Thomas Hix-Janssens, Julia R Davies, Nicholas W Turner, Börje Sellergren, Mark V Sullivan
{"title":"Molecularly imprinted nanogels as synthetic recognition materials for the ultrasensitive detection of periodontal disease biomarkers.","authors":"Thomas Hix-Janssens, Julia R Davies, Nicholas W Turner, Börje Sellergren, Mark V Sullivan","doi":"10.1007/s00216-024-05395-6","DOIUrl":"10.1007/s00216-024-05395-6","url":null,"abstract":"<p><p>Periodontal disease affects supporting dental structures and ranks among one of the top most expensive conditions to treat in the world. Moreover, in recent years, the disease has also been linked to cardiovascular and Alzheimer's diseases. At present, there is a serious lack of accurate diagnostic tools to identify people at severe risk of periodontal disease progression. Porphyromonas gingivalis is often considered one of the most contributing factors towards disease progression. It produces the Arg- and Lys-specific proteases Rgp and Kgp, respectively. Within this work, a short epitope sequence of these proteases is immobilised onto a magnetic nanoparticle platform. These are then used as a template to produce high-affinity, selective molecularly imprinted nanogels, using the common monomers N-tert-butylacrylamide (TBAM), N-isopropyl acrylamide (NIPAM), and N-(3-aminopropyl) methacrylamide hydrochloride (APMA). N,N-Methylene bis(acrylamide) (BIS) was used as a crosslinking monomer to form the interconnected polymeric network. The produced nanogels were immobilised onto a planar gold surface and characterised using the optical technique of surface plasmon resonance. They showed high selectivity and affinity towards their template, with affinity constants of 79.4 and 89.7 nM for the Rgp and Kgp epitope nanogels, respectively. From their calibration curves, the theoretical limit of detection was determined to be 1.27 nM for the Rgp nanogels and 2.00 nM for the Kgp nanogels. Furthermore, they also showed excellent selectivity against bacterial culture supernatants E8 (Rgp knockout), K1A (Kgp knockout), and W50-d (wild-type) strains in complex medium of brain heart infusion (BHI).</p>","PeriodicalId":462,"journal":{"name":"Analytical and Bioanalytical Chemistry","volume":" ","pages":"7305-7316"},"PeriodicalIF":3.8,"publicationDate":"2024-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11584468/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141426004","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}
J Guercetti, N Pascual, A Aviñó, R Eritja, J-P Salvador, M-P Marco
{"title":"DNA-directed immobilization fluorescent immunoarray for multiplexed antibiotic residue determination in milk.","authors":"J Guercetti, N Pascual, A Aviñó, R Eritja, J-P Salvador, M-P Marco","doi":"10.1007/s00216-024-05481-9","DOIUrl":"10.1007/s00216-024-05481-9","url":null,"abstract":"<p><p>The presence of antibiotic residues in cow's milk entails high risk for consumers, the dairy industry, and the environment. Therefore, the development of highly specific and sensitive screening tools for the rapid and cost-effective identification of traces of these compounds is urgently needed. A multiplexed screening platform utilizing DNA-directed immobilization (DDI) was developed aiming to detect three classes of antibiotic residues (fluoroquinolones, sulfonamides, and tylosin) prevalently found in milk. Throughout this work, each oligonucleotide sequence was conjugated to a different hapten molecule, while the three complementary strands were immobilized in 24 independent microarray chips on a single glass slide. First, the array was incubated with the pool of hapten-oligonucleotide conjugate site encoded the signal through DNA hybridization. Next, commercial milk samples were incubated with the cocktail of monoclonal antibodies following a secondary fluorophore-labeled antibody which was required for fluorescent readout. Direct sample detection was achieved in milk diluting 20 times in assay buffer. The limits of detection (LODs) reached were 1.43 µg kg<sup>-1</sup>, 1.67 µg kg<sup>-1</sup>, and 0.89 µg kg<sup>-1</sup> for TYLA, STZ, and CIP, respectively, which represented in raw milk 7.15 µg kg<sup>-1</sup>, 8.35 µg kg<sup>-1</sup>, and 4.45 µg kg<sup>-1</sup> for TYLA, STZ, and CIP, respectively, that are below the EU regulatory limits. Cross-reactivity profiles were evaluated against the family of structurally related antibiotics in order to demonstrate the capability to detect antibiotics from the same family of compounds. A pre-validation study was performed by spiking 20 blind samples above and below the maximum residue limits established by the EU guidelines. The system was successfully implemented towards randomized sample classification as compliant or non-compliant. The proposed DDI-based immunoarray provides a fast and cost-effective alternative to obtain semi-quantitative information about the presence of three veterinary residues simultaneously in milk samples.