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Ag+-Mediated DNA Nanomachine Cascade Nanomaterial Amplification Enable One-Pot Electrochemical Analysis of Circulating Tumor DNA
IF 7.4 1区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2025-02-18 DOI: 10.1021/acs.analchem.4c06652
Runlian Qu, Zhen Zeng, Yue Wang, Ke Huang, Zeliang Wei, Kai Li, Weigang Gan, Feng Lin, Piaopiao Chen
Circular tumor DNA (ctDNA) is a trace nucleic acid that functions as an essential tumor marker. In this context, the present study proposes a one-pot electrochemical analysis of ctDNA EGFR L858R in lung cancer leveraging a Ag+-mediated DNA nanosphere (I amplification) and cation exchange reaction (II amplification), and Cu2+ acts as a signal molecule. Once the target L858R exists, it specifically destroys the structure of DNA nanosphere@Ag+, and large amounts of Ag+ are released. After the addition of copper sulfide nanoparticles, Cu2+ can be replaced by a cation exchange reaction. Eventually, the electrochemical signal of Cu2+ is elevated. The analytical performance of the method is satisfactory, L858R can be detected in the linear range of 1 aM-1 fM with a detection limit of 0.3 aM. Furthermore, the system exhibits notable selectivity in differentiating base mismatch targets and other ctDNA sequences. The recovery rate of blood samples is between 95.5 and 105%. The electrochemical results from the analysis of 42 clinical blood samples are consistent with those of the quantitative real-time polymerase chain reaction, computed tomography, and pathology results. In summary, this novel strategy utilizes preprepared functional nucleic acid nanomaterials and cascade amplification, which is expected to contribute to the sensitive and expeditious detection of trace nucleic acids.
{"title":"Ag+-Mediated DNA Nanomachine Cascade Nanomaterial Amplification Enable One-Pot Electrochemical Analysis of Circulating Tumor DNA","authors":"Runlian Qu, Zhen Zeng, Yue Wang, Ke Huang, Zeliang Wei, Kai Li, Weigang Gan, Feng Lin, Piaopiao Chen","doi":"10.1021/acs.analchem.4c06652","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c06652","url":null,"abstract":"Circular tumor DNA (ctDNA) is a trace nucleic acid that functions as an essential tumor marker. In this context, the present study proposes a one-pot electrochemical analysis of ctDNA EGFR L858R in lung cancer leveraging a Ag<sup>+</sup>-mediated DNA nanosphere (I amplification) and cation exchange reaction (II amplification), and Cu<sup>2+</sup> acts as a signal molecule. Once the target L858R exists, it specifically destroys the structure of DNA nanosphere@Ag<sup>+</sup>, and large amounts of Ag<sup>+</sup> are released. After the addition of copper sulfide nanoparticles, Cu<sup>2+</sup> can be replaced by a cation exchange reaction. Eventually, the electrochemical signal of Cu<sup>2+</sup> is elevated. The analytical performance of the method is satisfactory, L858R can be detected in the linear range of 1 aM-1 fM with a detection limit of 0.3 aM. Furthermore, the system exhibits notable selectivity in differentiating base mismatch targets and other ctDNA sequences. The recovery rate of blood samples is between 95.5 and 105%. The electrochemical results from the analysis of 42 clinical blood samples are consistent with those of the quantitative real-time polymerase chain reaction, computed tomography, and pathology results. In summary, this novel strategy utilizes preprepared functional nucleic acid nanomaterials and cascade amplification, which is expected to contribute to the sensitive and expeditious detection of trace nucleic acids.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"7 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-02-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143435729","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}
引用次数: 0
Functional Aptamers In Vitro Evolution for Protein–Protein Interaction Blockage
IF 7.4 1区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2025-02-18 DOI: 10.1021/acs.analchem.4c04609
Tongxuan Wei, Qinguo Liu, Jun Li, Song Song, Liqin Zhang
As aptamer development progresses, their applications have expanded significantly beyond high affinity to include functional capabilities. Currently, the identification of functional aptamers relies on traditional SELEX techniques, followed by functional validation and computer-assisted redesign of high-affinity aptamers. However, high affinity does not guarantee optimal functionality, making the search for functional aptamers from binding pools time-consuming and labor-intensive. Addressing this challenge, we introduce functional aptamers in vitro evolution (FAIVE), a novel screening method that links sequence functionality to fluorescence intensity. We demonstrated the effectiveness of FAIVE by obtaining modified DNA aptamers capable of disrupting the interaction between the SARS-CoV-2 spike receptor-binding domain (RBD) and hACE2, targeting protein–protein interaction inhibition. Furthermore, we investigated the criteria for validating the quality of the bead library generated for selection by modeling the emulsion PCR process, providing theoretical insights for future applications. The concept of incorporating fluorescent signal reporting of aptamer functionality into the aptamer selection process holds the potential to facilitate the identification of aptamers with diverse functionalities and is readily adaptable to various research contexts.
