Analytica Chimica Acta最新文献

{"title":"Simultaneous radionuclide determination using PSresin: 2in2 and 2in1 tandem configuration","authors":"I. Giménez, H. Bagán, A. Tarancón","doi":"10.1016/j.aca.2024.343573","DOIUrl":"https://doi.org/10.1016/j.aca.2024.343573","url":null,"abstract":"<h3>Background</h3>Analyzing mixtures of radionuclides is a complex task. Two situations are the mixtures of ⁸⁹Sr with ⁹⁰Sr and ⁹⁰Sr with plutonium isotopes. The challenge arises in emergency scenarios resulting from accidents where the activity of ⁸⁹Sr is over 20 times higher than that of ⁹⁰Sr, complicating its quantification and requiring delayed measurements. In scenarios involving accidents, both ⁹⁰Sr and plutonium isotopes, may be present within various matrices. Given their distinct elemental properties, separation is typically achieved using different methods, followed by a measurement post-elution through alpha spectrometry and scintillation techniques. Therefore, methods which allow the fast and reliable determination of those mixtures are still required in routine laboratories.<h3>Results</h3>A novel method for the simultaneous determination of radionuclide mixtures using PSresin is introduced. This innovative approach utilizes PSresins in tandem and has been applied to the analysis of ⁸⁹Sr and ⁹⁰Sr, as well as mixtures of ⁹⁰Sr and plutonium isotopes. Two strategies were investigated: using two PSresin in two cartridges and two measurements (2in2); and using two PSresin in a single cartridge and one measurement employing α/β discrimination (2in1). The methods were validated with standard solutions and applied to river water samples, achieving quantification errors below 10% for both strategies within 5 and 8 h, respectively, from sample reception.<h3>Significance</h3>This represents a great improvement for ⁸⁹Sr and ⁹⁰Sr quantification which is achieved in less than 5 h since sample reception reducing the 30 days required by conventional methods. Additionally, the simultaneous measurement of ⁹⁰Sr and plutonium isotopes reduce the number of required analysis to half. Reducing the overall time and cost of the analysis.","PeriodicalId":240,"journal":{"name":"Analytica Chimica Acta","volume":"82 1","pages":""},"PeriodicalIF":6.2,"publicationDate":"2024-12-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142857954","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}

{"title":"Preparation, mechanism, and biological applications of targeting LDs ratiometric fluorescent probes for HClO detection","authors":"Weiling Yan, Ying Liu, Yuhang Wang, Shizeng Pei, Caihong Zhang, Guomei Zhang, Shaomin Shuang, Chuan Dong","doi":"10.1016/j.aca.2024.343570","DOIUrl":"https://doi.org/10.1016/j.aca.2024.343570","url":null,"abstract":"Hypochlorous acid (HClO) is a well-known inflammatory signaling molecule, while lipid droplets (LDs) are dynamic organelles closely related to inflammation. Using organic small-molecule fluorescence imaging technology to target LDs for precise monitoring of HClO is one of the most effective methods for diagnosing inflammation-related diseases. A thorough investigation of how probes detect biological markers and the influencing factors can aid in the design of probe molecules, the selection of high-performance tools, and the accuracy of disease detection. To this end, three fluorescent probes (TPA-B, TPA-BF and TPA-SF) based on triphenylamine (TPA) containing C=N double bonds as potential reaction sites were prepared by condensing triphenylamine thiophene aldehyde (TPA-CHO) with a series of aromatic hydrazides (ArCONHNH₂). Their performance in ratiometric detecting HClO by targeting LDs had been systematically studied. The results showed that the Ar- structure in ArCONHNH₂ can not only effectively regulate the sensing performance to HClO, but also led to different oxidation products. The key reason for this was the electron cloud density around the C=N bond. Furthermore, the selected probe TPA-B, which demonstrated the best spectral performance, was proficiently utilized for the detection of HClO in cells and zebrafish, as well as the detection of HClO in inflammatory diseases. This study compared the oxidation products of C=N bonds by HClO and analyzed the key influencing factors. By integrating spectroscopic and imaging experiments, high-performance diagnostic agents (TPA-B) for inflammation were identified. The approach provided valuable insights into the design of multifunctional probes and opened new pathways for the diagnosis of inflammation-related diseases.","PeriodicalId":240,"journal":{"name":"Analytica Chimica Acta","volume":"28 1","pages":""},"PeriodicalIF":6.2,"publicationDate":"2024-12-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142848945","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}

