Analytical and Bioanalytical Chemistry最新文献_第2页

Glycan mixture analysis by kernel component composition for matrix factorization. 矩阵分解核成分组成的聚糖混合物分析。

IF 3.8 2区化学

Analytical and Bioanalytical Chemistry Pub Date : 2025-04-01 Epub Date: 2025-02-12 DOI: 10.1007/s00216-025-05777-4

Pengyu Hong, Chaoshuang Xia, Yang Tang, Juan Wei, Cheng Lin

{"title":"Glycan mixture analysis by kernel component composition for matrix factorization.","authors":"Pengyu Hong, Chaoshuang Xia, Yang Tang, Juan Wei, Cheng Lin","doi":"10.1007/s00216-025-05777-4","DOIUrl":"10.1007/s00216-025-05777-4","url":null,"abstract":"A major challenge in structural glycomics is the presence of isomeric glycan structures, which may not be fully resolved by separation techniques such as liquid chromatography (LC) and ion mobility spectrometry (IMS). Tandem mass spectrometry (MS/MS) can be employed following on-line separation to distinguish unresolved features, as the temporal profiles of various fragment ions reflect different combinations of those from their respective precursor ions. However, traditional principal component analysis can produce negative signals that are unrealistic for real data, and classic non-negative matrix factorization (NMF) methods may result in factors that include contributions from multiple components. This paper introduces a new variation of NMF, termed kernel component composition (KCC), which enables users to impose domain-specific prior knowledge about the components as parametric kernels. These kernel parameters are then learned directly from the data. We developed a theoretically guaranteed algorithm based on proximal gradient descent to solve the optimization problem posed by KCC and derived detailed parameter update rules when using Gaussian kernels. The effectiveness of the KCC algorithm is demonstrated through simulation tests and its application to deconvoluting chemical datasets, including LC- and IM-MS/MS analysis of isomeric glycan mixtures.","PeriodicalId":462,"journal":{"name":"Analytical and Bioanalytical Chemistry","volume":" ","pages":"1975-1984"},"PeriodicalIF":3.8,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143405004","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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

Cost-effective in-house-made whole blood materials for internal quality control in clinical flow cytometry analysis. 具有成本效益的自制全血材料，用于临床流式细胞术分析的内部质量控制。

IF 3.8 2区化学

Analytical and Bioanalytical Chemistry Pub Date : 2025-04-01 Epub Date: 2025-02-18 DOI: 10.1007/s00216-025-05801-7

Hui-Min Chong, Zhao-Wei Zhang, Jin-Mi Li, Xiao-Dong Ren, Chun-Mei Gong, Zhi-Xian Zhu, Nan Xiang, Zhong-Hua Ni, Qing Huang

{"title":"Cost-effective in-house-made whole blood materials for internal quality control in clinical flow cytometry analysis.","authors":"Hui-Min Chong, Zhao-Wei Zhang, Jin-Mi Li, Xiao-Dong Ren, Chun-Mei Gong, Zhi-Xian Zhu, Nan Xiang, Zhong-Hua Ni, Qing Huang","doi":"10.1007/s00216-025-05801-7","DOIUrl":"10.1007/s00216-025-05801-7","url":null,"abstract":"Internal quality control (IQC) is essential for ensuring the accuracy of results in clinical trials. However, there is a significant shortage of commercial quality control materials for IQC in flow cytometry. This study aimed to develop cost-effective in-house-made whole blood materials from clinically discarded samples to serve as IQC in clinical flow cytometry analysis. Discarded clinical whole blood samples were collected to prepare red blood cell (RBC) suspensions through density centrifugation. White blood cell (WBC) suspensions were prepared using made in-house (MiH) lysing buffer, followed by fixation with the MiH fixative solution. The in-house-made whole blood materials were then prepared by mixing the RBC and WBC suspensions. These mixtures were stored under controlled temperature conditions to ensure long-term stability. These materials are intended for use in internal quality control (IQC) for clinical flow cytometry analysis. The recovery rate of RBC suspensions achieved through density centrifugation was 95%. Different blood type RBC suspensions were effectively preserved in Alsever's solution via plasma washing and re-mixing. The average viability of MiH WBC suspensions was 97%, with a recovery rate of 84%, both significantly higher than those observed with ACK (p < 0.001). Among the in-house-made whole blood material samples, sample a1-which included plasma, Alsever's solution, RBC suspension, WBC suspension, and Proclin 300-exhibited the best stability in flow cytometry, demonstrating stable expression of cell antigens for over 5 months. The in-house-made whole blood materials proved to be cost-effective and suitable for use in IQC for clinical flow cytometry analysis.","PeriodicalId":462,"journal":{"name":"Analytical and Bioanalytical Chemistry","volume":" ","pages":"2121-2132"},"PeriodicalIF":3.8,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143447676","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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