{"title":"Functional Aptamers In Vitro Evolution for Protein–Protein Interaction Blockage","authors":"Tongxuan Wei, Qinguo Liu, Jun Li, Song Song, Liqin Zhang","doi":"10.1021/acs.analchem.4c04609","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c04609","url":null,"abstract":"As aptamer development progresses, their applications have expanded significantly beyond high affinity to include functional capabilities. Currently, the identification of functional aptamers relies on traditional SELEX techniques, followed by functional validation and computer-assisted redesign of high-affinity aptamers. However, high affinity does not guarantee optimal functionality, making the search for functional aptamers from binding pools time-consuming and labor-intensive. Addressing this challenge, we introduce functional aptamers <i>in vitro</i> evolution (FAIVE), a novel screening method that links sequence functionality to fluorescence intensity. We demonstrated the effectiveness of FAIVE by obtaining modified DNA aptamers capable of disrupting the interaction between the SARS-CoV-2 spike receptor-binding domain (RBD) and hACE2, targeting protein–protein interaction inhibition. Furthermore, we investigated the criteria for validating the quality of the bead library generated for selection by modeling the emulsion PCR process, providing theoretical insights for future applications. The concept of incorporating fluorescent signal reporting of aptamer functionality into the aptamer selection process holds the potential to facilitate the identification of aptamers with diverse functionalities and is readily adaptable to various research contexts.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"13 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-02-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143435624","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}
引用次数: 0
Advancing Biomarker Research: In Situ Cu Isotope Analysis in Liver Tumors by LA-MC-ICP-MS
IF 7.4 1区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2025-02-18 DOI: 10.1021/acs.analchem.4c05626
Mathias Schannor, Marcus Oelze, Heike Traub, Yubei He, Robin Schmidt, Luisa Heidemann, Lynn Jeanette Savic, Jochen Vogl, Björn Meermann
Stable metal isotopes have received increasing attention as medical biomarkers due to their potential to detect changes in metal metabolism related to diseases. In particular, copper stable isotopes are a powerful tool to identify isotopic variation between tumors and healthy tissue, suggesting application in cancer diagnosis. However, potential mechanisms causing isotope fractionation, such as redox- or bond-forming reactions and interactions of metals during transmembrane import and export, are less well understood. Here, we established an <i>in situ</i> method using laser ablation-multicollector-inductively coupled plasma-mass spectrometry (LA-MC-ICP-MS) to advance our understanding of the underlying processes responsible for isotope fractionation between normal and diseased tissues. Gelatin-based bracketing standards and quality control reference materials, crucial for laser ablation analysis, were developed to allow correction for instrumentally induced isotope fractionation during LA-MC-ICP-MS analysis. Using such matrix-matched standards, the method achieved intermediate precisions for delta values of better than 0.15 ‰ (2 <i>s</i>) for inorganic reference materials and of better than 0.17 ‰ (2 <i>s</i>) for biological reference materials. The developed routine