Pub Date : 2025-01-15DOI: 10.1021/acs.analchem.4c05949
Ning Ding, Bo Zhang, Eslam M. Hamed, Mingwei Qin, Li Ji, Shuo Qi, Sam Fong Yau Li, Zhouping Wang
Salmonella typhimurium (S. typhimurium) is a prominent pathogen responsible for intestinal infections, primarily transmitted through contaminated food and water. This underscores the critical need for precise and biocompatible technologies enabling early detection and intervention of bacterial colonization in vivo. Herein, a multifunctional nanoplatform (IR808-Au@ZIF-90-Apt) was designed, utilizing an S. typhimurium-specific aptamer to initiate cascade responses triggered by intracellular ATP and GSH. The nanoplatform precisely targets S. typhimuriumvia aptamer recognition, promoting bacterial aggregation through nanoparticle sedimentation in an oscillatory system. Furthermore, the intelligent nanoplatform significantly enhances the sensitivity of S. typhimurium detection based on near-infrared (NIR) fluorescence signals, achieving a detection limit as low as 2 CFU mL–1. Additionally, in situ NIR irradiation was applied at the 30 min peak of fluorescence detection, enabling rapid and irreversible inactivation of S. typhimurium through the synergistic effects of photothermal and photodynamic effects. Importantly, in a mouse model of intestinal infection, the nanoplatform successfully detected early S. typhimurium colonization and achieved highly efficient in situ inactivation without adversely affecting the major organs. In conclusion, the nanoplatform achieved precise localized detection and in situ inactivation of S. typhimurium, offering valuable insights for disease surveillance and epidemiological studies, with promising implications for food safety and public health.
{"title":"Aptamer-Driven Multifunctional Nanoplatform for Near-Infrared Fluorescence Imaging and Rapid In Situ Inactivation of Salmonella typhimurium","authors":"Ning Ding, Bo Zhang, Eslam M. Hamed, Mingwei Qin, Li Ji, Shuo Qi, Sam Fong Yau Li, Zhouping Wang","doi":"10.1021/acs.analchem.4c05949","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c05949","url":null,"abstract":"<i>Salmonella typhimurium</i> (<i>S. typhimurium</i>) is a prominent pathogen responsible for intestinal infections, primarily transmitted through contaminated food and water. This underscores the critical need for precise and biocompatible technologies enabling early detection and intervention of bacterial colonization <i>in vivo</i>. Herein, a multifunctional nanoplatform (IR808-Au@ZIF-90-Apt) was designed, utilizing an <i>S. typhimurium</i>-specific aptamer to initiate cascade responses triggered by intracellular ATP and GSH. The nanoplatform precisely targets <i>S. typhimurium</i><i>via</i> aptamer recognition, promoting bacterial aggregation through nanoparticle sedimentation in an oscillatory system. Furthermore, the intelligent nanoplatform significantly enhances the sensitivity of <i>S. typhimurium</i> detection based on near-infrared (NIR) fluorescence signals, achieving a detection limit as low as 2 CFU mL<sup>–1</sup>. Additionally, <i>in situ</i> NIR irradiation was applied at the 30 min peak of fluorescence detection, enabling rapid and irreversible inactivation of <i>S. typhimurium</i> through the synergistic effects of photothermal and photodynamic effects. Importantly, in a mouse model of intestinal infection, the nanoplatform successfully detected early <i>S. typhimurium</i> colonization and achieved highly efficient <i>in situ</i> inactivation without adversely affecting the major organs. In conclusion, the nanoplatform achieved precise localized detection and <i>in situ</i> inactivation of <i>S. typhimurium</i>, offering valuable insights for disease surveillance and epidemiological studies, with promising implications for food safety and public health.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"22 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-01-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142981246","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}
Developing a DNA autocatalysis-oriented cascade circuit (AOCC) via reciprocal navigation of two enzyme-free hug-amplifiers might be desirable for constructing a rapid, efficient, and sensitive assay-to-treat platform. In response to a specific trigger (T), seven functional DNA hairpins were designed to execute three-branched assembly (TBA) and three isotropic hybridization chain reaction (3HCR) events for operating the AOCC. This was because three new inducers were reconstructed in TBA arms to initiate 3HCR (TBA-to-3HCR) and periodic T repeats were resultantly reassembled in the tandem nicks of polymeric nanowires to rapidly activate TBA in the opposite direction (3HCR-to-TBA) without steric hindrance, thereby cooperatively manipulating sustainable AOCC progress for exponential hug-amplification (1:3Nn). Our experimental verifications manifested that the T-dependent AOCC amplifier achieved fast input transduction and efficient fluorescence readout. As predicted, the flexible programming of reactive hairpin species endowed the repeating nicks in productive 3HCR nanowires with great possibilities and accessibilities to graft tailored modular elements, such as G-rich AS1411 aptamers capable of adopting G-quadruplex conformations (G4) that readily facilitated the embedding of zinc(II) protoporphyrin IX (ZnPPIX), a kind of heme oxygenase-1 enzyme inhibitor. Thus, the cascading ZnPPIX/G4 entities acted as fluorescent signal reporters, photosensitizers and anticancer drugs, thereby creating an updated AOCC-based assay-to-treat platform for ultrasensitive biosensing, discernible cell imaging and efficient photodynamic therapy of cancer cells. This would offer a new paradigm to advance the rational integration of dynamic DNA assembly and amplifiable recycling circuits for applicable bioassay and theranostics.