Impact of NH₄⁺ on the catalytic activity of G-quadruplex/hemin DNAzyme for chemiluminescent sensing. NH4+对g -四联体/血红素DNAzyme化学发光传感催化活性的影响。

IF 3.8 2区化学

Analytical and Bioanalytical Chemistry Pub Date : 2025-04-01 DOI: 10.1007/s00216-025-05842-y

Xinyu Zhang, Chenxi Zhu, Yanying Wang, Yi Zhao, Honghu Tang, Xianming Li, Peng Wu

{"title":"Impact of NH4+ on the catalytic activity of G-quadruplex/hemin DNAzyme for chemiluminescent sensing.","authors":"Xinyu Zhang, Chenxi Zhu, Yanying Wang, Yi Zhao, Honghu Tang, Xianming Li, Peng Wu","doi":"10.1007/s00216-025-05842-y","DOIUrl":"https://doi.org/10.1007/s00216-025-05842-y","url":null,"abstract":"G-quadruplex/hemin DNAzyme, a versatile tool for biosensing, is challenged by its low peroxidase-mimic activities. The addition of NH4+ may offer an efficient approach to improve its activity. However, the detailed impact of NH4+ on its catalytic activity remains unclear, confusing the selection of appropriate DNAzymes for biosensing applications. Here, we conducted a comprehensive examination of the influence of NH4+ on G-quadruplex/hemin DNAzyme. The results revealed that all DNAzymes with different G-quadruplex topologies exhibited increased catalytic activities in the presence of NH4+ relative to K+, followed by the subsequent activity order: parallel > hybrid > antiparallel. Further investigations indicated that the increased catalytic activity can be ascribed to the increased stability of the G-quadruplex/hemin complex, elevated reaction velocity, and improved substrate affinity. Leveraging the significant disparity in enzymatic activity between parallel and antiparallel G-quadruplexes, an allosteric sensor based on the Pb2+-induced topological conformation was developed for sensitive detection of Pb2+ in the NH4+-boosted G-quadruplex/hemin DNAzyme system (LOD, 1.56 nM), indicating potential for practical applications. Our discovery improves the understanding of NH4+-boosted G-quadruplex/hemin DNAzyme and may facilitate the development of biosensors.","PeriodicalId":462,"journal":{"name":"Analytical and Bioanalytical Chemistry","volume":" ","pages":""},"PeriodicalIF":3.8,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143750438","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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

Automated QA/QC reporting for non-targeted analysis: a demonstration of "INTERPRET NTA" with de facto water reuse data. 用于非目标分析的自动化QA/QC报告：使用实际水再利用数据的“INTERPRET NTA”演示。

IF 3.8 2区化学

Analytical and Bioanalytical Chemistry Pub Date : 2025-04-01 Epub Date: 2025-02-15 DOI: 10.1007/s00216-025-05771-w

Jon R Sobus, Nickolas A Sayre-Smith, Alex Chao, Troy M Ferland, Jeffrey M Minucci, E Tyler Carr, Laura D Brunelle, Angela L Batt, Heather D Whitehead, Tommy Cathey, Matthew Boyce, Elin M Ulrich, James P McCord, Antony J Williams