was tested on rabbit VX2 liver tumor samples, a model system resembling human hepatocellular carcinoma (HCC) used to study liver cancer. <i>In situ</i> Cu isotope compositions between healthy (<i></i><span style="color: inherit;"></span><span data-mathml='<math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><msubsup><mrow><mi>&#x3B4;</mi></mrow><mrow><mi>NIST</mi><mn>976</mn></mrow><mrow><mi>65/63</mi></mrow></msubsup><mrow><mo stretchy="false">(</mo><mi>Cu</mi><mo stretchy="false">)</mo></mrow></math>' role="presentation" style="position: relative;" tabindex="0"><nobr aria-hidden="true"><span style="width: 5.514em; display: inline-block;"><span style="display: inline-block; position: relative; width: 5.003em; height: 0px; font-size: 110%;"><span style="position: absolute; clip: rect(1.48em, 1004.95em, 3.014em, -999.997em); top: -2.554em; left: 0em;"><span><span><span style="display: inline-block; position: relative; width: 3.185em; height: 0px;"><span style="position: absolute; clip: rect(3.128em, 1000.46em, 4.151em, -999.997em); top: -3.974em; left: 0em;"><span><span style="font-family: STIXMathJax_Normal-italic;">𝛿</span></span><span style="display: inline-block; width: 0px; height: 3.98em;"></span></span><span style="position: absolute; clip: rect(3.298em, 1001.71em, 4.151em, -999.997em); top: -4.372em; left: 0.457em;"><span><span style="font-size: 70.7%; font-family: STIXMathJax_Main;">65/63</span></span><span style="display: inline-block; width: 0px; height: 3.98em;"></span></span><span style="position: ab
{"title":"Advancing Biomarker Research: In Situ Cu Isotope Analysis in Liver Tumors by LA-MC-ICP-MS","authors":"Mathias Schannor, Marcus Oelze, Heike Traub, Yubei He, Robin Schmidt, Luisa Heidemann, Lynn Jeanette Savic, Jochen Vogl, Björn Meermann","doi":"10.1021/acs.analchem.4c05626","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c05626","url":null,"abstract":"Stable metal isotopes have received increasing attention as medical biomarkers due to their potential to detect changes in metal metabolism related to diseases. In particular, copper stable isotopes are a powerful tool to identify isotopic variation between tumors and healthy tissue, suggesting application in cancer diagnosis. However, potential mechanisms causing isotope fractionation, such as redox- or bond-forming reactions and interactions of metals during transmembrane import and export, are less well understood. Here, we established an &lt;i&gt;in situ&lt;/i&gt; method using laser ablation-multicollector-inductively coupled plasma-mass spectrometry (LA-MC-ICP-MS) to advance our understanding of the underlying processes responsible for isotope fractionation between normal and diseased tissues. Gelatin-based bracketing standards and quality control reference materials, crucial for laser ablation analysis, were developed to allow correction for instrumentally induced isotope fractionation during LA-MC-ICP-MS analysis. Using such matrix-matched standards, the method achieved intermediate precisions for delta values of better than 0.15 ‰ (2 &lt;i&gt;s&lt;/i&gt;) for inorganic reference materials and of better than 0.17 ‰ (2 &lt;i&gt;s&lt;/i&gt;) for biological reference materials. The developed routine was tested on rabbit VX2 liver tumor samples, a model system resembling human hepatocellular carcinoma (HCC) used to study liver cancer. &lt;i&gt;In situ&lt;/i&gt; Cu isotope compositions between healthy (&lt;i&gt;&lt;/i&gt;&lt;span style=\"color: inherit;\"&gt;&lt;/span&gt;&lt;span