Analytica Chimica Acta最新文献

{"title":"Post-synthesis surface modification of Cu/Zr metal azolate framework: A pathway to highly sensitive electrochemical biosensors for atrazine detection","authors":"Bhavna Hedau, Tae-Jun Ha","doi":"10.1016/j.aca.2024.343547","DOIUrl":"https://doi.org/10.1016/j.aca.2024.343547","url":null,"abstract":"<h3>Background</h3>Atrazine (ATZ), a pesticide that poses serious health problems, is observed in the environment, thereby prompting its periodic monitoring and control using functional biosensors. However, established methods for ATZ detection have limited applicability. Two-dimensional (2D) metal azolate frameworks (MAF) have a higher surface area per unit volume and provide easier access to active sites. The shorter diffusion path for guest molecules increases the diffusion rates, which is suitable for electrochemical detection. The sensing performance of electrochemical biosensors can be improved by modifying MAFs, resulting in their high affinity for highly sensitive and selective detection of ATZ in the environment.<h3>Results</h3>Cu/Zr-based MAF synthesized via a simple sonochemical method and surface-engineered ozonation are demonstrated for the electrochemical sensing of ATZ. The combination of ultrasonication and ultraviolet/ozone surface functionalization significantly enhance the properties of a two-dimensional MAF, including a reduction in resistance, an increase in specific surface area, and the creation of numerous active sites. The developed electrochemical biosensors exhibit a high sensitivity (8.8 μA μM^-1 cm^-2), low detection limit of 0.236 zM, and wide linear range of 1 zM to 1 M towards ATZ. Furthermore, excellent selectivity in the presence of diverse interferents and a long shelf life in ambient air for 60 d are achieved. The practical feasibility of the biosensor consisting of surface-engineered Cu/Zr-MAF is demonstrated by detecting the ATZ in agricultural wastewater and river water.<h3>Significance and Novelty</h3>Cu and Zr transition metals with multiple valence states in MAF facilitate the reduction of ATZ through coordination bonding, while the increased oxygenating active sites in 2D structure collectively accelerates the charge transfer. This synergy between the structural design and surface engineering ultimately improves the biosensor's sensitivity and efficiency for the detection of ATZ. This work can provide a new perspective on practical biosensor applications for the electrochemical detection of pesticides at extremely low concentrations.","PeriodicalId":240,"journal":{"name":"Analytica Chimica Acta","volume":"2 1","pages":""},"PeriodicalIF":6.2,"publicationDate":"2024-12-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142816222","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":"Flow electrolytic separation of radionuclides for interference suppression in γ-spectrometry","authors":"Paul Dutheil, Martin Heule, Fabian Köhler, Sandra Baur, Alexander Vögele, Patrick Steinegger","doi":"10.1016/j.aca.2024.343527","DOIUrl":"https://doi.org/10.1016/j.aca.2024.343527","url":null,"abstract":"&lt;h3&gt;Background:&lt;/h3&gt;The direct and accurate measurement of low-level &lt;span&gt;&lt;span style=\"\"&gt;&lt;/span&gt;&lt;span data-mathml='&lt;math xmlns=\"http://www.w3.org/1998/Math/MathML\"&gt;&lt;mi is=\"true\"&gt;&amp;#x3B3;&lt;/mi&gt;&lt;/math&gt;' role=\"presentation\" style=\"font-size: 90%; display: inline-block; position: relative;\" tabindex=\"0\"&gt;&lt;svg aria-hidden=\"true\" focusable=\"false\" height=\"1.855ex\" role=\"img\" style=\"vertical-align: -0.697ex;\" viewbox=\"0 -498.8 543.5 798.9\" width=\"1.262ex\" xmlns:xlink=\"http://www.w3.org/1999/xlink\"&gt;&lt;g fill=\"currentColor\" stroke=\"currentColor\" stroke-width=\"0\" transform=\"matrix(1 0 0 -1 0 0)\"&gt;&lt;g is=\"true\"&gt;&lt;use xlink:href=\"#MJMATHI-3B3\"&gt;&lt;/use&gt;&lt;/g&gt;&lt;/g&gt;&lt;/svg&gt;&lt;span role=\"presentation\"&gt;&lt;math xmlns=\"http://www.w3.org/1998/Math/MathML\"&gt;&lt;mi