan M. Chang, Andrea Blom, Elena Alfaro, Daniel B. Hatchett, Ayokunle O. Olanrewaju, Ellen R. Wald, Gregory P. DeMuri, Erwin Berthier, Sanitta Thongpang, Ashleigh B. Theberge","doi":"10.1021/acs.analchem.4c05063","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c05063","url":null,"abstract":"The CandyCollect is a lollipop-inspired open-fluidic oral sampling device designed to provide a comfortable user sampling experience. We demonstrate that the CandyCollect device can be coupled to a rapid antigen detection test (RADT) kit designed for Group A Streptococcus (GAS). Through <i>in vitro</i> experiments with pooled saliva spiked with <i>Streptococcus pyogenes</i>, we tested various reagents and elution volumes to optimize the RADT readout from CandyCollect device samples. The resulting optimized protocol uses the kit-provided reagents and lateral flow assay (LFA) while replacing the kit’s pharyngeal swab with the CandyCollect device, reducing the elution solution volume, and substituting the tube used for elution to accommodate the CandyCollect device. Positive test results were detected by eye with bacterial concentrations as low as the manufacturer’s “minimal detection limit” of 1.5 × 10<sup>5</sup> CFU/mL. LFA strips were also scanned and semiquantified with image analysis software to determine the signal-to-baseline ratio (SBR) and categorize positive test results without human bias. We tested our optimized protocol for integrating CandyCollect and RADT using CandyCollect clinical samples from pediatric patients (<i>n</i> = 6) who were previously diagnosed with GAS pharyngitis via pharyngeal swabs tested with RADT as part of their clinical care. The LFA results of these CandyCollect devices and interspersed negative controls were determined by independent observers with positive results obtained in four of the six participants on at least one LFA replicate. Taken together, our results show that CandyCollect devices from children with GAS pharyngitis can be tested by using LFA rapid tests.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"73 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143766653","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-04-02DOI: 10.1021/acs.analchem.5c00157
Yao Qian, Xiaoxiao Ma
Spatial metabolomics based on mass spectrometry imaging (MSI) is a promising approach for fundamental biological research and disease biomarker discovery. It simultaneously reveals the spatial distributions of hundreds of metabolites across tissue sections. While previous MSI experiments predominantly rely on high-resolution mass analysis for metabolite annotation, the high specificity in resolving molecular structures is essential to distinguish isomers or isobars to obtain ultimate identities of the metabolites. This is also critical for correlating their biological functions with spatial distribution patterns. Tandem mass spectrometry (MS/MS) is effectively used to obtain molecular structural information and has been integrated into MSI for spatial mapping of structurally distinct biomolecules, though typically with low coverage. The main technical challenge in achieving high-coverage, high-structure-resolving spatial mapping of biomolecules lies in the limited amount of sample available from each tissue pixel in conventional MS/MS analysis, which restricts the number of MS/MS scans that can be conducted on the metabolite precursors of interest. In this Perspective, we highlight recent developments in advanced MS/MS imaging strategies aimed at achieving high-coverage spatial metabolomics.