data-mathml='&lt;math xmlns=\"http://www.w3.org/1998/Math/MathML\" display=\"inline\"&gt;&lt;msubsup&gt;&lt;mrow&gt;&lt;mi&gt;&amp;#x3B4;&lt;/mi&gt;&lt;/mrow&gt;&lt;mrow&gt;&lt;mi&gt;NIST&lt;/mi&gt;&lt;mn&gt;976&lt;/mn&gt;&lt;/mrow&gt;&lt;mrow&gt;&lt;mi&gt;65/63&lt;/mi&gt;&lt;/mrow&gt;&lt;/msubsup&gt;&lt;mrow&gt;&lt;mo stretchy=\"false\"&gt;(&lt;/mo&gt;&lt;mi&gt;Cu&lt;/mi&gt;&lt;mo stretchy=\"false\"&gt;)&lt;/mo&gt;&lt;/mrow&gt;&lt;/math&gt;' role=\"presentation\" style=\"position: relative;\" tabindex=\"0\"&gt;&lt;nobr aria-hidden=\"true\"&gt;&lt;span style=\"width: 5.514em; display: inline-block;\"&gt;&lt;span style=\"display: inline-block; position: relative; width: 5.003em; height: 0px; font-size: 110%;\"&gt;&lt;span style=\"position: absolute; clip: rect(1.48em, 1004.95em, 3.014em, -999.997em); top: -2.554em; left: 0em;\"&gt;&lt;span&gt;&lt;span&gt;&lt;span style=\"display: inline-block; position: relative; width: 3.185em; height: 0px;\"&gt;&lt;span style=\"position: absolute; clip: rect(3.128em, 1000.46em, 4.151em, -999.997em); top: -3.974em; left: 0em;\"&gt;&lt;span&gt;&lt;span style=\"font-family: STIXMathJax_Normal-italic;\"&gt;𝛿&lt;/span&gt;&lt;/span&gt;&lt;span style=\"display: inline-block; width: 0px; height: 3.98em;\"&gt;&lt;/span&gt;&lt;/span&gt;&lt;span style=\"position: absolute; clip: rect(3.298em, 1001.71em, 4.151em, -999.997em); top: -4.372em; left: 0.457em;\"&gt;&lt;span&gt;&lt;span style=\"font-size: 70.7%; font-family: STIXMathJax_Main;\"&gt;65/63&lt;/span&gt;&lt;/span&gt;&lt;span style=\"display: inline-block; width: 0px; height: 3.98em;\"&gt;&lt;/span&gt;&lt;/span&gt;&lt;span style=\"position: ab","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"21 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-02-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143435625","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}
引用次数: 0
Electrochemiluminescence Biosensor Based on a Self-protected DNAzyme Walker with a Circular Bulging DNA Shield for MicroRNA Detection
IF 7.4 1区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2025-02-18 DOI: 10.1021/acs.analchem.4c06552
Juan Zhang, Haonan He, Shimao Du, Benting Xie, Hejun Gao, Hongquan Fu, Yunwen Liao
Herein, an electrochemiluminescence (ECL) biosensor is established for the ultrasensitive detection of microRNA (miRNA) by integrating a self-protected DNAzyme walker machine on a Au nanoparticle–modified electrode. Using Let-7a miRNA as the model target and by introducing a target-binding domain into the middle of the catalytic core, the catalytic core of the DNAzyme walker is separated by a target-binding domain that can inhibit the cleavage activity and serve as an arch-like protective shield, resulting in a self-protected DNAzyme walker. High-efficiency hybridization between the target Let-7a miRNA and the target-binding domain activates the DNAzyme walker machine, enabling high catalytic cleavage of its substrate without requiring additional energy input. Importantly, each step of the DNAzyme walker results in the cleavage of a substrate strand and the liberation of a Ru(bpy)2(mcpbpy)2+ (Ru)-labeled DNA fragment, considerably reducing the ECL signal of Ru. Under optimized experimental conditions, the limit of detection of Let-7a miRNA is 51.4 aM within a wide linear range of 100 aM–100 pM. This proposed strategy is a bold innovation in the rapid and sensitive detection of low-abundance biomarkers, offering a promising application for early cancer diagnosis and relevant research.