{"title":"A Sensitive Post-Column Derivatization Approach for Enhancing Hydroxyl Metabolites Detection","authors":"Yen-Chu Lin, Shiu-Wen Huang, San-Yuan Wang, Jing-Rong Su, Jimmy Junxiang Wang, Ming-Jen Hsu, Hsiao-Wei Liao","doi":"10.1016/j.aca.2024.343559","DOIUrl":"https://doi.org/10.1016/j.aca.2024.343559","url":null,"abstract":"<h3>Background</h3>Chemical derivatization is a common technique in liquid chromatography-mass spectrometry (LC-MS) metabolomics used to improve the ionizability and chromatographic properties of metabolites in complex biological samples. This process facilitates better detection and separation of a wide array of compounds. The reagent 2-(4-boronobenzyl) isoquinolin-2-ium bromide (BBII), developed as a glucose labeling reagent for matrix-assisted laser desorption/ionization MS, enhances ionization for glucose and other hydroxyl metabolites. Its quaternary ammonium group increases ionization efficiency, and its rapid reaction time simplifies pretreatment procedures.<h3>Results</h3>We developed a novel post-column derivatization (PCD) method using BBII to boost the detection sensitivity of hydroxyl metabolites in LC-MS. By optimizing this BBII PCD approach with 14 hydroxyl-containing compounds, we were able to detect previously undetectable metabolites such as glucose, ribose, and long-chain alcohols. Sensitivity enhancements for these metabolites ranged from 1.1 to 42.9-fold. Applying this method to metabolic profiling of hydroxyl metabolites in the DBTRG-05MG glioblastoma cell line, with and without treatment with the new drug MFB [1-(4-chlorobenzyl)-2-(5-methyl-2-furfurylideneamino)benzimidazole], revealed several hydroxyl metabolites with significantly reduced levels post-treatment.<h3>Significance and Novelty</h3>This study presents a new BBII PCD method that substantially improves the detection sensitivity of hydroxyl metabolites in LC-MS. This innovative approach is highly valuable for untargeted metabolomics studies in biological and clinical research, offering a robust tool for identifying metabolite changes and advancing our understanding of metabolic processes in disease and therapeutic contexts.","PeriodicalId":240,"journal":{"name":"Analytica Chimica Acta","volume":"18 1","pages":""},"PeriodicalIF":6.2,"publicationDate":"2024-12-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142840829","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}

{"title":"Enhancing the Interactions of Ion-Tagged Oligonucleotides and Magnetic Ionic Liquid Supports for the Sequence-Specific Extraction of Hepatitis B Virus DNA","authors":"Seong-Soo Lee, Derek R. Eitzmann, Jared L. Anderson","doi":"10.1016/j.aca.2024.343563","DOIUrl":"https://doi.org/10.1016/j.aca.2024.343563","url":null,"abstract":"<h3>Background</h3>Infections from the hepatitis B virus (HBV) are a major risk factor for hepatocellular carcinoma, one of the most common types of liver cancer. Circulating cell-free DNA (ccfDNA) in human plasma can be used as a non-invasive biomarker for diagnosing HBV-related liver diseases. The isolation of target ccfDNA sequences is often challenging due to the co-extraction of highly abundant non-target DNA from samples. Ion-tagged oligonucleotide (ITO) probes coupled with magnetic ionic liquids (MIL) support have emerged as a promising methodology for sequence-specific DNA extractions to address challenges associated with solid supports such as streptavidin-coated magnetic bead.<h3>Results</h3>ITOs, disubstituted ion-tagged oligonucleotide (DTO), and ion-tagged disubstituted oligonucleotide (ITDO) probes featuring various substituents including linear alkyl, branched alkyl, and perfluoroalkyl moieties were examined to enhance hydrophobic and fluorophilic interactions between the probes and a trihexyl(tetradecyl)phosphonium manganese(II) hexafluoroacetylacetonate ([P₆₆₆₁₄⁺][Mn(hfacac)₃⁻]) MIL support. The ITO-MIL approach was optimized by adjusting the annealing temperature (45 °C), molar ratio of target DNA to ITO probe (1:100), and ionic strength (200 mM NaCl) to maximize the extraction of target DNA. The 3-allyl-1-(23-bis(pentylthio)propyl)imidazolium bromide ([AI(C₅S)₂⁺][Br^-])-ITO probe featuring a branched alkyl substituent yielded a higher loading efficiency (48.05 ± 6.72%) due to increased hydrophobic ITO-MIL interactions, compared to that of 24.57 ± 4.40% for the 3-allyl-1-(3-(pentylthio)propyl)imidazolium bromide ([AIC₅S⁺][Br^-])-ITO probe with a linear alkyl substituent. The high affinity of ITO-MILinteractions minimized the loss of probe during successive wash steps, yielding an approximate 10-fold greater amount of extracted target DNA using the [AI(C₅S)₂⁺][Br^-])-ITO probe compared to [AIC₅S⁺][Br^-])-ITO probe.