{"title":"Automated QA/QC reporting for non-targeted analysis: a demonstration of \"INTERPRET NTA\" with de facto water reuse data.","authors":"Jon R Sobus, Nickolas A Sayre-Smith, Alex Chao, Troy M Ferland, Jeffrey M Minucci, E Tyler Carr, Laura D Brunelle, Angela L Batt, Heather D Whitehead, Tommy Cathey, Matthew Boyce, Elin M Ulrich, James P McCord, Antony J Williams","doi":"10.1007/s00216-025-05771-w","DOIUrl":"10.1007/s00216-025-05771-w","url":null,"abstract":"The US Environmental Protection Agency (EPA) uses non-targeted analysis (NTA) to characterize potential risks associated with environmental pollutants and anthropogenic materials. NTA is used throughout EPA's Office of Research and Development (ORD) to support the needs of states, tribes, EPA regions, EPA program offices, and other outside partners. NTA methods are complex and conducted via myriad instrumental platforms and software products. Comprehensive standards do not yet exist to guide NTA quality assurance/quality control (QA/QC) procedures. Furthermore, no single software tool meets EPA's needs for QA/QC review and documentation. Considering these factors, ORD developed \"INTERPRET NTA\" (Interface for Processing, Reviewing, and Translating NTA data) to support liquid chromatography (LC) high-resolution mass spectrometry (HRMS) NTA experiments. For purposes of NTA QA/QC, INTERPRET NTA (1) calculates data quality statistics related to accuracy, precision, and reproducibility; (2) produces interactive visualizations to facilitate quality threshold optimization; and (3) outputs comprehensive documentation for inclusion in official reports and research publications. INTERPRET NTA has additional functionality to facilitate rapid chemical identification and risk-based prioritization. The current article describes only the QA/QC elements of INTERPRET NTA's MS1 workflow, which are demonstrated using published data from a de facto water reuse study. INTERPRET NTA, in its current form, exists primarily to meet the needs of EPA and its partners, but a public release is planned. Workflows, terminology, and outputs of INTERPRET NTA provide a focal point for necessary discussions on the harmonization of NTA QA/QC practices.","PeriodicalId":462,"journal":{"name":"Analytical and Bioanalytical Chemistry","volume":" ","pages":"1897-1914"},"PeriodicalIF":3.8,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143424698","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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

Examining environmental matrix effects on quantitative non-targeted analysis estimates of per- and polyfluoroalkyl substances. 研究环境基质对全氟烷基和多氟烷基物质定量非目标分析估计的影响。

IF 3.8 2区化学

Analytical and Bioanalytical Chemistry Pub Date : 2025-04-01 Epub Date: 2025-02-27 DOI: 10.1007/s00216-025-05796-1

Shirley Pu, James P McCord, Rebecca A Dickman, Nickolas A Sayresmith, Helen Sepman, Anneli Kruve, Diana S Aga, Jon R Sobus

{"title":"Examining environmental matrix effects on quantitative non-targeted analysis estimates of per- and polyfluoroalkyl substances.","authors":"Shirley Pu, James P McCord, Rebecca A Dickman, Nickolas A Sayresmith, Helen Sepman, Anneli Kruve, Diana S Aga, Jon R Sobus","doi":"10.1007/s00216-025-05796-1","DOIUrl":"10.1007/s00216-025-05796-1","url":null,"abstract":"Non-targeted analysis (NTA) is commonly used for the detection and identification of emerging pollutants, including many per- and polyfluoroalkyl substances (PFAS). While NTA outputs are often non-quantitative, concentration estimation is now possible using quantitative non-targeted analysis (qNTA) approaches. To date, few studies have examined matrix effects on qNTA performance, and little is therefore known about the implications of matrix effects on qNTA results and interpretations. Using a set of 19 PFAS, we examined the impacts of drinking water (DW) and waste-activated sludge matrices on qNTA performance across three qNTA approaches: one structure-independent approach based on \"global\" surrogates and two structure-dependent approaches based on \"expert-selected\" surrogates and predicted ionization efficiency (IE) regression. The performance of each qNTA approach was examined separately for the PFAS prepared in pure solvent, DW extract, and sludge extract using leave-one-out modeling. Performance was evaluated using previously defined qNTA metrics that describe predictive accuracy, uncertainty, and reliability. The studied sample matrices had minimal effects on qNTA accuracy and larger effects on qNTA uncertainty and reliability. Using solvent-based surrogate data to inform matrix-based estimations yielded lower uncertainty, but also lower reliability, emphasizing that uncertainty must be considered in context of reliability. No single qNTA approach uniformly performed best across all comparisons. Since the IE regression and global surrogates approaches proved most reliable, we recommended them for future qNTA applications. This study highlights the importance of examining multiple performance metrics and utilizing matrix-matched surrogate data in qNTA studies.","PeriodicalId":462,"journal":{"name":"Analytical and Bioanalytical Chemistry","volume":" ","pages":"2097-2110"},"PeriodicalIF":3.8,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143514161","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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