is=\"true\"&gt;γ&lt;/mi&gt;&lt;/math&gt;&lt;/span&gt;&lt;/span&gt;&lt;script type=\"math/mml\"&gt;&lt;math&gt;&lt;mi is=\"true\"&gt;γ&lt;/mi&gt;&lt;/math&gt;&lt;/script&gt;&lt;/span&gt;-emitters in samples from nuclear facilities is a challenging task due to the presence of high activities of dominant radionuclides. In this case a complex chemical separation is required to remove interfering radionuclides prior to &lt;span&gt;&lt;span style=\"\"&gt;&lt;/span&gt;&lt;span data-mathml='&lt;math xmlns=\"http://www.w3.org/1998/Math/MathML\"&gt;&lt;mi is=\"true\"&gt;&amp;#x3B3;&lt;/mi&gt;&lt;/math&gt;' role=\"presentation\" style=\"font-size: 90%; display: inline-block; position: relative;\" tabindex=\"0\"&gt;&lt;svg aria-hidden=\"true\" focusable=\"false\" height=\"1.855ex\" role=\"img\" style=\"vertical-align: -0.697ex;\" viewbox=\"0 -498.8 543.5 798.9\" width=\"1.262ex\" xmlns:xlink=\"http://www.w3.org/1999/xlink\"&gt;&lt;g fill=\"currentColor\" stroke=\"currentColor\" stroke-width=\"0\" transform=\"matrix(1 0 0 -1 0 0)\"&gt;&lt;g is=\"true\"&gt;&lt;use xlink:href=\"#MJMATHI-3B3\"&gt;&lt;/use&gt;&lt;/g&gt;&lt;/g&gt;&lt;/svg&gt;&lt;span role=\"presentation\"&gt;&lt;math xmlns=\"http://www.w3.org/1998/Math/MathML\"&gt;&lt;mi is=\"true\"&gt;γ&lt;/mi&gt;&lt;/math&gt;&lt;/span&gt;&lt;/span&gt;&lt;script type=\"math/mml\"&gt;&lt;math&gt;&lt;mi is=\"true\"&gt;γ&lt;/mi&gt;&lt;/math&gt;&lt;/script&gt;&lt;/span&gt;-spectrometric analysis. Several radionuclides such as, &lt;sup&gt;110m&lt;/sup&gt;Ag, &lt;sup&gt;124,125&lt;/sup&gt;Sb, &lt;sup&gt;113&lt;/sup&gt;Sn and &lt;sup&gt;123m&lt;/sup&gt;Te are of relevance for radioanalytical analysis in nuclear facilities. These may be readily electrodeposited at controlled-potential using flow electrolysis in aqueous solution. Here, the development and use of flow electrolysis for the pre-analytical separation of different radionuclides to suppress interferences in &lt;span&gt;&lt;span style=\"\"&gt;&lt;/span&gt;&lt;span data-mathml='&lt;math xmlns=\"http://www.w3.org/1998/Math/MathML\"&gt;&lt;mi is=\"true\"&gt;&amp;#x3B3;&lt;/mi&gt;&lt;/math&gt;' role=\"presentation\" style=\"font-size: 90%; display: inline-block; position: relative;\" tabindex=\"0\"&gt;&lt;svg aria-hidden=\"true\" focusable=\"false\" height=\"1.855ex\" role=\"img\" style=\"vertical-align: -0.697ex;\" viewbox=\"0 -498.8 543.5 798.9\" width=\"1.262ex\" xmlns:xlink=\"http://www.w3.org/1999/xlink\"&gt;&lt;g fill=\"currentColor\" stroke=\"currentColor\" stroke-width=\"0\" transform=\"matrix(1 0 0 -1 0 0)\"&gt;&lt;g is=\"true\"&gt;&lt;use xlink:href=\"#MJMATHI-3B3\"&gt;&lt;/use&gt;&lt;/g&gt;&lt;/g&gt;&lt;/svg&gt;&lt;span role=\"presentation\"&gt;&lt;math","PeriodicalId":240,"journal":{"name":"Analytica Chimica Acta","volume":"233 1","pages":""},"PeriodicalIF":6.2,"publicationDate":"2024-12-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142816223","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":"Visible light-responsive enrofloxacin PEC aptasensor based on CN QDs sensitized Bi4O5Br2 nanosheets","authors":"Lijun Ding, Yuan Wang, Lianxi Pu, Tianshuo Wang, Yuanhao Liu, Xilong Zhou, Kun Wang","doi":"10.1016/j.aca.2024.343545","DOIUrl":"https://doi.org/10.1016/j.aca.2024.343545","url":null,"abstract":"<h3>Background</h3>The excessive application of enrofloxacin (ENR) results in residues contaminating both food and the environment. Consequently, developing robust analytical methods for the selective detection of ENR is crucial. The photoelectrochemical (PEC) sensor has emerged as a highly sensitive analytical technique that has seen rapid development in recent years. The functioning of a PEC sensor relies on the reducing capacity of photogenerated electrons and the oxidizing capacity of photogenerated holes produced by the photoactive material. Bi₄O₅Br₂ demonstrates its potential in electrochemical detection, but faces inherent challenges, including swift electron-hole recombination and slow carrier migration, which hinder its catalytic activity.