{"title":"Electrochemiluminescence Biosensor Based on a Self-protected DNAzyme Walker with a Circular Bulging DNA Shield for MicroRNA Detection","authors":"Juan Zhang, Haonan He, Shimao Du, Benting Xie, Hejun Gao, Hongquan Fu, Yunwen Liao","doi":"10.1021/acs.analchem.4c06552","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c06552","url":null,"abstract":"Herein, an electrochemiluminescence (ECL) biosensor is established for the ultrasensitive detection of microRNA (miRNA) by integrating a self-protected DNAzyme walker machine on a Au nanoparticle–modified electrode. Using Let-7a miRNA as the model target and by introducing a target-binding domain into the middle of the catalytic core, the catalytic core of the DNAzyme walker is separated by a target-binding domain that can inhibit the cleavage activity and serve as an arch-like protective shield, resulting in a self-protected DNAzyme walker. High-efficiency hybridization between the target Let-7a miRNA and the target-binding domain activates the DNAzyme walker machine, enabling high catalytic cleavage of its substrate without requiring additional energy input. Importantly, each step of the DNAzyme walker results in the cleavage of a substrate strand and the liberation of a Ru(bpy)<sub>2</sub>(mcpbpy)<sup>2+</sup> (Ru)-labeled DNA fragment, considerably reducing the ECL signal of Ru. Under optimized experimental conditions, the limit of detection of Let-7a miRNA is 51.4 aM within a wide linear range of 100 aM–100 pM. This proposed strategy is a bold innovation in the rapid and sensitive detection of low-abundance biomarkers, offering a promising application for early cancer diagnosis and relevant research.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"24 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-02-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143435626","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}
引用次数: 0
Single-Cell/Particle Sample Introduction Device for Mass Cytometry Based on Gas-Driven Flow Focusing
IF 7.4 1区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2025-02-17 DOI: 10.1021/acs.analchem.4c06466
Huaiyi Chen, Jinhui Liu, Yu Zhao, Haitao Xu, Weiliang Liu, Zhi Xing, Fei Tang, Sichun Zhang, Xinrong Zhang
Mass cytometry is considered the second generation of flow cytometry technology, which uses metal-labeled antibodies instead of traditional fluorescent antibodies and can measure much more markers from a single cell simultaneously. However, due to frequent clogging of the capillary and nebulizer, it is still a complicated task to perform the sample introduction smoothly for a long-term determination. Herein, a plug-and-play sample introduction device for mass cytometry analysis was developed based on a gas-driven flow focusing protocol. The device is integrated with a virtual hole to generate liquid jet and omit a conventional nebulizer. Single-cell monodispersion can be achieved by liquid jet breakup instead of the commonly used nebulization by the Venturi effect, thus avoiding clogging of thin central capillary. The device has high universality and compatibility and can be plug-and-play on a mass cytometry instrument or common inductively coupled plasma mass spectrometry for single-cell or single-particle determination. High-speed microscopy imaging was used to capture and study the dynamic processes of monodispersion on microsphere suspensions achieved by the device. We also compared the analysis capabilities when using the device and a conventional nebulizer in mass cytometry analysis of four element calibration beads and cell samples. The results obtained by using the flow focusing device and the conventional nebulizer show great consistency, which means the device has no negative impact on the detection performance of mass cytometry and single-cell/particle monodispersion can be achieved without clogging.