Comparative analysis of glycoproteomic software using a tailored glycan database. 糖蛋白组学软件使用定制的聚糖数据库进行比较分析。

IF 3.8 2区化学

Analytical and Bioanalytical Chemistry Pub Date : 2025-04-01 Epub Date: 2025-03-18 DOI: 10.1007/s00216-025-05780-9

Reuben A Hogan, Lauren E Pepi, Nicholas M Riley, Robert J Chalkley

{"title":"Comparative analysis of glycoproteomic software using a tailored glycan database.","authors":"Reuben A Hogan, Lauren E Pepi, Nicholas M Riley, Robert J Chalkley","doi":"10.1007/s00216-025-05780-9","DOIUrl":"10.1007/s00216-025-05780-9","url":null,"abstract":"Glycoproteomics is a rapidly developing field, and data analysis has been stimulated by several technological innovations. As a result, there are many software tools from which to choose; and each comes with unique features that can be difficult to compare. This work presents a head-to-head comparison of five modern analytical software: Byonic, Protein Prospector, MSFraggerGlyco, pGlyco3, and GlycoDecipher. To enable a meaningful comparison, parameter variables were minimized. One potential confounding variable is the glycan database that informs glycoproteomic searches. We performed glycomic profiling of the samples and used the output to construct matched glycan databases for each software. Up to 17,000 glycopeptide spectra were identified across three replicates of wild-type SH-SY5Y cells. There was overlap among all software for glycoproteins identified, locations of glycosites, and glycans; but there was no clear winner. Incorporation of several comparative criteria was critically important for learning the most information in this study and should be used more broadly when assessing software. A single criterion, such as number of glycopeptide spectra found, is not sufficient. We present evidence that suggests Byonic reports many spurious results at the glycoprotein and glycosite level. Overall, our results indicate that glycoproteomic searches should involve more than one software, excluding the current version of Byonic, to generate confidence by consensus. It may be useful to consider software with peptide-first approaches and with glycan-first approaches.","PeriodicalId":462,"journal":{"name":"Analytical and Bioanalytical Chemistry","volume":" ","pages":"1985-2001"},"PeriodicalIF":3.8,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143646737","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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 novel method for semi-quantitative detection of HPV16 and HPV18 mRNA with a low-cost, open-source fluorimeter. 一种低成本开源荧光仪半定量检测HPV16和HPV18 mRNA的新方法。

IF 3.8 2区化学

Analytical and Bioanalytical Chemistry Pub Date : 2025-04-01 Epub Date: 2025-02-07 DOI: 10.1007/s00216-025-05765-8

Kathryn A Kundrod, Mary E Natoli, Chelsey A Smith, Jackson B Coole, Megan M Chang, Emilie Newsham Novak, Elizabeth Chiao, Elizabeth A Stier, Jane R Montealegre, Michael E Scheurer, Philip E Castle, Kathleen M Schmeler, Rebecca R Richards-Kortum