<h3>Results</h3>In this study, we synthesized carbon nitride quantum dots doped with Bi₄O₅Br₂ (CN QDs/ Bi₄O₅Br₂) through an in situ growth method, utilizing this composite as a photoactive material. The incorporation of CN QDs leads to a 17-fold increase in photocurrent compared to Bi₄O₅Br₂ alone. This enhancement is attributed not only to the improved separation of electron-hole pairs, facilitated by the CN QDs, which boosts photocatalytic activity, but also to the enlarged range of visible light absorption. We employed an ENR-specific aptamer as the recognition element, resulting in the construction of a high-performance photoelectrochemical aptasensor for ENR detection. The sensor exhibited a linear detection range of 1×10^-1 to 1×10⁶ ng mL^-1 and a detection limit of 0.033 ng mL^-1. The impressive performance of the CN QDs/Bi₄O₅Br₂ sensing platform demonstrates its potential application in detecting ENR concentrations in food, biomedical contexts, and environmental analyses.<h3>Significance</h3>Benefiting from the sensitization of CN QDs, CN QDs/Bi₄O₅Br₂ exhibited 17-fold PEC signal of pure Bi₄O₅Br₂. The presence of quantum dots in CN QDs/Bi₄O₅Br₂ facilitates rapid separation of electron-hole pairs, leading to significantly enhanced PEC activity and improved detection performance for ENR. This research convincingly illustrates that integrating CN QDs with Bi₄O₅Br₂ nanosheets could pave the way for designing more efficient bismuth-based semiconductor photoactive materials for sensing applications.","PeriodicalId":240,"journal":{"name":"Analytica Chimica Acta","volume":"21 1","pages":""},"PeriodicalIF":6.2,"publicationDate":"2024-12-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142816224","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":"Insights into the separation, enantioseparation and recognition mechanisms of methamphetamine isotopologues on achiral and polysaccharide-based chiral columns in high-performance liquid chromatography","authors":"Giorgi Kobidze, Giorgia Sprega, Alfredo Fabrizio Lo Faro, Aurora Balloni, Paola Peluso, Tivadar Farkas, Marina Karchkhadze, Giuseppe Basile, Francesco Paolo Busardò, Bezhan Chankvetadze","doi":"10.1016/j.aca.2024.343542","DOIUrl":"https://doi.org/10.1016/j.aca.2024.343542","url":null,"abstract":"<h3>Background</h3>Isotopologues resulting from the labelling of molecules with deuterium have attracted interest due to the isotope effect observed in chemistry and biosciences. Isotope effect may also play out in noncovalent interactions and mechanisms leading to intermolecular recognition. In chromatography, differences in retention time between isotopologues, as well as between isotopomers have been observed resulting in two different elution sequences (isotope effects): the normal isotope effect when heavier isotopologues retain longer than lighter analogues, and the inverse isotope effect featuring the opposite elution order. Although several cases of deuterium isotope effects have been reported so far, the molecular bases of these phenomena remain unclear.<h3>Results</h3>We report the separation of isotopologues of methamphetamine (<em>N</em>-methyl-1-phenylpropan-2-amine) (MET), featuring different number and location of deuterium substituents, on an achiral column by high-performance liquid chromatography (HPLC), as well as the simultaneous separation of isotopologues and their enantiomers on some polysaccharide-based chiral columns. The effects of the number and location of deuterium substituents introduced in MET’s structure, of the surface chemistry of the adsorbent, and the mobile phase composition and pH on the retention and separation of isotopologues and their enantiomers were examined. In several cases, the effect of temperature was also evaluated, and the thermodynamic quantities associated with isotopologue adsorption, separation, and enantioseparation were also calculated. To elucidate the molecular bases of the experimental observations, quantum mechanics calculations were performed focusing on the vibrational degree of freedom calculated for models of isotopologue-selector complexes. On this basis, zero-point vibrational energies were computed as useful descriptors to differentiate computationally between deuterated isotopologues.