Analytical Chemistry最新文献_第4页

Improved Hematology Analysis Based on Microfluidic Impedance Spectroscopy: Erythrocyte Orientation and Anisotropic Dielectric Properties of Flowing Blood 基于微流控阻抗光谱技术的血液分析改进：流动血液的红细胞定向和各向异性介电特性

IF 7.4 1区化学

Analytical Chemistry Pub Date : 2025-01-25 DOI: 10.1021/acs.analchem.4c03975

Alexander Zhbanov, Ye Sung Lee, Minkook Son, Byung Jun Kim, Sung Yang

{"title":"Improved Hematology Analysis Based on Microfluidic Impedance Spectroscopy: Erythrocyte Orientation and Anisotropic Dielectric Properties of Flowing Blood","authors":"Alexander Zhbanov, Ye Sung Lee, Minkook Son, Byung Jun Kim, Sung Yang","doi":"10.1021/acs.analchem.4c03975","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c03975","url":null,"abstract":"Electrochemical impedance spectroscopy has great potential for laboratory blood tests. The overall aim of this study is to develop a microfluidic sensor for determining the physical properties and hematological parameters of blood based on its dielectric spectra. Impedance was measured in flowing blood to prevent aggregation and sedimentation at frequencies between 40 Hz and 110 MHz. Two major factors make accurate analysis of impedance spectra difficult: forced orientation of erythrocytes in a microchannel and hemoglobin hydration. A theoretical approach based on the effective medium theory was applied to find the preferred erythrocyte orientation and dielectric properties of blood components. The cytoplasm of erythrocytes was considered a colloidal suspension of hemoglobin molecules surrounded by a double hydration shell. The proposed preferred orientation factor demonstrates that approximately 66% of the erythrocytes in the microfluidic channel have a random distribution and approximately 34% of them occupy random positions and are oriented along the blood flow. The experiments did not reveal any significant changes in the preferred orientation factor when the blood flow rate changed from 2 to 20 mL/h. Finally, several hematological parameters of blood samples were determined (erythrocyte count, hemoglobin level, hematocrit, mean corpuscular volume, mean corpuscular hemoglobin, and mean corpuscular hemoglobin concentration). A comparison of routine hematological studies and the developed technique proves its effectiveness.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"1 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-01-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143035040","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

Deep-Learning-Assisted Digital Fluorescence Immunoassay on Magnetic Beads for Ultrasensitive Determination of Protein Biomarkers

IF 7.4 1区化学

Analytical Chemistry Pub Date : 2025-01-24 DOI: 10.1021/acs.analchem.4c05877

Jian Zhang, Wenshuai Zhou, Honglan Qi, Xiaowei He

{"title":"Deep-Learning-Assisted Digital Fluorescence Immunoassay on Magnetic Beads for Ultrasensitive Determination of Protein Biomarkers","authors":"Jian Zhang, Wenshuai Zhou, Honglan Qi, Xiaowei He","doi":"10.1021/acs.analchem.4c05877","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c05877","url":null,"abstract":"Digital fluorescence immunoassay (DFI) based on random dispersion magnetic beads (MBs) is one of the powerful methods for ultrasensitive determination of protein biomarkers. However, in the DFI, improving the limit of detection (LOD) is challenging since the ratio of signal-to-background and the speed of manual counting beads are low. Herein, we developed a deep-learning network (ATTBeadNet) by utilizing a new hybrid attention mechanism within a UNet3+ framework for accurately and fast counting the MBs and proposed a DFI using CdS quantum dots (QDs) with narrow peak and optical stability as reported at first time. The developed ATTBeadNet was applied to counting the MBs, resulting in the F1 score (95.91%) being higher than those of other methods (ImageJ, 68.33%; computer vision-based, 92.99%; fully convolutional network, 75.00%; mask region-based convolutional neural network, 70.34%). On principle-on-proof, a sandwich MB-based DFI was proposed, in which human interleukin-6 (IL-6) was taken as a model protein biomarker, while antibody-bound streptavidin-coated MBs were used as capture MBs and antibody-HRP-tyramide-functionalized CdS QDs were used as the binding reporter. When the developed ATTBeadNet was applied to the MB-based DFI of IL-6 (20 μL), the linear range from 5 to 100 fM and an LOD of 3.1 fM were achieved, which are better than those using the ImageJ method (linear range from 30 to 100 fM and LOD of 20 fM). This work demonstrates that the integration of the deep-learning network with DFI is a promising strategy for the highly sensitive and accurate determination of protein biomarkers.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"9 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-01-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143027032","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