<h3>Significance</h3>This study provides novel synthetic approaches for tailoring probe substituents using thiol-ene and thiol-yne “click” chemistry. Hydrophobic and fluorophilic ITO-MIL interactions were systematically investigated. Optimal conditions for the ITO-MIL method significantly improved the amount of extracted DNA. The ITO-MIL method using the [AI(C₅S)₂⁺][Br^-]-HBV-ITO probe demonstrated selective extraction of target HBV DNA in both DI water and diluted human plasma containing a high abundance of background DNA.","PeriodicalId":240,"journal":{"name":"Analytica Chimica Acta","volume":"106 1","pages":""},"PeriodicalIF":6.2,"publicationDate":"2024-12-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142848947","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}

{"title":"Stylus Pen-based Ambient Ionization Mass Spectrometry for the Analysis of Volatiles and Semivolatiles from Liquid, Viscous, and Solid Samples","authors":"Yi-Ying Wu, Chin-Pao Chiu, Yu-Chie Chen","doi":"10.1016/j.aca.2024.343560","DOIUrl":"https://doi.org/10.1016/j.aca.2024.343560","url":null,"abstract":"<h3>Background</h3>Ambient ionization mass spectrometry (MS) has attracted significant attention due to its simplicity and ease of operation. Contactless, or field-induced, ionization is one of the ambient ionization techniques. In this approach, no direct electrical contact or additional voltage is required on the ionization-assisted substrate. Instead, the electric field is induced by the high voltage applied to the orifice of the mass spectrometer. However, there remains a demand for exploring compact and readily available ionization substrates for use in field-induced ionization techniques. <u>Results</u>: A stylus pen, typically used for touch screens, is used as an ion source for analyzing volatile and semivolatile organic compounds. Vapors originating from volatile and semivolatile compounds placed underneath the inlet of the mass spectrometer were ionized when the stylus pen was positioned near the inlet, which is applied with a high voltage. The limits of detection for semivolatiles and volatiles were in the range of mM to a few hundred nM, depending on the vapor pressure and chemical structures of these analytes. Additionally, semivolatile compounds found in real samples could be directly detected using our method. Moreover, we also demonstrated the feasibility of using the stylus pen as the sampling probe to pick up samples from the surface of a glass slide, followed by bringing the pen close to the inlet of the mass spectrometer for direct MS analysis using our approach. <u>Significance</u>: The developed method provides a straightforward approach for analyzing volatiles and semi-volatiles under ambient conditions. Ionization of the analyte vapor near the mass spectrometer inlet can readily occur by placing a stylus pen close to the inlet, highlighting simplicity as the main advantage of the developed method. Consequently, this method can be easily coupled with a mass spectrometer that has a high voltage applied to its orifice.","PeriodicalId":240,"journal":{"name":"Analytica Chimica Acta","volume":"79 1","pages":""},"PeriodicalIF":6.2,"publicationDate":"2024-12-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142848946","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}

{"title":"Amidine-functionalized aggregation-induced emission luminogen and a 3D-printed digital sensor platform for ultrafast and visual detection of heparin","authors":"Feilong Tang, Siyu Shi, Chiyuan Wei, Yuanqiang Sun, Ran Yang, Lingbo Qu, Zhaohui Li","doi":"10.1016/j.aca.2024.343564","DOIUrl":"https://doi.org/10.1016/j.aca.2024.343564","url":null,"abstract":"<h3>Background</h3>Heparin is a widely used anticoagulant in clinic. However, improper dosing can increase the risk of thromboembolic events, potentially leading to life-threatening complications. Clinic monitoring of heparin is very important for its use safety. Rapid and accurate point-of-care testing can significantly reduce the risk of thrombotic events. The detection of heparin using fluorescent probes has emerged as a significant area of research, driven by the need for rapid, sensitive, and selective methods for monitoring this crucial anticoagulant in clinical settings. However, the absence of convenient and user-friendly heparin testing methods continues to pose a challenge.