{"title":"A High-Efficiency Autocatalysis-Oriented Cascade Circuit via Reciprocal Hug-Amplification for Assay-to-Treat Application","authors":"Chunli Yang, Yuqing Zhang, Zhaorong Mo, Jiayang He, Zhihan Zhang, Yaqin Chai, Ruo Yuan, Wenju Xu","doi":"10.1021/acs.analchem.4c05701","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c05701","url":null,"abstract":"Developing a DNA autocatalysis-oriented cascade circuit (AOCC) via reciprocal navigation of two enzyme-free hug-amplifiers might be desirable for constructing a rapid, efficient, and sensitive assay-to-treat platform. In response to a specific trigger (<b>T</b>), seven functional DNA hairpins were designed to execute three-branched assembly (TBA) and three isotropic hybridization chain reaction (3HCR) events for operating the AOCC. This was because three new inducers were reconstructed in TBA arms to initiate 3HCR (TBA-to-3HCR) and periodic <b>T</b> repeats were resultantly reassembled in the tandem nicks of polymeric nanowires to rapidly activate TBA in the opposite direction (3HCR-to-TBA) without steric hindrance, thereby cooperatively manipulating sustainable AOCC progress for exponential hug-amplification (1:3<i>N</i><sup>n</sup>). Our experimental verifications manifested that the <b>T</b>-dependent AOCC amplifier achieved fast input transduction and efficient fluorescence readout. As predicted, the flexible programming of reactive hairpin species endowed the repeating nicks in productive 3HCR nanowires with great possibilities and accessibilities to graft tailored modular elements, such as G-rich AS1411 aptamers capable of adopting G-quadruplex conformations (G4) that readily facilitated the embedding of zinc(II) protoporphyrin IX (ZnPPIX), a kind of heme oxygenase-1 enzyme inhibitor. Thus, the cascading ZnPPIX/G4 entities acted as fluorescent signal reporters, photosensitizers and anticancer drugs, thereby creating an updated AOCC-based assay-to-treat platform for ultrasensitive biosensing, discernible cell imaging and efficient photodynamic therapy of cancer cells. This would offer a new paradigm to advance the rational integration of dynamic DNA assembly and amplifiable recycling circuits for applicable bioassay and theranostics.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"4 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-01-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142981245","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 : 2025-01-15DOI: 10.1021/acs.analchem.4c02924
Yuanliang Zhang, Ying Yang, Kecheng Li, Lei Chen, Yang Yang, Chenxi Yang, Zhi Xie, Hongwei Wang, Qian Zhao
Alternative proteins (AltProts) are a class of proteins encoded by DNA sequences previously classified as noncoding. Despite their historically being overlooked, recent studies have highlighted their widespread presence and distinctive biological roles. So far, direct detection of AltProt has been relying on data-dependent acquisition (DDA) mass spectrometry (MS). However, data-independent acquisition (DIA) MS, a method that is rapidly gaining popularity for the analysis of canonical proteins, has seen limited application in AltProt research, largely due to the complexities involved in constructing DIA libraries. In this study, we present a novel DIA workflow that leverages a fragmentation spectra predictor for the efficient construction of DIA libraries, significantly enhancing the detection of AltProts. Our method achieved a 2-fold increase in the identification of AltProts and a 50% reduction in missing values compared to DDA. We conducted a comprehensive comparison of four AltProt databases, four DIA-library construction strategies, and three analytical software tools to establish an optimal workflow for AltProt analysis. Utilizing this workflow, we investigated the mouse heart development process and identified over 50 AltProts with differential expression between embryonic and adult heart tissues. Over 30 unannotated mouse AltProts were validated, including ASDURF, which played a crucial role in cardiac development. Our findings not only provide a practical workflow for MS-based AltProt analysis but also reveal novel AltProts with potential significance in biological functions.