</p>","PeriodicalId":462,"journal":{"name":"Analytical and Bioanalytical Chemistry","volume":" ","pages":"7325-7336"},"PeriodicalIF":3.8,"publicationDate":"2024-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11584450/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142078721","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}
María A García-Trejo, Gregorio Castañeda, Ángel Ríos
{"title":"Analytical control of imatinib in bioanalytical samples using graphene quantum dots sensing.","authors":"María A García-Trejo, Gregorio Castañeda, Ángel Ríos","doi":"10.1007/s00216-024-05346-1","DOIUrl":"10.1007/s00216-024-05346-1","url":null,"abstract":"<p><p>An analytical method for the determination of imatinib (IMA, the primary treatment for chronic myeloid leukemia), based on the fluorescence properties of graphene quantum dots (GQDs), is reported in this work. The method is addressed to the analytical control of IMA in biological and pharmaceutical samples, due to the present interest in the control of the doses of this anticancer drug, as well as the therapeutic monitoring. The whole method involves the use of a solid-phase extraction (SPE) procedure, followed by an evaporation step, for the treatment of biological samples. For that, tC18 sorbent cartridges were used. After the sample treatment, the solution containing the analyte was mixed with an aqueous solution of GQDs at pH 7.2, and the fluorescent quenching of GQDs was measured. IMA was determined in the 10-250 µg L<sup>-1</sup> range, with a limit of detection of 21 µg L<sup>-1</sup> and a precision of 1.5% as relative standard deviation, measured in terms of reproducibility. The recovery for biological samples was in the 84-113% range.</p>","PeriodicalId":462,"journal":{"name":"Analytical and Bioanalytical Chemistry","volume":" ","pages":"7267-7276"},"PeriodicalIF":3.8,"publicationDate":"2024-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141097191","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}
Andaravaas Patabadige Jude P Vaas, Raymond B Yu, Joselito P Quirino
{"title":"Stacking in electrophoresis by electroosmotic flow-assisted admicelle to solvent microextraction.","authors":"Andaravaas Patabadige Jude P Vaas, Raymond B Yu, Joselito P Quirino","doi":"10.1007/s00216-024-05554-9","DOIUrl":"10.1007/s00216-024-05554-9","url":null,"abstract":"<p><p>An in-line sample concentration method for capillary electrophoresis called admicelle to solvent microextraction was proposed. In this technique, analytes were trapped in the cetyltrimethylammonium bromide admicelles formed in situ on the negatively charged capillary surface. A solvent plug was then partially injected hydrodynamically to collapse the admicelles, which liberated and focused the analytes at the solvent front. Voltage was applied across the capillary, completing the stacking process. Various solvents, namely, methanol, ethanol, and acetonitrile, were investigated. The optimal solvent for solvent to admicelle microextraction was 30% acetonitrile in 24 mM sodium tetraborate (pH 9.2). Sample injection time and solvent to sample injection ratio were also optimised. For this demonstration, the optimum sample injection time and solvent to sample injection ratio were 320 s and 1:2, respectively. Using the optimum conditions, UV detection sensitivity was enhanced 132-176-fold for the model anions. The LOQ, %intra-/inter-day (n = 6/n = 12, 2 days) repeatability, and linearity (R<sup>2</sup>) of admicelle to solvent microextraction were 0.08-2 µg/mL, 1.9-3.9%, 2.8-4.9%, and 0.992, respectively. Admicelle to solvent microextraction was applied to the analysis of various fortified water samples, with good repeatability (%RSD = 0.5-3.6%), and no matrix interferences.