Suppression of Collision-Induced Dissociation in a Supersonically Expanding Gas

IF 7.4 1区化学

Analytical Chemistry Pub Date : 2025-01-24 DOI: 10.1021/acs.analchem.4c06342

Uma Namangalam, Salvi Mohandas, Hemanth Dinesan, Sunil Kumar S.

引用次数: 0

Energy Resolved Mass Spectrometry Data from Surfaced Induced Dissociation Improves Prediction of Protein Complex Structure

IF 7.4 1区化学

Analytical Chemistry Pub Date : 2025-01-24 DOI: 10.1021/acs.analchem.4c05837

Robert M. Bolz, Justin T. Seffernick, Zachary C. Drake, Sophie R. Harvey, Vicki H. Wysocki, Steffen Lindert

{"title":"Energy Resolved Mass Spectrometry Data from Surfaced Induced Dissociation Improves Prediction of Protein Complex Structure","authors":"Robert M. Bolz, Justin T. Seffernick, Zachary C. Drake, Sophie R. Harvey, Vicki H. Wysocki, Steffen Lindert","doi":"10.1021/acs.analchem.4c05837","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c05837","url":null,"abstract":"Native Mass Spectrometry (nMS) is a versatile technique for elucidating protein structure. Surface-Induced Dissociation (SID) is an activation method in tandem MS predominantly employed for determining protein complex stoichiometry alongside information about interface strengths. SID-nMS data can be collected over a range of acceleration energies, yielding Energy Resolved Mass Spectrometry (ERMS) data. Previous work demonstrated that the onset and appearance energy from SID-nMS can be used in integrative computational and experimental modeling to guide multimeric structure determination in some cases. However, the appearance energy is a single data point, while the ERMS data provide a full pattern of interface breakage. We hypothesized that incorporation of ERMS data into multimeric protein structure prediction would significantly outperform appearance energy. To test this hypothesis, we generated models of 20 protein complexes with RosettaDock using subunits generated from AlphaFold2. We simulated the ERMS data for each predicted model and rescored based on its agreement to experimental ERMS data. We demonstrated that more accurately predicted models exhibited simulated ERMS data in better agreement with the experimental data. As part of our ERMS-based rescoring, we matched or improved the RMSD of the best scoring model compared to Rosetta in 16 out of 20 cases, with 4 out of 20 cases improving to become a highly accurate (below 5 Å) structure. Finally, we benchmarked our method against our previously published appearance energy-based rescoring and showed improvement in 14 out of 20 cases, with 6 out of 20 becoming a highly accurate (below 5 Å) model. Our method is freely available through Rosetta Commons, with a usage tutorial and test files provided in the Supporting Information.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"120 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-01-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143031170","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

Silver Microdisc Array Electrode Chip for Urea Detection in Saliva Samples from Patients with Chronic Nephritis

IF 7.4 1区化学

Analytical Chemistry Pub Date : 2025-01-24 DOI: 10.1021/acs.analchem.4c05823

Xingyu Meng, Bingbing Pan, Hongyi Tong, Yaojin Xu, Meihong Peng, Qiongjing Yuan, Jiao Quan, Sijue Zou, Baisheng Wang, Zhangzhe Peng, Yi-Ge Zhou