{"title":"Enhanced Discovery of Alternative Proteins (AltProts) in Mouse Cardiac Development Using Data-Independent Acquisition (DIA) Proteomics","authors":"Yuanliang Zhang, Ying Yang, Kecheng Li, Lei Chen, Yang Yang, Chenxi Yang, Zhi Xie, Hongwei Wang, Qian Zhao","doi":"10.1021/acs.analchem.4c02924","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c02924","url":null,"abstract":"Alternative proteins (AltProts) are a class of proteins encoded by DNA sequences previously classified as noncoding. Despite their historically being overlooked, recent studies have highlighted their widespread presence and distinctive biological roles. So far, direct detection of AltProt has been relying on data-dependent acquisition (DDA) mass spectrometry (MS). However, data-independent acquisition (DIA) MS, a method that is rapidly gaining popularity for the analysis of canonical proteins, has seen limited application in AltProt research, largely due to the complexities involved in constructing DIA libraries. In this study, we present a novel DIA workflow that leverages a fragmentation spectra predictor for the efficient construction of DIA libraries, significantly enhancing the detection of AltProts. Our method achieved a 2-fold increase in the identification of AltProts and a 50% reduction in missing values compared to DDA. We conducted a comprehensive comparison of four AltProt databases, four DIA-library construction strategies, and three analytical software tools to establish an optimal workflow for AltProt analysis. Utilizing this workflow, we investigated the mouse heart development process and identified over 50 AltProts with differential expression between embryonic and adult heart tissues. Over 30 unannotated mouse AltProts were validated, including ASDURF, which played a crucial role in cardiac development. Our findings not only provide a practical workflow for MS-based AltProt analysis but also reveal novel AltProts with potential significance in biological functions.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"3 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-01-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142986224","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 : 2025-01-15DOI: 10.1021/acs.analchem.4c04183
Lluís Mangas-Florencio, Alba Herrero-Gómez, James Eills, Marc Azagra, Marina Batlló-Rius, Irene Marco-Rius
Nuclear magnetic resonance (NMR) spectroscopy is a valuable diagnostic tool limited by low sensitivity due to low nuclear spin polarization. Hyperpolarization techniques, such as dissolution dynamic nuclear polarization, significantly enhance sensitivity, enabling real-time tracking of cellular metabolism. However, traditional high-field NMR systems and bioreactor platforms pose challenges, including the need for specialized equipment and fixed sample volumes. This study introduces a scalable, 3D-printed bioreactor platform compatible with low-field NMR spectrometers, designed to accommodate bioengineered 3D cell models. The bioreactor is fabricated using biocompatible materials and features a microfluidic system for media recirculation, ensuring optimal culture conditions during NMR acquisition and cell maintenance. We characterized the NMR compatibility of the bioreactor components and confirmed minimal signal distortion. The bioreactor’s efficacy was validated using HeLa and HepG2 cells, demonstrating prolonged cell viability and enhanced metabolic activity in 3D cultures compared to 2D cultures. Hyperpolarized [1-13C] pyruvate experiments revealed distinct metabolic profiles for the two cell types, highlighting the bioreactor’s ability to discern metabolic profiles among samples. Our results indicate that the bioreactor platform supports the maintenance and analysis of 3D cell models in NMR studies, offering a versatile and accessible tool for metabolic and biochemical research in tissue engineering. This platform bridges the gap between advanced cellular models and NMR spectroscopy, providing a robust framework for future applications in nonspecialized laboratories. The design files for the 3D printed components are shared within the text for easy download and customization, promoting their use and adaptation for further applications.