<h3>Significance</h3>Using HPLC as experimental technique with the following dual function: 1) separation of MET isotopologues and their enantiomers; 2) exploring noncovalent interactions underlying their separation. The degree of deuteration, location of deuterium substituents, and mobile phase pH play key roles in isotopologue separations. By integrating experimental and computational analyses, noncovalent interactions underlying normal and inverse isotope effects were deconvoluted, highlighting the contribution of hydrogen bond, hydrophobic and dispersive forces in isotopologue and enantiomer separation.","PeriodicalId":240,"journal":{"name":"Analytica Chimica Acta","volume":"28 1","pages":""},"PeriodicalIF":6.2,"publicationDate":"2024-12-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142809514","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":"Enhanced Nano-LC-MS for Analyzing Dansylated Oral Cancer Tissue Metabolome Dissolved in Solvents with High Elution Strength","authors":"Ya-Ju Hsieh, Cheng-Yu Hung, Yi-Ting Chen, Yu-Tsun Lin, Kai-Ping Chang, Wei-Fan Chiang, Chih-Yen Chien, Chih-Ching Wu, Liang Li, Jau-Song Yu, Kun-Yi Chien","doi":"10.1016/j.aca.2024.343514","DOIUrl":"https://doi.org/10.1016/j.aca.2024.343514","url":null,"abstract":"<h3>Background</h3>Tissue metabolomics analysis, alongside genomics and proteomics, offers crucial insights into the regulatory mechanisms of tumorigenesis. To enhance metabolite detection sensitivity, chemical isotope labeling (CIL) techniques, such as dansylation, have been developed to improve metabolite separation and ionization in mass spectrometry (MS). However, the dissolution of hydrophobic derivatized metabolites in solvents with high acetonitrile content limits the use of liquid chromatography (LC) systems with small-volume reversed-phase (RP) columns. In this study, we established a nano-LC-MS system with an online dilution design to address this issue, enabling sensitive analysis of oral cancer tissue metabolomes.<h3>Results</h3>Our nano-LC system features a flow path design with online sample dilution before an RP trap column and backflushing of the trap column before entering the analytical column. Compared to other nano-LC systems, both with and without online dilution designs, our system demonstrates the superiority of the T-connector-based dilution method. Using only 1/20^th of the sample required for popular micro-LC systems, our nano-LC detects a larger number of peak pairs with similar recovery rates for both hydrophilic and hydrophobic metabolites, ensuring unbiased results. Thirty-two matched pairs of oral squamous cell carcinoma (OSCC) tissue samples and adjacent noncancerous tissues (ANTs) underwent high-throughput CIL-metabolome analysis using our nano-LC system. Compared to our previous micro-LC methods, the nano-LC-MS system exhibits enhanced detection sensitivity, significantly reducing sample requirements.<h3>Significance</h3>Our findings highlight the efficacy of our platform for metabolomic analysis with limited sample amounts. The nano-LC system’s ability to analyze samples dissolved in strong eluents suggests potential applications for handling other hydrophobic compounds using RPLC or other separation methods facing similar solvent incompatibility issues. This approach holds promise for identifying novel metabolite biomarkers for oral cancers, advancing our understanding of tumorigenesis, and enhancing clinical applications.","PeriodicalId":240,"journal":{"name":"Analytica Chimica Acta","volume":"77 1","pages":""},"PeriodicalIF":6.2,"publicationDate":"2024-12-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142805032","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 of Novel Chiral Stationary Phases Based on Chiral Metal-organic Cages Enable Extensive