{"title":"Single-Cell/Particle Sample Introduction Device for Mass Cytometry Based on Gas-Driven Flow Focusing","authors":"Huaiyi Chen, Jinhui Liu, Yu Zhao, Haitao Xu, Weiliang Liu, Zhi Xing, Fei Tang, Sichun Zhang, Xinrong Zhang","doi":"10.1021/acs.analchem.4c06466","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c06466","url":null,"abstract":"Mass cytometry is considered the second generation of flow cytometry technology, which uses metal-labeled antibodies instead of traditional fluorescent antibodies and can measure much more markers from a single cell simultaneously. However, due to frequent clogging of the capillary and nebulizer, it is still a complicated task to perform the sample introduction smoothly for a long-term determination. Herein, a plug-and-play sample introduction device for mass cytometry analysis was developed based on a gas-driven flow focusing protocol. The device is integrated with a virtual hole to generate liquid jet and omit a conventional nebulizer. Single-cell monodispersion can be achieved by liquid jet breakup instead of the commonly used nebulization by the Venturi effect, thus avoiding clogging of thin central capillary. The device has high universality and compatibility and can be plug-and-play on a mass cytometry instrument or common inductively coupled plasma mass spectrometry for single-cell or single-particle determination. High-speed microscopy imaging was used to capture and study the dynamic processes of monodispersion on microsphere suspensions achieved by the device. We also compared the analysis capabilities when using the device and a conventional nebulizer in mass cytometry analysis of four element calibration beads and cell samples. The results obtained by using the flow focusing device and the conventional nebulizer show great consistency, which means the device has no negative impact on the detection performance of mass cytometry and single-cell/particle monodispersion can be achieved without clogging.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"49 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-02-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143427106","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}
引用次数: 0
Removal of Homogeneous Broadening from 1H-Detected Multidimensional Solid-State NMR Spectra
IF 7.4 1区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2025-02-17 DOI: 10.1021/acs.analchem.4c06696
Frédéric A. Perras, Songlin Wang, Jacob Mayer, Mita Halder, Alexander L. Paterson, Damien B. Culver, Chad M. Rienstra
1H-detected magic-angle spinning (MAS) NMR experiments have revolutionized the NMR studies of biological and inorganic solids by providing unparalleled sensitivity and resolution. Despite these gains, homogeneous broadening, originating from the incomplete removal of homonuclear dipolar interactions under fast MAS, remains highly prevalent and limits the achievable resolution. In direct analogy to super-resolution microscopy methods, we show that resolution beyond that currently achievable by fast MAS alone can be obtained by experiment-driven deconvolution. Following the acquisition of a single 2D NMR spectrum to measure the frequency-dependent homogeneous lineshapes, any number of 1H-detected spectra can be enhanced in resolution, yielding comparable spectra as obtained with twice the MAS frequency. The versatility of this approach is demonstrated in the enhancement of single- and double-quantum homonuclear correlation spectra, in addition to heteronuclear correlation spectra acquired on a surface organometallic complex and the protein GB1.
{"title":"Removal of Homogeneous Broadening from 1H-Detected Multidimensional Solid-State NMR Spectra","authors":"Frédéric A. Perras, Songlin Wang, Jacob Mayer, Mita Halder, Alexander L. Paterson, Damien B. Culver, Chad M. Rienstra","doi":"10.1021/acs.analchem.4c06696","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c06696","url":null,"abstract":"<sup>1</sup>H-detected magic-angle spinning (MAS) NMR experiments have revolutionized the NMR studies of biological and inorganic solids by providing unparalleled sensitivity and resolution. Despite these gains, homogeneous broadening, originating from the incomplete removal of homonuclear dipolar interactions under fast MAS, remains highly prevalent and limits the achievable resolution. In direct analogy to super-resolution microscopy methods, we show that resolution beyond that currently achievable by fast MAS alone can be obtained by experiment-driven deconvolution. Following the acquisition of a single 2D NMR spectrum to measure the frequency-dependent homogeneous lineshapes, any number of <sup>1</sup>H-detected spectra can be enhanced in resolution, yielding comparable spectra as obtained with twice the MAS frequency. The versatility of this approach is demonstrated in the enhancement of single- and double-quantum homonuclear correlation spectra, in addition to heteronuclear correlation spectra acquired on a surface organometallic complex and the protein GB1.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"64 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-02-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143435728","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}
引用次数: 0
Electronic Chemical Sensors Based on Conductive Framework Materials
IF 7.4 1区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2025-02-17 DOI: 10.1021/acs.analchem.4c02522
Emma K. Ambrogi, Katherine A. Mirica
The development of portable electronic chemical sensors is key to solving a number of challenges, including monitoring environmental and industrial hazards, as well as understanding and improving human health. Framework materials possess several desirable characteristics that make them well-suited for electroanalytical applications, including high surface area, atomically precise distribution of active sites, and tunable properties that can be leveraged through modular reticular chemistry. This review highlights the emergence of conductive framework materials as active components in electrically transduced chemical sensors, including the development of new materials for the detection of a wide variety of analytes in both gas and liquid phase. The efforts to gain fundamental understanding of the molecular interactions and sensing mechanisms between framework materials and analytes are described, along with applications of these materials on portable and flexible substrates. The review suggests areas for further study, including the study of material–analyte interactions at the molecular level and the continued development of scalable methods for the integration of framework materials into low-power, portable sensing devices.