{"title":"A DIY Bioreactor for in Situ Metabolic Tracking in 3D Cell Models via Hyperpolarized 13C NMR Spectroscopy","authors":"Lluís Mangas-Florencio, Alba Herrero-Gómez, James Eills, Marc Azagra, Marina Batlló-Rius, Irene Marco-Rius","doi":"10.1021/acs.analchem.4c04183","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c04183","url":null,"abstract":"Nuclear magnetic resonance (NMR) spectroscopy is a valuable diagnostic tool limited by low sensitivity due to low nuclear spin polarization. Hyperpolarization techniques, such as dissolution dynamic nuclear polarization, significantly enhance sensitivity, enabling real-time tracking of cellular metabolism. However, traditional high-field NMR systems and bioreactor platforms pose challenges, including the need for specialized equipment and fixed sample volumes. This study introduces a scalable, 3D-printed bioreactor platform compatible with low-field NMR spectrometers, designed to accommodate bioengineered 3D cell models. The bioreactor is fabricated using biocompatible materials and features a microfluidic system for media recirculation, ensuring optimal culture conditions during NMR acquisition and cell maintenance. We characterized the NMR compatibility of the bioreactor components and confirmed minimal signal distortion. The bioreactor’s efficacy was validated using HeLa and HepG2 cells, demonstrating prolonged cell viability and enhanced metabolic activity in 3D cultures compared to 2D cultures. Hyperpolarized [1-<sup>13</sup>C] pyruvate experiments revealed distinct metabolic profiles for the two cell types, highlighting the bioreactor’s ability to discern metabolic profiles among samples. Our results indicate that the bioreactor platform supports the maintenance and analysis of 3D cell models in NMR studies, offering a versatile and accessible tool for metabolic and biochemical research in tissue engineering. This platform bridges the gap between advanced cellular models and NMR spectroscopy, providing a robust framework for future applications in nonspecialized laboratories. The design files for the 3D printed components are shared within the text for easy download and customization, promoting their use and adaptation for further applications.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"8 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-01-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142986225","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 : 2025-01-15DOI: 10.1021/acs.analchem.4c05910
Hsi-Chun Chao, Scott A. McLuckey
Lipid A, a well-known saccharolipid, acts as the inner lipid–glycan anchor of lipopolysaccharides in Gram-negative bacterial cell membranes and functions as an endotoxin. Its structure is composed of two glucosamines with β(1 → 6) linkages and various fatty acyl and phosphate groups. The lipid A structure can be used for the identification of bacterial species, but its complexity poses significant structural characterization challenges. In this work, we present a comprehensive strategy combining condensed-phase sample preparation, electrospray ionization, and gas-phase ion/ion reactions with tandem mass spectrometry for detailed lipid A structural elucidation. We use proton transfer reactions, charge-inversion reactions, and sequential ion/ion reactions for magnesium transfer to generate targeted lipid A ions. The strategy, established with a synthetic monophosphoryl lipid A (MPLA) and known MPLA and diphosphorylated lipid A (DPLA) from Escherichia coli F583, demonstrated that [MPLA – 2H]2–, [MPLA – H]−, and [MPLA – H + Mg]+ precursor ions offer complementary information for MPLA, while [DPLA – H]−, [DPLA + H]+, and [DPLA – H + Mg]+ precursor ions provide analogous information for DPLA analysis. We validated the strategy using known lipid A species and also successfully applied this strategy to profile unknown MPLA and DPLA in the same E. coli strain.