HPLC Enantioseparation","authors":"Zhen Wang, Wei Wang, Liquan Sun, Axin Liang, Juntao Duan, Yukui Zhang, Bo Tang, Aiqin Luo","doi":"10.1016/j.aca.2024.343541","DOIUrl":"https://doi.org/10.1016/j.aca.2024.343541","url":null,"abstract":"<h3>Background</h3>The metal organic cages (MOCs) are an emerging type of porous material that has attracted considerable research interest due to their unique properties, including good stability and well-defined intrinsic cavities. The chiral MOCs with porous structures have broad application prospects in enantiomeric recognition and separation. However, there are almost no relevant reports on chiral MOCs as chiral stationary phases (CSPs) for enantioseparation by high-performance liquid chromatography (HPLC).<h3>Results</h3>Here, we report for the first time, the chiral MOCs, MOC-PA was “wrapped” onto the silica gel to create a novel HPLC CSP of chiral MOC-PA@SiO₂ through wrapped in net method. There are 24 and 20 chiral compounds or chiral drugs, including alcohols, diols, esters, ketones, alkene, epoxides, ethers, organic acids, phenols and amines, were enantioseparated by vary degrees on MOC-PA@SiO₂ packed column under both normal phase (NP) and reversed phase (RP) modes, respectively. Furthermore, compared with commercial Chiralpak AD-H and Chiralcel OD-H columns, the MOC-PA@SiO₂ packed column exhibits well chiral separation complementarity to them. It can separate some racemates that unable to be or not to be well separated by the Chiralpak AD-H and Chiralcel OD-H columns. Besides, there are four positional isomers were also well separated by MOC-PA@SiO₂ packed column.<h3>Significance</h3>The effects of temperature and injection volume on separation of MOC-PA@SiO₂ packed column were further investigated. This column also exhibited excellent repeatability, stability and column-to-column reproducibility on separation in HPLC. This work indicates that chiral MOCs are a promising class of chiral materials to prepare new CSPs for HPLC enantioseparation.","PeriodicalId":240,"journal":{"name":"Analytica Chimica Acta","volume":"28 1","pages":""},"PeriodicalIF":6.2,"publicationDate":"2024-12-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142805101","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":"Aliphatic substrates-mediated unique rapid room temperature synthesis of carbon quantum dots for fenofibrate versatile analysis","authors":"Ali Abdel-Hakim, Fathalla Belal, Mohamed A. Hammad, Abdelaziz Elgaml, Mahmoud El-Maghrabey","doi":"10.1016/j.aca.2024.343539","DOIUrl":"https://doi.org/10.1016/j.aca.2024.343539","url":null,"abstract":"<h3>Background</h3>The current synthetic strategies for carbon dots (CDs) are usually time-consuming, rely on complicated processes, and need high temperatures and energy. Recent studies have successfully synthesized CDs at room temperature. Unfortunately, most CDs synthesized at room temperature are obtained under harsh reaction conditions, prepared using aromatic precursors, or need a long time to generate. Therefore, an energy-free room-temperature rapid synthesis of CDs under mild conditions using aliphatic substrates is important. We aim to provide an innovative approach to synthesizing CDs to be used to develop the first fluorescence-based assay of the non-fluorescent anti-hyperlipidemic drug, fenofibrate.<h3>Results</h3>We report an innovative, energy-free, and room-temperature preparation of fluorescent N-doped CDs utilizing aliphatic substrates in only 20 minutes. The synthesis was based on a self-exothermic Schiff base condensation reaction between methylglyoxal and ethylenediamine. The prepared CDs' antibacterial properties, biocompatibility, and cell-imaging ability were investigated. The fluorescence signal of the CDs was quantitively quenched upon adding increasing concentrations of fenofibrate in the range of 0.50-15.0 μg/mL. Therefore, the prepared CDs were applied as a nanosensor to develop the first fluorescence-based assay of fenofibrate. The reliability of the synthesized nanosensor was confirmed by the successful quantification of fenofibrate in pharmaceutical dosage forms, environmental water, weight-loss herbal products, and dietary supplements. The obtained recovery ranged from 95.33 to 104.58%. In addition, the minimal environmental impact of the developed fenofibrate sensing strategy was confirmed using the recently reported metrics.