<h3>Results</h3>In this work, a tetraphenylethylene derivatives with four amidine active groups (TPE-4⁺) was prepared. TPE-4⁺ has obvious aggregation-induced emission (AIE) effect on the heparin with a 127-fold enhancement occurring within just 3 seconds. The molecular docking simulation showed that TPE-4⁺ was closely embedded in the heparin by the electrostatic force between four amidine of TPE-4⁺ and sulfate ester group of heparin, restricted intramolecular motion of TPE-4⁺, and causing obvious AIE features. The fluorescence intensity of TPE-4⁺ was line with the concentration of heparin in the range of 0–2.0 U/mL with a lowest detection limit of 0.0038 U/mL. The possible interference in the serum samples had no influence on the determination of heparin. Using 3D printing technology, a compact, portable digital sensor platform for straightforward monitoring of heparin levels was fabricated.<h3>Significance</h3>The proposed innovative platform provides a powerful tool to make portable and real-time monitoring of heparin possible, and thereby contributing to achieve point-of-care testing and decrease the risk of thrombotic events. This novel method of combining the probe with the sensing platform simplifies the detection process and enhances patient care by providing more accurate diagnostic capabilities.","PeriodicalId":240,"journal":{"name":"Analytica Chimica Acta","volume":"144 1","pages":""},"PeriodicalIF":6.2,"publicationDate":"2024-12-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142840831","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}

{"title":"Ligand engineering boosts catalase-like activity of gold nanoclusters for cascade reactions combined with glucose oxidase in ZIF-8 matrix","authors":"Yi-Shu Wang, Chen Dong, Li Zou, Lin Zhao, Jian-Hua Qin, Hui-Lin Mo","doi":"10.1016/j.aca.2024.343565","DOIUrl":"https://doi.org/10.1016/j.aca.2024.343565","url":null,"abstract":"<h3>Background</h3>Integrating natural enzymes and nanomaterials exhibiting tailored enzyme-like activities is an effective strategy for the application of cascade reactions. It is essential to develop a highly efficient and robust glucose oxidase-catalase (GOx-CAT) cascade system featuring controllable enzyme activity, a reliable supply of oxygen, and improved stability for glucose depletion in cancer starvation therapy. However, the ambiguous relationship between structure and performance, and the difficulty in controlling enzyme-mimic activity, significantly hinder their broader application. Herein, the CAT-like activity of atomically precise Au₂₅(MPA)₁₈ (MPA = 3-mercaptopropionic acid) nanoclusters (AuNCs) was modulated by incorporating N-acetyl-L-cysteine (NAC) in a series of ratio.<h3>Results</h3>It is found that Au₂₅(NAC)_14-17(MPA)_4-1 exhibited superior CAT-like activity and structural stability than Au₂₅(MPA)₁₈ owing to the intramolecular hydrogen bond in NAC. Moreover, the synergetic effects of glucose-depletion catalyzed by GOx, oxygen generation from the intermediate hydrogen peroxide (H₂O₂) facilitated by Au₂₅(NAC)_14-17(MPA)_4-1, and protective function and nanoconfinement effect of zeolitic imidazolate framework-8 (ZIF-8) enabled the GOx-Au₂₅(NAC)_14-17(MPA)_4-1@ZIF-8 composite to degrade more glucose. Compared to that treated with a single enzyme or free enzymes, the residual intermediate H₂O₂ level after treatment with GOx-Au₂₅(NAC)_14-17(MPA)_4-1@ZIF-8 was about 93% lower than that after treatment with GOx alone. This composite showed higher catalytic activity, stability, and tolerance when applied to GOx-mediated glucose depletion.<h3>Significance</h3>In brief, the study provides a feasible strategy for realizing robust and efficient cascade reaction by integrating the merits of natural enzymes and atomically precise metal NCs with adjustable enzyme-like activity. This research offers essential guidance for developing a biocompatible and tailored cascade system.","PeriodicalId":240,"journal":{"name":"Analytica Chimica Acta","volume":"23 1","pages":""},"PeriodicalIF":6.2,"publicationDate":"2024-12-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142848948","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}