{"title":"Altering Lipid A Precursor Ion Types in the Gas Phase for In-Depth Structural Elucidation via Tandem Mass Spectrometry","authors":"Hsi-Chun Chao, Scott A. McLuckey","doi":"10.1021/acs.analchem.4c05910","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c05910","url":null,"abstract":"Lipid A, a well-known saccharolipid, acts as the inner lipid–glycan anchor of lipopolysaccharides in Gram-negative bacterial cell membranes and functions as an endotoxin. Its structure is composed of two glucosamines with β(1 → 6) linkages and various fatty acyl and phosphate groups. The lipid A structure can be used for the identification of bacterial species, but its complexity poses significant structural characterization challenges. In this work, we present a comprehensive strategy combining condensed-phase sample preparation, electrospray ionization, and gas-phase ion/ion reactions with tandem mass spectrometry for detailed lipid A structural elucidation. We use proton transfer reactions, charge-inversion reactions, and sequential ion/ion reactions for magnesium transfer to generate targeted lipid A ions. The strategy, established with a synthetic monophosphoryl lipid A (MPLA) and known MPLA and diphosphorylated lipid A (DPLA) from <i>Escherichia coli</i> F583, demonstrated that [MPLA – 2H]<sup>2–</sup>, [MPLA – H]<sup>−</sup>, and [MPLA – H + Mg]<sup>+</sup> precursor ions offer complementary information for MPLA, while [DPLA – H]<sup>−</sup>, [DPLA + H]<sup>+</sup>, and [DPLA – H + Mg]<sup>+</sup> precursor ions provide analogous information for DPLA analysis. We validated the strategy using known lipid A species and also successfully applied this strategy to profile unknown MPLA and DPLA in the same <i>E. coli</i> strain.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"26 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-01-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142986245","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 : 2025-01-15DOI: 10.1021/acs.analchem.4c06211
Yun Tan, Dan Huang, Guan A. Wang, Chenlan Shen, Hui Deng, Feng Li
Isothermal nucleic acid amplification techniques are promising alternatives to polymerase chain reaction (PCR) for amplifying and detecting nucleic acids under resource-limited conditions. While many isothermal amplification strategies, such as recombinase polymerase amplification (RPA), offer comparable sensitivity to PCR, they often lack the specificity and robustness for discriminating single nucleotide variants (SNVs), mainly due to the uncontrolled production of massive amplicons. Herein, we introduce a mismatch-guided DNA assembly (MGDA) approach capable of discriminating SNVs in the presence of high concentrations of wild-type (WT) interferences. We show that an optimal MGDA design can effectively suppress interfering signals from WT while maintaining high detection signals for the targeted SNV. A further introduction of a competitive sink probe allowed the detection of challenging SNVs, such as those containing G-T wobbles, with high sensitivity and specificity. Because it is highly specific and tolerant to massively produced interfering amplicons during isothermal nucleic acid amplification, we integrated MGDA with RPA for discriminating clinically relevant SNVs in point-of-care settings. We demonstrate that our RPA-MGDA is highly sensitive and specific, allowing the detection of as low as 1 aM SNVs with an allele frequency of 0.5%. We also evaluated the clinical potential of RPA-MGDA by analyzing epidermal growth factor receptor L858R mutations in tumor tissue samples collected from non-small-cell lung cancer patients (n = 44). A multiplexed RPA-MGDA assay was also developed for the simultaneous detection of pharmacogenetic mutations in buccal swab samples (n = 30).
{"title":"Concentration-Bias-Free Discrimination of Single Nucleotide Variants Using Isothermal Nucleic Acid Amplification and Mismatch-Guided DNA Assembly","authors":"Yun Tan, Dan Huang, Guan A. Wang, Chenlan Shen, Hui Deng, Feng Li","doi":"10.1021/acs.analchem.4c06211","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c06211","url":null,"abstract":"Isothermal nucleic acid amplification techniques are promising alternatives to polymerase chain reaction (PCR) for amplifying and detecting nucleic acids under resource-limited conditions. While many isothermal amplification strategies, such as recombinase polymerase amplification (RPA), offer comparable sensitivity to PCR, they often lack the specificity and robustness for discriminating single nucleotide variants (SNVs), mainly due to the uncontrolled production of massive amplicons. Herein, we introduce a mismatch-guided DNA assembly (MGDA) approach capable of discriminating SNVs in the presence of high concentrations of wild-type (WT) interferences. We show that an optimal MGDA design can effectively suppress interfering signals from WT while maintaining high detection signals for the targeted SNV. A further introduction of a competitive sink probe allowed the detection of challenging SNVs, such as those containing G-T wobbles, with high sensitivity and specificity. Because it is highly specific and tolerant to massively produced interfering amplicons during isothermal nucleic acid amplification, we integrated MGDA with RPA for discriminating clinically relevant SNVs in point-of-care settings. We demonstrate that our RPA-MGDA is highly sensitive and specific, allowing the detection of as low as 1 aM SNVs with an allele frequency of 0.5%. We also evaluated the clinical potential of RPA-MGDA by analyzing epidermal growth factor receptor L858R mutations in tumor tissue samples collected from non-small-cell lung cancer patients (<i>n</i> = 44). A multiplexed RPA-MGDA assay was also developed for the simultaneous detection of pharmacogenetic mutations in buccal swab samples (<i>n</i> = 30).","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"94 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-01-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142986246","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 : 2025-01-15DOI: 10.1021/acs.analchem.4c06384