<h3>Significance and novelty</h3>The key advantage of this work is the use of an energy-free approach to synthesize CDs rapidly under mild conditions without aromatic substrates. This opens a new window for the eco-friendly synthesis of CDs that avoids the drawbacks of the traditional methods. Additionally, it is the first fluorescence nanosensor for sensing fenofibrate in various matrices, avoiding the limitations of the previous methods, such as high cost, poor selectivity, and low sensitivity.","PeriodicalId":240,"journal":{"name":"Analytica Chimica Acta","volume":"38 1","pages":""},"PeriodicalIF":6.2,"publicationDate":"2024-12-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142797236","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":"Bifunctional Probe Propelling Multipath Strand Displacement Amplification Tandem CRISPR/Cas12a for Ultrasensitive and Robust Assay of DNA Methyltransferase Activity","authors":"Fei Yu, Qiongwen Zhang, Tiantian Ma, Shuying Zhang, Fanting Wang, Dan Yue, Shihan Liu, Yueqi Liao, Li-e Liu, Yongjun Wu, Wenqiao Zang","doi":"10.1016/j.aca.2024.343540","DOIUrl":"https://doi.org/10.1016/j.aca.2024.343540","url":null,"abstract":"<h3>Background</h3>DNA methylation catalyzed by various DNA methyltransferases (DNA MTases) is one of the important epigenetic regulations in both eukaryotes and prokaryotes. Therefore, the detection of DNA MTase activity is a vital target and direction in the study of methylation-related diseases.<h3>Results</h3>In this study, an ultrasensitive and robust strategy was developed for DNA MTase activity sensing based on bifunctional probe propelling multipath strand displacement amplification and CRISPR/Cas12a techniques. First, a bifunctional hairpin probe (bHpDNA) was designed instead of a conventional single-function probe. In the presence of DNA MTase, the bHpDNA was methylated and cleaved by a restriction endonuclease into two independent primers, both of which bind with the templates to trigger strand displacement amplification and produce the active DNA of CRISPR/Cas12a. Second, annealing-assisted binding instead of free diffusion adhesion was used to improve hybridization efficiency between the primers and templates. Finally, the CRISPR/Cas12a system was used to achieve fluorescence signal output to analyze DNA MTase activity. If targets were absent, there was no signal because no primers were released from the bHpDNA. To verify the reliability of the method, two key DNA MTases, Dam and M.SssI, were analyzed, and their limits of detection were 2.458 × 10⁻³ and 3.820 × 10⁻³ U/mL, respectively, which were lower than those of most reported fluorescence methods.<h3>Significance</h3>This method was successfully used in the evaluation of DNA MTase inhibitors and the detection of DNA MTase activity in complex biological systems with good recoveries and relative standard deviation at low spiked concentrations (0.1–1 U/mL), which all indicate that this method is an ultrasensitive and robust strategy in DNA MTase activity assay and has great potential in biomedical and clinical detection.","PeriodicalId":240,"journal":{"name":"Analytica Chimica Acta","volume":"12 1","pages":""},"PeriodicalIF":6.2,"publicationDate":"2024-12-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142797233","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":"Low-potential bionic electrochemiluminescence sensing platform based on SnS2/CuNWs synergistic promotion for highly selective detection of glycocholic acid","authors":"Yuwei Wang, Shanshan Tang, Miao Liu, Wei Wang, Axin Liang, Aiqin