{"title":"Electronic Chemical Sensors Based on Conductive Framework Materials","authors":"Emma K. Ambrogi, Katherine A. Mirica","doi":"10.1021/acs.analchem.4c02522","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c02522","url":null,"abstract":"The development of portable electronic chemical sensors is key to solving a number of challenges, including monitoring environmental and industrial hazards, as well as understanding and improving human health. Framework materials possess several desirable characteristics that make them well-suited for electroanalytical applications, including high surface area, atomically precise distribution of active sites, and tunable properties that can be leveraged through modular reticular chemistry. This review highlights the emergence of conductive framework materials as active components in electrically transduced chemical sensors, including the development of new materials for the detection of a wide variety of analytes in both gas and liquid phase. The efforts to gain fundamental understanding of the molecular interactions and sensing mechanisms between framework materials and analytes are described, along with applications of these materials on portable and flexible substrates. The review suggests areas for further study, including the study of material–analyte interactions at the molecular level and the continued development of scalable methods for the integration of framework materials into low-power, portable sensing devices.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"32 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-02-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143427104","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}
引用次数: 0
Structural Lipidomics Enabled by Isomer-Resolved Tandem Mass Spectrometry
IF 7.4 1区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2025-02-17 DOI: 10.1021/acs.analchem.4c06680
Yikun Liu, Yu Xia, Wenpeng Zhang
This article has not yet been cited by other publications.
{"title":"Structural Lipidomics Enabled by Isomer-Resolved Tandem Mass Spectrometry","authors":"Yikun Liu, Yu Xia, Wenpeng Zhang","doi":"10.1021/acs.analchem.4c06680","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c06680","url":null,"abstract":"This article has not yet been cited by other publications.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"64 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-02-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143427107","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}
引用次数: 0
Bidirectionally Favorable Platform: A Dual-Targeting Probe-Encoded Maple Leaf-Type Fluorescent Lateral Flow Immunoassay for Multiple Biomarker Detection
IF 7.4 1区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2025-02-17 DOI: 10.1021/acs.analchem.4c06414
Siqi Zeng, Wanchao Zuo, Huilin Zhang, Jiaren Song, Qing Yang, Qiannan Hu, Xiangming Meng, Wenxuan Chen, Yazhou Wang, Jianjun Dai, Yanmin Ju
In the traditional multiplexed lateral flow immunoassay (LFIA), different detection probes against different targets are necessary. However, the relative complexity and high cost of probe preparation, as well as the insufficient user-friendliness, limit the application of the multiplexed LFIA in disease diagnosis. Here, we reported a bidirectionally favorable LFIA (BDF-LFIA) platform to maximize convenience for both manufacturers and users. Red-emitting time-resolved fluorescent nanoparticles were coated with different antibodies to recognize multiple targets simultaneously, which greatly simplified probe preparation by the manufacturers. Ultrabright green-emitting gold nanoclusters were pre-embedded on the test line as a reference signal to achieve a target concentration-dependent maple leaf-type hue readout from green to yellow to red, which was quite user-friendly. Taking cancer biomarkers alpha-fetoprotein and carcinoembryonic antigen as examples, this assay achieved a visual detection limit of 2 ng/mL. Compared with the conventional fluorescent LFIA, the BDF-LFIA could generate a more discernible signal around the threshold concentration of the targets. Moreover, the assay successfully diagnosed 54 clinical samples. Overall, the BDF-LFIA showed bidirectional benefits for both manufacturers and users and provided a new concept for the LFIA in multiplexed detection.