Dongliu Xiang, Xueting Yan, Jia Liu, Yuan Zhou, Aiping Cui, Qing Wang, Xiaoxiao He, Mingze Ma, Jin Huang, Jianbo Liu, Xiaohai Yang, Kemin Wang
To facilitate on-site detection by nonspecialists, there is a demand for the development of portable “sample-to-answer” devices capable of executing all procedures in an automated or easy-to-operate manner. Here, we developed an automated detection device that integrated a magnetofluidic manipulation system and a signal acquisition system. Both systems were controllable via a smartphone. In the device, the mixing of solutions and magnetic beads in the static chamber was enhanced by steel bead agitation, which improved the reaction efficiency. We demonstrate the performance of the device using myoglobin detection as an example. During the detection process, the plasma was separated from the whole blood sample using a homemade mini-centrifuge, and subsequently, the plasma, magnetic beads, and reagents were added to a magnetofluidic chip with multiple chambers. After the chip was loaded, the device was initiated with a smartphone App via Bluetooth. Then, the magnetic beads were shuttled through different chambers of the chip and multiple steps were completed automatically: first, the targets were separated and enriched using antibody-modified magnetic beads, followed by washing, binding with aptamer-functionalized G-quadruplex, signal amplifying (optional), and chromogenic reaction. Finally, the images of colored solutions were captured and processed by a smartphone to obtain the concentrations of myoglobin. The detection limits depended on the mode of signal conversion, which were 0.1 or 2.7 nM (with or without signal amplifying). With its simple operation, compact design, low cost, and ease of scalability, this automated detection device holds potential applications in human health, food safety, environmental monitoring, etc.
{"title":"Magnetofluidic-Assisted Portable Automated Microfluidic Devices for Protein Detection","authors":"Dongliu Xiang, Xueting Yan, Jia Liu, Yuan Zhou, Aiping Cui, Qing Wang, Xiaoxiao He, Mingze Ma, Jin Huang, Jianbo Liu, Xiaohai Yang, Kemin Wang","doi":"10.1021/acs.analchem.4c06384","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c06384","url":null,"abstract":"To facilitate on-site detection by nonspecialists, there is a demand for the development of portable “sample-to-answer” devices capable of executing all procedures in an automated or easy-to-operate manner. Here, we developed an automated detection device that integrated a magnetofluidic manipulation system and a signal acquisition system. Both systems were controllable via a smartphone. In the device, the mixing of solutions and magnetic beads in the static chamber was enhanced by steel bead agitation, which improved the reaction efficiency. We demonstrate the performance of the device using myoglobin detection as an example. During the detection process, the plasma was separated from the whole blood sample using a homemade mini-centrifuge, and subsequently, the plasma, magnetic beads, and reagents were added to a magnetofluidic chip with multiple chambers. After the chip was loaded, the device was initiated with a smartphone App via Bluetooth. Then, the magnetic beads were shuttled through different chambers of the chip and multiple steps were completed automatically: first, the targets were separated and enriched using antibody-modified magnetic beads, followed by washing, binding with aptamer-functionalized G-quadruplex, signal amplifying (optional), and chromogenic reaction. Finally, the images of colored solutions were captured and processed by a smartphone to obtain the concentrations of myoglobin. The detection limits depended on the mode of signal conversion, which were 0.1 or 2.7 nM (with or without signal amplifying). With its simple operation, compact design, low cost, and ease of scalability, this automated detection device holds potential applications in human health, food safety, environmental monitoring, etc.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"53 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-01-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142986247","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 : 2025-01-15DOI: 10.1021/acs.analchem.4c05658
Dou Dou, Mingqi Jiao, Mingyang Feng, Mu Liang, Kaijun Mu, Yingying Qiao, Lei Li, Chongxin Shan
The photoacoustic spectroscopy (PAS) system commonly enhances the efficiency of optical-acoustic-electrical energy conversion by increasing the laser power, optimizing the resonance characteristics of the photoacoustic cell (PAC), and improving the sensitivity of acoustic sensors. However, conventional systems using a single-microphone or a dual-microphone differential setup for point sampling of the photoacoustic signal fail to account for its spatial distribution, leading to a loss of spatial gain. Drawing on microphone array theory derived from sonar technology, this study, for the first time, presents a PAS sensing system based on a four-microphone array, which is applied to detect chloroform gas. The microphones are positioned at 90° intervals around the PAC resonance chamber wall, enhancing the spatial sampling rate of the signals. A digital phase-locked algorithm demodulates the combined signals from the four microphones into the concentration data. Experimental results show that, compared to a single-microphone system, the four-microphone array system increases sensitivity by a factor of 4, doubles the signal-to-noise ratio, and achieves a minimum detection limit of 69 ppb, demonstrating a significant improvement in sensitivity by capturing the spatial distribution of PA signals.