{"title":"Lysosome-targeted dual-locked NIR fluorescent probe for visualization of H2S and viscosity in drug-induced liver injury and tumor models","authors":"Jingcan Qin, Fei Kong, Jie Huang, Bang Xiao, Yun Bian, Chengwei Shao","doi":"10.1016/j.aca.2024.343558","DOIUrl":"https://doi.org/10.1016/j.aca.2024.343558","url":null,"abstract":"<h3>Background</h3>Lysosomes, as an indispensable subcellular organelle have numerous physiological functions closely associated with H₂S and viscosity, and accurate assessment of H₂S/viscosity fluctuations in lysosomes is essential for gaining a comprehensive understanding of lysosome-related physiological activities and pathological processes. The previous single-response fluorescent probes for either H₂S or viscosity alone have the potential to generate \"false positive\" signals in a complex biological environment. In contrast, dual-locked probes can simultaneously respond to multiple targets simultaneously, which could effectively eliminate this defect. Therefore, it is essential to constructed a lysosome-targeted dual-locked NIR fluorescent probe for imaging H₂S and viscosity.<h3>Results</h3>In this study, we developed a lysosome-targeted dual-locked NIR fluorescent probe (LFP-N₃) for imaging H₂S and viscosity based on an integrated ICT-TICT process. In the presence of both H₂S and high viscosity conditions, the azide moiety of LFP-N₃ reacts with H₂S, resulting in the formation of LFP-NH₂ that facilitates the ICT process; high viscosity condition further restricts the chemical bond rotation of LFP-NH₂, which suppresses the TICT process. As a result, the fluorescence signal of LFP-N₃ is significantly enhanced at 690 nm with a large Stokes shift (190 nm). Cytotoxicity assay and colocalization experiments in living cells indicated LFP-N₃ possessed low cytotoxicity and precise lysosome-targeted capability. Moreover, both in vitro and in vivo experiments further validated that the fluorescence signal of LFP-N₃ can be triggered by the presence of both H₂S and high viscosity in tumor and drug-induced liver injury models.<h3>Significance</h3>The lysosome-targeted dual-locked NIR fluorescent probe has been successfully utilized to imaging H₂S and viscosity in vitro and in vivo. Compared with the single-response fluorescent probes, the dual-locked NIR probe (LFP-N₃) could effectively mitigate false-positive signals and increase spatial resolution, and has great potential to be developed as a novel diagnostic agent for lysosome-related diseases.","PeriodicalId":240,"journal":{"name":"Analytica Chimica Acta","volume":"19 1","pages":""},"PeriodicalIF":6.2,"publicationDate":"2024-12-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142840865","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}

{"title":"Composition-dependent MRM transitions and structure-indicative elution segments (CMTSES)-based LC-MS strategy for disaccharide profiling and isomer differentiation","authors":"Wen Miao, Na Li, Jia-Qian Chen, Jian-Lin Wu","doi":"10.1016/j.aca.2024.343562","DOIUrl":"https://doi.org/10.1016/j.aca.2024.343562","url":null,"abstract":"<h3>Background</h3>Carbohydrates exhibit diverse functions and extensive biological activities and are notable in the field of life sciences. However, their inherent diversity and complexity—steaming from variations in isomeric monomers, glycosidic bonds, configurations, etc.—present considerable challenges in structural analysis. Considering these challenges, the disaccharide building blocks with simpler structures could provide more structural information. Although various approaches have been explored, sufficient standards or specialized equipment are required to differentiate and characterize isomers. Therefore, a strategy that addresses these challenges is urgently needed.<h3>Results</h3>A <strong>C</strong>omposition-dependent <strong>M</strong>RM <strong>T</strong>ransitions and <strong>S</strong>tructure-indicative <strong>E</strong>lution <strong>S</strong>egments (CMTSES)-based liquid chromatography-triple quadrupole mass spectrometry (LC-QQQ-MS) strategy was developed to comprehensively profile disaccharide units and differentiate isomers. First, the composition-related precursor and structure-specific product ions of disaccharides were generated by QQQ-MS. Thereout, MRM transitions were proposed to enable the comprehensive profiling of disaccharides and rapid annotation of their compositions and saccharide types at both termini. Next, the linkage, composition, and configuration isomers of disaccharides were effectively differentiated and presented characteristic LC elution. Furthermore, low-cost and available “location references” (mannose, galactose, and isomaltose) were sought to define structure-indicative elution segments for the identification of isomeric hexose disaccharides. Building on this foundation, the novel CMTSES-based LC-MS strategy was designed, and its feasibility was further verified by successfully differentiating and identifying mixed homogenous and/or heterogenous disaccharide isomers in real samples. Sufficient structural information was obtained even for those consisting of diversified monomer types.