{"title":"A novel method for semi-quantitative detection of HPV16 and HPV18 mRNA with a low-cost, open-source fluorimeter.","authors":"Kathryn A Kundrod, Mary E Natoli, Chelsey A Smith, Jackson B Coole, Megan M Chang, Emilie Newsham Novak, Elizabeth Chiao, Elizabeth A Stier, Jane R Montealegre, Michael E Scheurer, Philip E Castle, Kathleen M Schmeler, Rebecca R Richards-Kortum","doi":"10.1007/s00216-025-05765-8","DOIUrl":"10.1007/s00216-025-05765-8","url":null,"abstract":"Despite global calls to eliminate cervical cancer, rates of cervical cancer incidence and mortality remain high in resource-limited settings, where it is challenging to implement and sustain screening, diagnosis, and treatment programs. The presence of high-risk HPV mRNA in cervical cells is a sensitive and specific biomarker of cervical precancer. Yet, current testing methods are too costly and complex for use in resource-limited settings. Here, we present a novel method for semi-quantitative detection of HPV16 and HPV18 mRNA with minimal infrastructure requirements. The assay relies on isothermal reverse transcription recombinase polymerase amplification (RT-RPA) with real-time fluorescence readout, demonstrated on rugged, portable, and affordable instruments. We demonstrate adapting the assay from DNA detection to RNA detection, characterizing the test with samples of increasing biological complexity, and ultimately establishing a limit of detection of 1000 HPV16 or HPV18 transcripts per reaction with RNA extracted from cell lines. HPV16 and HPV18 mRNA assays were used to test total RNA from 11 patient samples; results for 10 samples (91%) agreed with the gold standard of RT-qPCR. To reduce cost, the assay was demonstrated with multiplexed detection of HPV16 and HPV18 DNA, validated with a reaction volume that was reduced from 50 to 5 µL with DNA and RNA, and performed using a low-cost, portable reader with DNA and RNA. With incorporation of point-of-care-friendly sample preparation and detection of additional genotypes, this test has the potential to expand global access to HPV testing.","PeriodicalId":462,"journal":{"name":"Analytical and Bioanalytical Chemistry","volume":" ","pages":"1765-1778"},"PeriodicalIF":3.8,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11913951/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143370198","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Alkaline persulfate oxidation as an intermediate step for the development of a wet chemical oxidation interface for compound-specific δ¹⁵N analysis by LC-IRMS. 碱性过硫酸盐氧化作为开发湿化学氧化界面的中间步骤，用于LC-IRMS分析化合物特异性δ15N。

IF 3.8 2区化学

Analytical and Bioanalytical Chemistry Pub Date : 2025-04-01 Epub Date: 2025-02-22 DOI: 10.1007/s00216-025-05795-2

Daniel Köster, Tobias Hesse, Felix Niemann, Maik A Jochmann, Torsten C Schmidt

{"title":"Alkaline persulfate oxidation as an intermediate step for the development of a wet chemical oxidation interface for compound-specific δ15N analysis by LC-IRMS.","authors":"Daniel Köster, Tobias Hesse, Felix Niemann, Maik A Jochmann, Torsten C Schmidt","doi":"10.1007/s00216-025-05795-2","DOIUrl":"10.1007/s00216-025-05795-2","url":null,"abstract":"For the measurement of compound-specific isotope ratios by liquid chromatography isotope ratio mass spectrometry (LC-IRMS), complete mineralization of organic compounds to a single species of measurement gas is required so that isotopic fractionation can be minimized and corrected by identical treatment with standards. The established use of peroxydisulfate in an acidic environment has its limitations, especially when it comes to the complete oxidation of nitrogen-containing compounds with aromatic ring systems. Under acidic oxidation conditions, ammonium and nitrate were identified as the main nitrogen containing mineralization products of the oxidation of different model compounds. In contrast to the oxidation in an acidic environment, alkaline peroxydisulfate oxidation leads to nitrate as a final mineralization product. The concept of alkaline oxidation was transferred from large-scale batch experiments to a commercially available oxidation reactor used in LC-IRMS systems. The obtained nitrate recoveries indicate that alkaline oxidation could be a promising step towards the measurement of compound-specific nitrogen isotope ratios by LC-IMRS. In our work, we show that alkaline peroxydisulfate oxidation allows faster and more complete mineralization of nitrogen-containing compounds. For several model compounds, 63 to 100% of the initially present nitrogen was converted to nitrate within a reaction time of 43 s.","PeriodicalId":462,"journal":{"name":"Analytical and Bioanalytical Chemistry","volume":" ","pages":"2085-2096"},"PeriodicalIF":3.8,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11961470/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143476072","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Differentiating between normal and inflammatory blood serum samples using spectrochemical analytical techniques and chemometrics. 使用光谱化学分析技术和化学计量学区分正常和炎症血清样本。

IF 3.8 2区化学

Analytical and Bioanalytical Chemistry Pub Date : 2025-04-01 Epub Date: 2025-03-06 DOI: 10.1007/s00216-025-05802-6