{"title":"Ppb-Level Photoacoustic Detection of Chloroform Using Four-Microphone Array","authors":"Dou Dou, Mingqi Jiao, Mingyang Feng, Mu Liang, Kaijun Mu, Yingying Qiao, Lei Li, Chongxin Shan","doi":"10.1021/acs.analchem.4c05658","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c05658","url":null,"abstract":"The photoacoustic spectroscopy (PAS) system commonly enhances the efficiency of optical-acoustic-electrical energy conversion by increasing the laser power, optimizing the resonance characteristics of the photoacoustic cell (PAC), and improving the sensitivity of acoustic sensors. However, conventional systems using a single-microphone or a dual-microphone differential setup for point sampling of the photoacoustic signal fail to account for its spatial distribution, leading to a loss of spatial gain. Drawing on microphone array theory derived from sonar technology, this study, for the first time, presents a PAS sensing system based on a four-microphone array, which is applied to detect chloroform gas. The microphones are positioned at 90° intervals around the PAC resonance chamber wall, enhancing the spatial sampling rate of the signals. A digital phase-locked algorithm demodulates the combined signals from the four microphones into the concentration data. Experimental results show that, compared to a single-microphone system, the four-microphone array system increases sensitivity by a factor of 4, doubles the signal-to-noise ratio, and achieves a minimum detection limit of 69 ppb, demonstrating a significant improvement in sensitivity by capturing the spatial distribution of PA signals.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"11 3 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-01-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142986243","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 : 2025-01-15DOI: 10.1021/acs.analchem.4c05794
Xi Gao, Jin-yu Wang, Yufei Qin, Yiling Zhu, Ya-jun Liu, Kaixiang Zhou, Mengchao Cui
The development of long-wavelength near-infrared II (NIR-II, 900–1700 nm) dyes is highly desirable but challenging. To achieve both red-shifted absorption/emission and superior in vivo imaging capabilities, a donor–acceptor–donor (D–A–D) xanthene core was strategically modified by extending π-conjugated double bonds and enhancing electron-donating properties. Two dyes named VIX-1250 and VIX-1450 were synthesized and exhibited notably red-shifted absorption/emission peaks at 942/1250 and 1098/1450 nm, respectively. Among them, VIX-1450 demonstrated superior chemo- and photostability even at such long wavelengths. Fluorescent angiography using VIX-1450 micelles enabled high-clarity blood vessel imaging with a remarkable signal-to-noise ratio (SNR), underscoring that the dye’s large Stokes shift (352 nm), good brightness (13 M–1 cm–1), and long wavelength served as key factors for high-quality in vivo biosensing. Additionally, VIX-1450 combined with ICG for dual-color imaging achieved near-zero optical cross talk, enabling different organ labeling. This study provides a new direction for the design of long-wavelength organic dyes.