Luo","doi":"10.1016/j.aca.2024.343537","DOIUrl":"https://doi.org/10.1016/j.aca.2024.343537","url":null,"abstract":"<h3>Background</h3>Glycholic acid (GCA) can dynamically reflect the process of liver injury, and can be used for early diagnosis and curative effect evaluation of early hepatitis and cirrhosis. The highly sensitive detection of liver injury markers is conducive to a more accurate and effective auxiliary diagnosis of liver diseases. In addition, the low trigger potential helps to avoid more chemical interference and improve the detection sensitivity. It is of great significance to develop a high sensitive and low potential ECL sensor for GCA detection.<h3>Results</h3>In this work, a low trigger potential molecularly imprinted electrochemiluminescence sensor (MIECLS) combining SnS₂ and CuNWs was proposed for highly selective and sensitive detection of GCA, a marker of liver injury. The stabilization and enhancement of ECL signal can be attributed to the synergistic promotion strategy of SnS₂ and CuNWs. CuNWs not only has good ECL performance, but also serves as a substrate material for loading SnS₂ to enhance the film forming performance. In addition, the Sn⁴⁺ active site can be regenerated by redox reaction, significantly improving the efficiency of the co-reactant and the stability of the sensor. By studying the ECL luminescence mechanism and specific recognition quenching mechanism of MIECLS in detail, a selective detection method for GCA was established. Under optimal conditions, in the range of 5 × 10⁻¹⁰ to 5 × 10⁻⁶ mol L⁻¹, the quenching value of ECL intensity is proportional to Lg<em>C</em>_GCA, and the limit of detection is 1.30 × 10⁻¹⁰ mol L⁻¹.<h3>Significance and novelty</h3>In addition, satisfactory recovery rate was obtained in human serum samples, showing good practical application, providing a new way for clinical detection of GCA. At the same time, it not only broadens the development of CuNWs in the ECL field, but also provides a new way to reduce the triggering potential.","PeriodicalId":240,"journal":{"name":"Analytica Chimica Acta","volume":"83 1","pages":""},"PeriodicalIF":6.2,"publicationDate":"2024-12-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142793584","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":"Feasible band boundaries computation in bilinear matrix decomposition using essential data","authors":"Somaye Vali Zade, Mathias Sawall, Klaus Neymeyr, Alejandro C. Olivieri, Roma Tauler, Hamid Abdollahi","doi":"10.1016/j.aca.2024.343538","DOIUrl":"https://doi.org/10.1016/j.aca.2024.343538","url":null,"abstract":"<h3>Background</h3>Multivariate curve resolution methods are usually confronted with non-unique pure component factors. This rotational ambiguity can be represented by ranges of feasible profiles, which are equally compatible with the imposed constraints. Sensor-wise N-BANDS is an effective algorithm for the calculation of the bounds of feasible profiles in the presence of noise, but suffers from high computational cost.<h3>Results</h3>Sensor-wise N-BANDS has been combined with the concept of essential data points to speed up the computation. The combined algorithm provides full curve resolution independent of the number of chemical species. The effectiveness of the proposed algorithm is demonstrated for simulated chromatographic data and experimental spectro-electrochemical data.<h3>Significance</h3>With the new proposal, the boundaries of the set of feasible profiles in bilinear matrix decomposition can be estimated in a reasonable time, for any number of components, and in the presence of instrumental noise. For the simulated data, the reduction in computation time was more than 95%. Similarly, for the relatively large experimental spectro-electrochemical data, the reduction in computation time was over 85%.","PeriodicalId":240,"journal":{"name":"Analytica Chimica Acta","volume":"4 1","pages":""},"PeriodicalIF":6.2,"publicationDate":"2024-12-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142797242","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}