{"title":"Advances in Tandem Mass Spectrometry Imaging for Next-Generation Spatial Metabolomics","authors":"Yao Qian, Xiaoxiao Ma","doi":"10.1021/acs.analchem.5c00157","DOIUrl":"https://doi.org/10.1021/acs.analchem.5c00157","url":null,"abstract":"Spatial metabolomics based on mass spectrometry imaging (MSI) is a promising approach for fundamental biological research and disease biomarker discovery. It simultaneously reveals the spatial distributions of hundreds of metabolites across tissue sections. While previous MSI experiments predominantly rely on high-resolution mass analysis for metabolite annotation, the high specificity in resolving molecular structures is essential to distinguish isomers or isobars to obtain ultimate identities of the metabolites. This is also critical for correlating their biological functions with spatial distribution patterns. Tandem mass spectrometry (MS/MS) is effectively used to obtain molecular structural information and has been integrated into MSI for spatial mapping of structurally distinct biomolecules, though typically with low coverage. The main technical challenge in achieving high-coverage, high-structure-resolving spatial mapping of biomolecules lies in the limited amount of sample available from each tissue pixel in conventional MS/MS analysis, which restricts the number of MS/MS scans that can be conducted on the metabolite precursors of interest. In this Perspective, we highlight recent developments in advanced MS/MS imaging strategies aimed at achieving high-coverage spatial metabolomics.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"25 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-04-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143758448","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2025-04-01DOI: 10.1021/acs.analchem.5c01621
Siyu Zhao, Corey Giles, Kevin Huynh, Johannes Kettunen, Marjo-Riitta Järvelin, Mika Kähönen, Jorma Viikari, Terho Lehtimäki, Olli T. Raitakari, Peter J. Meikle, Ville-Petteri Mäkinen, Mika Ala-Korpela
In our original article, two minor errors need corrected: (1) On page 20363, in the Materials and Methods section, under the Population Cohorts subsection, there is a wrong number given for the number of participants in the Young Finns Study (YFS). Instead of “the Young Finns Study (YFS) with 2036 participants (43 years, 55% women)”, it should be “the Young Finns Study (YFS) with 2173 participants (39 years, 55% women)”. Importantly, all analyses and data used in the work are correct; i.e., this is only a mistake with the number and the age of the participants. These numbers came from another time point of YFS, but no data from that time point were used. The numbers referring to YFS in all other places in the paper are correct. (2) An identification line is missing from Figure S4 (page S27) of the Supporting Information regarding the heatmap for phosphatidylcholine (PC). The missing identification is PC(18:0_22:5)(n3) and PC(20:1_20:4). This is now corrected in the attached Supporting Information file. The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.analchem.5c01621. Detailed information regarding study populations, data, methods, funding, and supplementary results (PDF) Correction to “Personalized Profiling of Lipoproteinand Lipid Metabolism Based on 1018 Measures from Combined QuantitativeNMR and LC-MS/MS Platforms” 0 views 0 shares 0 downloads Most electronic Supporting Information files are available without a subscription to ACS Web Editions. Such files may be downloaded by article for research use (if there is a public use license linked to the relevant article, that license may permit other uses). Permission may be obtained from ACS for other uses through requests via the RightsLink permission system: http://pubs.acs.org/page/copyright/permissions.html. This article has not yet been cited by other publications.
{"title":"Correction to “Personalized Profiling of Lipoprotein and Lipid Metabolism Based on 1018 Measures from Combined Quantitative NMR and LC-MS/MS Platforms”","authors":"Siyu Zhao, Corey Giles, Kevin Huynh, Johannes Kettunen, Marjo-Riitta Järvelin, Mika Kähönen, Jorma Viikari, Terho Lehtimäki, Olli T. Raitakari, Peter J. Meikle, Ville-Petteri Mäkinen, Mika Ala-Korpela","doi":"10.1021/acs.analchem.5c01621","DOIUrl":"https://doi.org/10.1021/acs.analchem.5c01621","url":null,"abstract":"In our original article, two minor errors need corrected: (1) On page 20363, in the Materials and Methods section, under the Population Cohorts subsection, there is a wrong number given for the number of participants in the Young Finns Study (YFS). Instead of “the Young Finns Study (YFS) with 2036 participants (43 years, 55% women)”, it should be “the Young Finns Study (YFS) with 2173 participants (39 years, 55% women)”. Importantly, all analyses and data used in the work are correct; i.e., this is only a mistake with the number and the age of the participants. These numbers came from another time point of YFS, but no data from that time point were used. The numbers referring to YFS in all other places in the paper are correct. (2) An identification line is missing from Figure S4 (page S27) of the Supporting