{"title":"Silver Microdisc Array Electrode Chip for Urea Detection in Saliva Samples from Patients with Chronic Nephritis","authors":"Xingyu Meng, Bingbing Pan, Hongyi Tong, Yaojin Xu, Meihong Peng, Qiongjing Yuan, Jiao Quan, Sijue Zou, Baisheng Wang, Zhangzhe Peng, Yi-Ge Zhou","doi":"10.1021/acs.analchem.4c05823","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c05823","url":null,"abstract":"Urea is an important biomarker for diagnosing various kidney and liver disorders. However, many existing methods rely on invasive blood sampling, which can potentially harm patients. Saliva has been recently recognized as a noninvasive and easily collectible alternative to blood for urea quantification. Electrochemical urea detection in saliva remains limited, with catalytic materials typically applied to the electrode surface via drop casting. This results in a random distribution of materials and potential aggregation on the electrode, which inevitably hinders the efficient mass transport of analytes, reducing both detection sensitivity and the utilization of catalytic materials. In this work, a silver nanoparticle (AgNP)-integrated microdisc array electrode chip was fabricated through the in situ growth of AgNPs on polydopamine (PDA) arrays, which were patterned using the microcontact printing (μCP) technique on an indium tin oxide (ITO) glassy substrate. The resulting AgNP microdisc array chip sensor exhibited much higher sensitivity toward urea sensing and greater material utilization as compared to traditional drop-cast electrodes, due to the enhanced mass transfer. Furthermore, the chip sensors demonstrated superior selectivity when challenged with potential interferences. More importantly, reliable urea quantification was achieved in clinical saliva samples from nephritis patients. These results indicate that the current sensor presents great opportunities for developing a noninvasive and sensitive liquid biopsy platform for urea determination in clinical diagnosis applications.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"2 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-01-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143027029","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

Amplification Bias-Free Sequence-Generic Exponential Amplification Reaction

IF 7.4 1区化学

Analytical Chemistry Pub Date : 2025-01-24 DOI: 10.1021/acs.analchem.4c05633

Xinrong Yan, Qingyuan Wang, Peiru Yang, Yuan Liu, Bin Liu, Tian Wang, Dehui Qiu, Shijiong Wei, Desheng Chen, Jun Zhou, Chenghui Liu, Xiaobo Zhang

{"title":"Amplification Bias-Free Sequence-Generic Exponential Amplification Reaction","authors":"Xinrong Yan, Qingyuan Wang, Peiru Yang, Yuan Liu, Bin Liu, Tian Wang, Dehui Qiu, Shijiong Wei, Desheng Chen, Jun Zhou, Chenghui Liu, Xiaobo Zhang","doi":"10.1021/acs.analchem.4c05633","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c05633","url":null,"abstract":"Despite the unique advantage of the isothermal exponential amplification reaction (EXPAR) for the rapid detection of short nucleic acids, it severely suffers from the drawback of sequence-dependent amplification bias, mainly arising from the secondary structures of the EXPAR template under the commonly used reaction temperature (55 °C). As such, the limits of detection (LOD) for different target sequences may vary considerably from aM to nM. Here we report a sequence-generic exponential amplification reaction (SG-EXPAR) that eliminates sequence-dependent amplification bias and achieves similar amplification performance for different targets with generally sub-fM LODs. The assay innovatively employs a thermophilic nicking enzyme that allows SG-EXPAR to work efficiently at higher temperatures (60–70 °C) while eliminating the secondary structures of the templates, which is the basis for eliminating the amplification bias. Furthermore, we increased the probability of trigger/template binding through rational modification of the locked nucleic acids and template optimization, further ensuring the high amplification efficiency for various targets. According to these critical principles, we have developed an automated design platform that allows nonspecialists to obtain the optimal SG-EXPAR template for any desired sequence. The robust performance of the proposed methodology was demonstrated by quantifying microRNA, SARS-CoV-2, monkeypox virus, and HPV B19 at the 1 fM level without sequence screening. SG-EXPAR significantly expands the potential applications of EXPAR and facilitates the development of reliable point-of-care nucleic acid assays.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"6 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-01-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143031169","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

Ultrasensitive Detection of Circulating Plasma Cells Using Surface-Enhanced Raman Spectroscopy and Machine Learning for Multiple Myeloma Monitoring

IF 7.4 1区化学

Analytical Chemistry Pub Date : 2025-01-24 DOI: 10.1021/acs.analchem.4c06244

Dechun Zhang, Xianling Chen, Jia Lin, Shiyan Jiang, Min Fan, Nenrong Liu, Zufang Huang, Jing Wang