<h3>Significance and Novelty</h3>This strategy comprehensively profiles both major and minor disaccharides and effectively differentiates multiple types of isomers. The use of readily available “location references” facilitated the identification of isomeric hexose disaccharide with reduced dependence on standards, thereby broadening the applicability of this strategy. However, the characterization of disaccharides with other compositions is challenging. Further in-depth investigations into intramolecular hydrogen bond simulation should provide solutions. Additionally, CMTSES-based LC-MS strategy is promising to analyze complex structures and samples.","PeriodicalId":240,"journal":{"name":"Analytica Chimica Acta","volume":"1 1","pages":""},"PeriodicalIF":6.2,"publicationDate":"2024-12-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142840861","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}

{"title":"Highly Parallel Simulation Tool for the Design of Isotachophoresis Experiments","authors":"Alexandre S. Avaro, Adar Schwarzbach, Amit Jangra, Supreet S. Bahga, Juan G. Santiago","doi":"10.1016/j.aca.2024.343553","DOIUrl":"https://doi.org/10.1016/j.aca.2024.343553","url":null,"abstract":"<h3>Background</h3>Isotachophoresis (ITP) is a well-established electrokinetic method for separation and preconcentration of analytes. Several simulation tools for ITP have been published, but their use for experimental design is limited by the computational time for a single run and/or by the number of conditions that can be investigated per simulation run. A large fraction of the existing solvers also do not account for ionic strength effects, which can influence whether an analyte focuses in ITP. There is currently no publicly available tool for the easy and rapid design of ITP experiments.<h3>Results</h3>We present a rapid, highly parallelized steady-state solver for the design of buffer electrolytes in ITP experiments. The tool is called <u>B</u>rowser-based <u>E</u>lectrolyte <u>An</u>alyses for ITP (BEAN). BEAN is designed to facilitate the evaluation and identification of functional buffer chemistries for ITP. Given a user-defined chemistry system, BEAN solves a set of coupled, non-linear integral conservation equations to determine whether a specific analyte is focused by the ITP system, and estimates quantities of interest in the design of related ITP processes. These quantities include zone concentrations, pH, and effective (observable) mobility values. BEAN also computes 972 variations of the specified ITP chemistry, including a broad range of buffer titrations and ion mobilities. All the calculations performed in BEAN include ionic strength and finite ionic radius effects, and the solver handles species with arbitrary valence. The tool further includes a searchable database of 521 commonly used electrolytes. BEAN is available at <span><span>microfluidics.stanford.edu/bean</span><svg aria-label=\"Opens in new window\" focusable=\"false\" height=\"20\" viewbox=\"0 0 8 8\"><path d=\"M1.12949 2.1072V1H7V6.85795H5.89111V2.90281L0.784057 8L0 7.21635L5.11902 2.1072H1.12949Z\"></path></svg></span>.<h3>Significance</h3>This study introduces a novel tool that integrates known ITP steady-state equations with a highly parallel computational framework, an electrolyte database, and a web-based interface. BEAN requires no license nor compilation, and its parallel computations are performed automatically without specific implementation needed from the user. This enables users to screen wide ranges of experimental conditions in the design of ITP experiments.","PeriodicalId":240,"journal":{"name":"Analytica Chimica Acta","volume":"50 1","pages":""},"PeriodicalIF":6.2,"publicationDate":"2024-12-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142840868","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}