{"title":"Design, Synthesis, and In Vivo Imaging of a Stable Xanthene-Based Dye with NIR-II Emission up to 1450 nm","authors":"Xi Gao, Jin-yu Wang, Yufei Qin, Yiling Zhu, Ya-jun Liu, Kaixiang Zhou, Mengchao Cui","doi":"10.1021/acs.analchem.4c05794","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c05794","url":null,"abstract":"The development of long-wavelength near-infrared II (NIR-II, 900–1700 nm) dyes is highly desirable but challenging. To achieve both red-shifted absorption/emission and superior <i>in vivo</i> imaging capabilities, a donor–acceptor–donor (D–A–D) xanthene core was strategically modified by extending π-conjugated double bonds and enhancing electron-donating properties. Two dyes named <b>VIX-1250</b> and <b>VIX-1450</b> were synthesized and exhibited notably red-shifted absorption/emission peaks at 942/1250 and 1098/1450 nm, respectively. Among them, <b>VIX-1450</b> demonstrated superior chemo- and photostability even at such long wavelengths. Fluorescent angiography using <b>VIX-1450</b> micelles enabled high-clarity blood vessel imaging with a remarkable signal-to-noise ratio (SNR), underscoring that the dye’s large Stokes shift (352 nm), good brightness (13 M<sup>–1</sup> cm<sup>–1</sup>), and long wavelength served as key factors for high-quality <i>in vivo</i> biosensing. Additionally, <b>VIX-1450</b> combined with <b>ICG</b> for dual-color imaging achieved near-zero optical cross talk, enabling different organ labeling. This study provides a new direction for the design of long-wavelength organic dyes.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"48 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-01-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142986244","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 : 2025-01-15DOI: 10.1021/acs.analchem.4c06405
Min Liu, Huanhuan Zhang, Chenzhao Wang, Kaihua Su, Kaixin Hu, Enqi Liu, Boyao Sun, Xuechun Li, Guoying Sun, Lehui Lu
Arginine (Arg) is involved in tissue metabolism and regulates the immune function; thereby, achieving the detection of Arg is crucial for early diagnosis and treatment of diseases. Herein, dual ratiometric fluorescence sensors were prepared with the blue emission of levorotatory/dextrorotatory carbon dots (CDs) and the red emission of porphyrin (L/D-CDs-PP) for the sensitive and portable detection of Arg. Interestingly, L-CDs-PP and D-CDs-PP displayed not only the dual emission peaks at 493 and 650 nm but also different response modes to Arg; thus, they could serve as dual ratiometric fluorescence sensors to achieve the accurate and reliable detection of Arg, with the detection limit of 23.87 μM for L-CDs-PP and 2.39 μM for D-CDs-PP. Importantly, the solid-state sensors successfully achieved dual-mode visual and portable detection of Arg with the support of a smartphone platform. In addition, L-CDs-PP and D-CDs-PP exhibited excellent biocompatibility and cell imaging capabilities, and they could achieve the detection of Arg in cells and biological samples of urine and rat plasma. Therefore, the dual ratiometric fluorescence sensors exhibited broad application prospects in the fields of analytical sensing, biological imaging, and medical diagnosis.
{"title":"Dual Ratiometric Fluorescence Sensors Based on Chiral Carbon Dots for the Sensitive and Specific Detection of Arginine","authors":"Min Liu, Huanhuan Zhang, Chenzhao Wang, Kaihua Su, Kaixin Hu, Enqi Liu, Boyao Sun, Xuechun Li, Guoying Sun, Lehui Lu","doi":"10.1021/acs.analchem.4c06405","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c06405","url":null,"abstract":"Arginine (Arg) is involved in tissue metabolism and regulates the immune function; thereby, achieving the detection of Arg is crucial for early diagnosis and treatment of diseases. Herein, dual ratiometric fluorescence sensors were prepared with the blue emission of levorotatory/dextrorotatory carbon dots (CDs) and the red emission of porphyrin (L/D-CDs-PP) for the sensitive and portable detection of Arg. Interestingly, L-CDs-PP and D-CDs-PP displayed not only the dual emission peaks at 493 and 650 nm but also different response modes to Arg; thus, they could serve as dual ratiometric fluorescence sensors to achieve the accurate and reliable detection of Arg, with the detection limit of 23.87 μM for L-CDs-PP and 2.39 μM for D-CDs-PP. Importantly, the solid-state sensors successfully achieved dual-mode visual and portable detection of Arg with the support of a smartphone platform. In addition, L-CDs-PP and D-CDs-PP exhibited excellent biocompatibility and cell imaging capabilities, and they could achieve the detection of Arg in cells and biological samples of urine and rat plasma. Therefore, the dual ratiometric fluorescence sensors exhibited broad application prospects in the fields of analytical sensing, biological imaging, and medical diagnosis.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"23 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-01-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142981304","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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