{"title":"Ultrasensitive Detection of Circulating Plasma Cells Using Surface-Enhanced Raman Spectroscopy and Machine Learning for Multiple Myeloma Monitoring","authors":"Dechun Zhang, Xianling Chen, Jia Lin, Shiyan Jiang, Min Fan, Nenrong Liu, Zufang Huang, Jing Wang","doi":"10.1021/acs.analchem.4c06244","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c06244","url":null,"abstract":"Multiple myeloma is a hematologic malignancy characterized by the proliferation of abnormal plasma cells in the bone marrow. Despite therapeutic advancements, there remains a critical need for reliable, noninvasive methods to monitor multiple myeloma. Circulating plasma cells (CPCs) in peripheral blood are robust and independent prognostic markers, but their detection is challenging due to their low abundance. Next-generation flow cytometry is commonly used for CPC detection but is not performed in routine clinical practice because it requires expensive instruments, is costly, and time-consuming. This study introduces a cost-effective, rapid surface-enhanced Raman spectroscopy (SERS) assay leveraging gold-deposited magnetic nanoparticles and plasmonic nanoparticles functionalized with anti-CD138 and anti-CD38 antibodies for detecting CPCs in peripheral blood samples. A portable optical device was used for signal recording, enhancing the potential for point-of-care applications. The developed assay is highly sensitive and specific, capable of detecting as few as one or two cells. The application of machine learning algorithms to SERS signal analysis yielded area under the curve values ranging from 0.90 to 0.95, demonstrating excellent performance in differentiating multiple myeloma patients from healthy donors. This SERS method provides a sensitive and accessible way for CPC detection, showing significant potential for multiple myeloma diagnosis, treatment monitoring, and prognosis prediction.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"78 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-01-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143031171","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

A Fast, High-Sensitivity 96-Well Plate-Based MICROFASP Method for Processing Low Microgram Proteomics Sample within 1.5 h

IF 7.4 1区化学

Analytical Chemistry Pub Date : 2025-01-24 DOI: 10.1021/acs.analchem.4c04857

Guojin Ying, Yu He, Mengqing Yang, Gang Lu, Yang Li, Wei Cui, Zhengyan Hu, Zhenbin Zhang

{"title":"A Fast, High-Sensitivity 96-Well Plate-Based MICROFASP Method for Processing Low Microgram Proteomics Sample within 1.5 h","authors":"Guojin Ying, Yu He, Mengqing Yang, Gang Lu, Yang Li, Wei Cui, Zhengyan Hu, Zhenbin Zhang","doi":"10.1021/acs.analchem.4c04857","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c04857","url":null,"abstract":"A rapid, sensitive, and high-throughput sample preparation method is of paramount significance for proteomics analysis. Here, we report a fast, high-sensitivity MICROFASP method that is capable of completing sample preparation within 1.5 h, enhancing the throughput by over 13 times compared to the previous reports. Protein digestion time was significantly cut from 17 h to 20 min in a limited volume. Simultaneous reduction and alkylation occurred within 30 min. The label-free quantitation intensities of proteins from the fast and conventional MICROFASP methods were highly correlated (r = 0.91), validating the reliability of the fast-MICROFASP method. When starting with 1 μg of K562 cell lysate, the fast-MICROFASP method identified over 6 times more protein groups and 19 times more peptides than did the iST method. A 96-well plate-based version was developed to process 8 brain tissue samples from APP/PS1 transgenic mice in parallel. Averagely, with only 1 μg of protein lysate, 2826 protein groups (n = 8, RSD = 0.7%) and 12,972 peptides (n = 8, RSD = 1.5%) were identified from each sample. Amyloid-beta protein was successfully identified as a highly expressed protein, which shows its potential for detecting diagnostic markers and proteome profiling with low-microgram samples. We anticipate the high-sensitivity 96-well plate-based fast-MICROFASP method will have wide application in high-throughput and rapid preparation of large cohorts of low-microgram samples (e.g., clinical biopsy) for comprehensive proteome profiling. Data are available via ProteomeXchange with the identifier PXD053720.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"38 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-01-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143027028","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