Information regarding the heatmap for phosphatidylcholine (PC). The missing identification is PC(18:0_22:5)(n3) and PC(20:1_20:4). This is now corrected in the attached Supporting Information file. The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.analchem.5c01621. Detailed information regarding study populations, data, methods, funding, and supplementary results (PDF) Correction to “Personalized Profiling of Lipoprotein\u0000and Lipid Metabolism Based on 1018 Measures from Combined Quantitative\u0000NMR and LC-MS/MS Platforms” <span> 0 </span><span> views </span> <span> 0 </span><span> shares </span> <span> 0 </span><span> downloads </span> Most electronic Supporting Information files are available without a subscription to ACS Web Editions. Such files may be downloaded by article for research use (if there is a public use license linked to the relevant article, that license may permit other uses). Permission may be obtained from ACS for other uses through requests via the RightsLink permission system: http://pubs.acs.org/page/copyright/permissions.html. This article has not yet been cited by other publications.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"32 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143745554","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Protein glycosylation, classified into N-glycosylation and O-glycosylation, is the most prevalent and complex protein post-translational modification. Bioorthogonal chemistry reactions combining the biotin–streptavidin interaction system are the most commonly used for investigating protein glycosylation. In this study, a one-step enzymatic labeling strategy for the simultaneous and global profiling of multiple types of protein glycosylation was developed. A “one-step probe” directly carrying the enrichment support poly(N-isopropylacrylamide) (PNIPAM) was designed and synthesized. Although the designed probe carried a large enrichment group (the number-average molecular weight of PNIPAM was up to 10,000 Da), it was well accepted by the two substrate-specific sialyltransferases to label N-glycopeptides and O-glycopeptides. PNIPAM is a temperature-sensitive polymer. When the temperature was below the lower critical solution temperature, PNIPAM was water-soluble and precipitated when it was above the lower critical solution temperature. The advantage of this property was that the labeled glycopeptides were enriched from complex biological samples by simply changing the temperature without the need for additional enrichment resins. Following enzymatic and ultraviolet-light-mediated cleavage, the labeled N-glycopeptide, core-fucosylated glycopeptide, and truncated mucin-type O-glycopeptides (Tn, STn, T, and ST antigens) were released sequentially for glycosylation profiling via mass spectrometry. This work provides an effective strategy to significantly reduce enrichment costs for profiling multiple glycosylation types.
{"title":"One-Step Labeling Strategy for the Profiling of Multiple Types of Protein Glycosylation","authors":"Yinping Tian, Yuqiu Wang, Ying Zhang, Jingyi Guo, Pengfei Zhang, Xia Li, Hu Zhou, Liuqing Wen","doi":"10.1021/acs.analchem.4c06400","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c06400","url":null,"abstract":"Protein glycosylation, classified into <i>N</i>-glycosylation and <i>O</i>-glycosylation, is the most prevalent and complex protein post-translational modification. Bioorthogonal chemistry reactions combining the biotin–streptavidin interaction system are the most commonly used for investigating protein glycosylation. In this study, a one-step enzymatic labeling strategy for the simultaneous and global profiling of multiple types of protein glycosylation was developed. A “one-step probe” directly carrying the enrichment support poly(<i>N</i>-isopropylacrylamide) (PNIPAM) was designed and synthesized. Although the designed probe carried a large enrichment group (the number-average molecular weight of PNIPAM was up to 10,000 Da), it was well accepted by the two substrate-specific sialyltransferases to label <i>N</i>-glycopeptides and <i>O</i>-glycopeptides. PNIPAM is a temperature-sensitive polymer. When the temperature was below the lower critical solution temperature, PNIPAM was water-soluble and precipitated when it was above the lower critical solution temperature. The advantage of this property was that the labeled glycopeptides were enriched from complex biological samples by simply changing the temperature without the need for additional enrichment resins. Following enzymatic and ultraviolet-light-mediated cleavage, the labeled <i>N</i>-glycopeptide, core-fucosylated glycopeptide, and truncated mucin-type <i>O</i>-glycopeptides (Tn, STn, T, and ST antigens) were released sequentially for glycosylation profiling via mass spectrometry. This work provides an effective strategy to significantly reduce enrichment costs for profiling multiple glycosylation types.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"13 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143745400","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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