Rania M Abdelazeem, Zienab Abdel-Salam, Mohamed Abdel-Harith

{"title":"Differentiating between normal and inflammatory blood serum samples using spectrochemical analytical techniques and chemometrics.","authors":"Rania M Abdelazeem, Zienab Abdel-Salam, Mohamed Abdel-Harith","doi":"10.1007/s00216-025-05802-6","DOIUrl":"10.1007/s00216-025-05802-6","url":null,"abstract":"Inflammation detection in blood serum samples is commonly performed using clinical analyzers, which are expensive and complex and require specific labels or markers. Spectrochemical analytical techniques, such as laser-induced breakdown spectroscopy (LIBS) and laser-induced fluorescence (LIF), have emerged as alternative methods for qualitative and non-destructive analysis in various fields. This study explores applying LIBS and LIF techniques for label-free discrimination between normal and inflammatory blood serum samples. In the LIBS analysis, the serum samples are deposited on ashless filter paper and exposed to a high-power Nd:YAG laser source to induce plasma emission. The emitted light is dispersed in a spectrometer and an ICCD camera that captures the spectral lines. The LIF technique utilizes a diode-pumped solid-state laser source to excite the blood serum sample placed in a quartz cuvette. The resulting emission spectra are collected and analyzed using a spectrometer equipped with a CCD detector. The obtained spectroscopic data from both techniques is subjected to principal component analysis (PCA) and graph theory for classification and clustering. The PCA classified the two classes with a data variance of 85.4% and 92.8% based on the first two principal components (PCs) for LIBS and LIF spectra. The graph theory clustered the two classes with an accuracy of 76% and 100% based on LIBS and LIF spectra. The statistical methods effectively discriminate between normal and inflammatory serum samples, providing satisfactory results. The proposed spectrochemical methods offer several advantages over traditional clinical analyzers. They are cost-effective and rapid, making them suitable for the fast and reliable identification of serum samples in laboratories. The non-destructive nature of these techniques eliminates the need for specific labels or markers, further streamlining the analysis process.","PeriodicalId":462,"journal":{"name":"Analytical and Bioanalytical Chemistry","volume":" ","pages":"2133-2142"},"PeriodicalIF":3.8,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11961507/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143565569","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Species-specific optimization of oxylipin ionization in LC-MS: a design of experiments approach to improve sensitivity. LC-MS中氧脂质电离的物种特异性优化：一种提高灵敏度的实验方法设计。

IF 3.8 2区化学

Analytical and Bioanalytical Chemistry Pub Date : 2025-04-01 Epub Date: 2025-02-01 DOI: 10.1007/s00216-025-05759-6

Louis Schmidt, Ulrike Garscha

{"title":"Species-specific optimization of oxylipin ionization in LC-MS: a design of experiments approach to improve sensitivity.","authors":"Louis Schmidt, Ulrike Garscha","doi":"10.1007/s00216-025-05759-6","DOIUrl":"10.1007/s00216-025-05759-6","url":null,"abstract":"Oxylipins are diverse bioactive signaling molecules, which occur in very low concentrations in complex matrices, posing challenges in achieving consistent and sensitive analysis. UHPLC-MS/MS is the preferred technique to separate and quantify these molecules, often optimized using a time-consuming trial-and-error approach. In this study, we applied the design of experiments (DoE) approach to systematically investigate the ionization properties of multiple oxylipin species. Fractional factorial and central composite designs were employed to detect relevant instrument parameters and optimize signal intensity in ESI-MS/MS analysis. Response surface modeling revealed distinct ionization and fragmentation behaviors between polar and apolar oxylipins, driven by their responses to interface temperature and collision-induced dissociation (CID) gas pressure. Particularly, prostaglandins and lipoxins benefit from higher CID gas pressure and lower temperatures compared to the lipophilic HODEs and HETEs to achieve optimal intensity in multiple reaction monitoring analysis. While global source parameters were optimized, analyte-specific entrance/exit potentials and collision energies required individual adjustments. The final method was applied to analyze seven oxylipin classes including leukotrienes, prostaglandins, lipoxins, resolvins, HETEs, HODES, and HoTrEs. Although improvements in lower limits of quantification were modest (< 1 pg on-column), signal-to-noise ratios increased two-fold for lipoxins and resolvins and three- to four-fold for leukotrienes and HETEs, enhancing detection at trace levels. This DoE-guided strategy provides a powerful tool to improve UHPLC-MS/MS analysis of oxylipins across various instrument vendors, guiding the way towards inter-laboratory comparability.","PeriodicalId":462,"journal":{"name":"Analytical and Bioanalytical Chemistry","volume":" ","pages":"1807-1818"},"PeriodicalIF":3.8,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11913994/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143073376","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0