Tracing of Amino Acids Dynamics in Cell Lines Based on 18O Stable Isotope Labeling 基于18O稳定同位素标记的细胞系氨基酸动态追踪

IF 7.4 1区化学

Analytical Chemistry Pub Date : 2025-01-23 DOI: 10.1021/acs.analchem.4c05015

Cemil Can Eylem, İpek Baysal, Samiye Yabanoğlu Çiftçi, Emirhan Nemutlu

{"title":"Tracing of Amino Acids Dynamics in Cell Lines Based on 18O Stable Isotope Labeling","authors":"Cemil Can Eylem, İpek Baysal, Samiye Yabanoğlu Çiftçi, Emirhan Nemutlu","doi":"10.1021/acs.analchem.4c05015","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c05015","url":null,"abstract":"Metabolite levels and turnover rates are necessary to understand metabolomic dynamics in a living organism fully. Amino acids can play distinct roles in various cellular processes, and their abnormal levels are associated with pathological conditions, including cancer. Therefore, their levels, especially turnover rates, may provide enormous information about a phenotype. 13C- or 13C,15N-labeled amino acids have also been commonly used to trace amino acid metabolism. This study presented a new methodology based on 18O labeling for amino acids that relied on monitoring mass isotopologues to calculate the turnover rates of amino acids. The method optimization studies were carried over for selective amino acid monitoring. This methodology provides a rapid, robust, and simple GC-MS method for analyzing the fluxes of amino acid metabolism. The developed method was applied to fetal human colon (FHC) and human colon carcinoma (Caco-2) cell lines to determine cancer-induced shifts in the turnover rates of amino acids. These results defined metabolic reprogramming in Caco-2 cells through increased glutamate and serine turnovers and sharply decreased turnovers of aspartate, threonine, and methionine, therefore pointing to some metabolic vulnerabilities in the metabolism of cancerous cells. The simple mechanism of the developed methodology, the availability of affordable 18O-enriched water, and the ease of application can open a new arena in fluxomics analysis.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"74 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-01-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143020165","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

tDDA: A Targeted Data-Dependent Acquisition Mode for Rapid Screening of Targets in Complex Matrices tDDA：复杂矩阵中快速筛选目标的目标数据依赖获取模式

IF 7.4 1区化学

Analytical Chemistry Pub Date : 2025-01-23 DOI: 10.1021/acs.analchem.4c06301

Ang Li, Heyuan Jia, Jie Hong, Shi Zhang, Dayu Li, Wei Xu

{"title":"tDDA: A Targeted Data-Dependent Acquisition Mode for Rapid Screening of Targets in Complex Matrices","authors":"Ang Li, Heyuan Jia, Jie Hong, Shi Zhang, Dayu Li, Wei Xu","doi":"10.1021/acs.analchem.4c06301","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c06301","url":null,"abstract":"Miniaturized mass spectrometers offer significant potential for in situ analysis due to their high specificity and portability. In traditional data-dependent acquisition (DDA) mode, precursor ions for tandem analysis are selected based on the full-scan mass spectrum. However, in situ applications often require the direct analysis of complex samples without extensive sample pretreatment, making them susceptible to chemical noise that can result in false negatives. To address this challenge, we propose a targeted data-dependent acquisition (tDDA) mode that substantially improves the accurate detection of target compounds in complex matrices. Unlike conventional DDA, the tDDA method eliminates reliance on the full-scan mass spectrum, where signals of interest are often obscured by matrix effects. This approach leverages sine amplitude modulation of sinusoidal frequency modulated (SAM-SFM) waveforms technology, which enables the real-time generation of isolated waveforms, allowing tDDA to achieve parallel, high-speed screening. Additionally, targeted automatic gain control (AGC) technology enhances the detection of low-concentration analytes, further reducing the false-negative rate. The tDDA mode was successfully integrated and validated on a modified “Brick” miniaturized ion trap mass spectrometer. Experimental results demonstrated its capability to detect low concentrations of illicit drugs spiked in blood and saliva samples, highlighting its potential for effective in situ screening.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"74 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-01-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143020169","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