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引用次数: 0
Increased Sensitivity in VOC Detection by Using a Novel Photoinduced Multiple Ionization Mass Spectrometry
IF 7.4 1区 化学 Q1 CHEMISTRY, ANALYTICAL Pub Date : 2025-02-17 DOI: 10.1021/acs.analchem.4c05873
Xun Bao, Qu Liang, Qiangling Zhang, Xue Zou, Chaoqun Huang, Chengyin Shen, Yannan Chu
Proton transfer reaction mass spectrometry (PTR-MS) is an important online monitoring technique for volatile organic compounds (VOCs). VOCs have the characteristics of many types, rapid change, and low concentration. Enhancing the detection sensitivity and expanding the detection range of VOCs have been key challenges in PTR-MS research. In this work, we have developed and characterized a novel photoinduced multiple ionizations (PMI) source, which consists of four direct current (DC) vacuum ultraviolet Kr lamps and a V-shaped focusing quadrupole ion funnel (FQ-IF) drift tube. The novel PMI source has four ionization processes: proton transfer reaction, charge transfer reaction, single photon ionization, and photoelectron impact ionization. It is capable of detecting VOCs detectable by conventional PTR-MS via the PTR, as well as VOCs (carbon disulfide and acetylene) that are difficult to detect by conventional PTR-MS through other ionization processes, thus effectively expanding the detection range. In further comparative experiments, the improvements in sensitivity for the PMI-MS in FQ-IF mode range from 122.5 to 647.7 times compared to the PTR-MS in DC mode (conventional PTR-MS) for 12 test VOCs. Notably, the sensitivities of four BTEXs in 12 VOCs were more than 10,000 cps/ppb. Moreover, compared with PTR-MS in DC mode, the LOD of PMI-MS in FQ-IF mode for 12 test VOCs increased by 26–128.6 times. PMI-MS not only expands the detection range but also improves the sensitivity by 2 orders of magnitude, which would provide an important tool for the detection of ultratrace VOCs.
{"title":"Increased Sensitivity in VOC Detection by Using a Novel Photoinduced Multiple Ionization Mass Spectrometry","authors":"Xun Bao, Qu Liang, Qiangling Zhang, Xue Zou, Chaoqun Huang, Chengyin Shen, Yannan Chu","doi":"10.1021/acs.analchem.4c05873","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c05873","url":null,"abstract":"Proton transfer reaction mass spectrometry (PTR-MS) is an important online monitoring technique for volatile organic compounds (VOCs). VOCs have the characteristics of many types, rapid change, and low concentration. Enhancing the detection sensitivity and expanding the detection range of VOCs have been key challenges in PTR-MS research. In this work, we have developed and characterized a novel photoinduced multiple ionizations (PMI) source, which consists of four direct current (DC) vacuum ultraviolet Kr lamps and a V-shaped focusing quadrupole ion funnel (FQ-IF) drift tube. The novel PMI source has four ionization processes: proton transfer reaction, charge transfer reaction, single photon ionization, and photoelectron impact ionization. It is capable of detecting VOCs detectable by conventional PTR-MS via the PTR, as well as VOCs (carbon disulfide and acetylene) that are difficult to detect by conventional PTR-MS through other ionization processes, thus effectively expanding the detection range. In further comparative experiments, the improvements in sensitivity for the PMI-MS in FQ-IF mode range from 122.5 to 647.7 times compared to the PTR-MS in DC mode (conventional PTR-MS) for 12 test VOCs. Notably, the sensitivities of four BTEXs in 12 VOCs were more than 10,000 cps/ppb. Moreover, compared with PTR-MS in DC mode, the LOD of PMI-MS in FQ-IF mode for 12 test VOCs increased by 26–128.6 times. PMI-MS not only expands the detection range but also improves the sensitivity by 2 orders of magnitude, which would provide an important tool for the detection of ultratrace VOCs.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"2 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-02-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143427105","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}
引用次数: 0
期刊
Analytical Chemistry
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