</p>","PeriodicalId":462,"journal":{"name":"Analytical and Bioanalytical Chemistry","volume":" ","pages":"6789-6798"},"PeriodicalIF":3.8,"publicationDate":"2024-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142363899","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":"Development and application of a dual isotopic labeling method for enhanced detection and quantification of stimulants in urine samples using high-resolution mass spectrometry.","authors":"Yang Wang, Wanli Li, Xiaojun Deng","doi":"10.1007/s00216-024-05612-2","DOIUrl":"10.1007/s00216-024-05612-2","url":null,"abstract":"<p><p>Given the critical nature of anti-doping efforts, the detection of stimulant substances is shifting from accurate qualitative analysis to precise quantitative analysis. Additionally, the use of liquid chromatography-high-resolution mass spectrometry (LC-HRMS) in detecting stimulants is becoming more widespread. However, the lack of isotope-labeled internal standards is causing increasing issues with quantitative accuracy. Furthermore, challenges such as the mass spectrometric response of small molecules and the separation of isomers present additional difficulties. We have developed a quantitative method for stimulant substances containing amine or phenol hydroxyl groups, using a dual-label derivatization system. This method offers a new perspective for analyzing and detecting low molecular weight substances, isomers, or those with poor LC-MS response, and proposes a solution to the problem of missing isotope-labeled internal standards. Methodological validation has shown that this approach has promising application potential.</p>","PeriodicalId":462,"journal":{"name":"Analytical and Bioanalytical Chemistry","volume":" ","pages":"7073-7084"},"PeriodicalIF":3.8,"publicationDate":"2024-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142492486","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}
Wen-Ya Liu, Di Xu, Hui-Hui Meng, Cheng-Yao Wang, Xin Feng, Jun-Song Wang
{"title":"Metabolic fate of the natural anticancer agent cucurbitacin B: an LC-MS/MS-enabled profiling of its major phase I and II conjugates in vivo.","authors":"Wen-Ya Liu, Di Xu, Hui-Hui Meng, Cheng-Yao Wang, Xin Feng, Jun-Song Wang","doi":"10.1007/s00216-024-05608-y","DOIUrl":"10.1007/s00216-024-05608-y","url":null,"abstract":"<p><p>Cucurbitacin B (CuB) is a natural triterpenoid with diverse pharmacological effects including potent anticancer activity. However, its oral bioavailability is hampered by limited metabolism in vivo. We characterized CuB's in vivo metabolism in rats to uncover bioactive metabolites retaining therapeutic potential, using a robust UHPLC-Q-TOF-MS/MS workflow. This workflow combined molecular networking, fragmentation filtering, and mass defect filtering to identify CuB metabolites in rat urine, plasma, and feces following oral administration. Thirteen metabolites were identified and seven were confirmed. Major phase I transformations involved hydrolysis, reduction, epoxidation, and amination. Phase II conjugation included cysteine, glutathione, glucuronide, and gluconic acid conjugates. Notably, one of the main metabolites formed was the cysteine conjugate CuB-Cys. CuB-Cys maintained similar in vitro antiproliferative activity to CuB on HepG2, MCF-7, and PANC-1 cancer cell lines. However, it demonstrated lower cytotoxicity towards non-cancerous L02 cells, highlighting improved therapeutic selectivity. Mechanistically, CuB-Cys induced greater apoptotic signaling in HepG2 cells than CuB via enhanced caspase activation and disrupted BAX-Bcl-2 balance. This represents the first systematic characterization of CuB's in vivo metabolic pathway. The identification and confirmation of CuB-Cys provide insight for drug development efforts aiming to maintain therapeutic efficacy while reducing toxicity, via metabolite-based approaches. Our findings shed light on strategies for improving CuB's clinical potential.</p>","PeriodicalId":462,"journal":{"name":"Analytical and Bioanalytical Chemistry","volume":" ","pages":"7043-7062"},"PeriodicalIF":3.8,"publicationDate":"2024-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142492489","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}
Haojie Hu, Chen He, Di Zhu, Weilai Zhang, Xiaocun Zhuo, Yuguo Li, Quan Shi
{"title":"Revealing the backbone structures of land-based fulvic acids derived from river and soil through n-butylsilane reduction.","authors":"Haojie Hu, Chen He, Di Zhu, Weilai Zhang, Xiaocun Zhuo, Yuguo Li, Quan Shi","doi":"10.1007/s00216-024-05589-y","DOIUrl":"10.1007/s00216-024-05589-y","url":null,"abstract":"<p><p>While ultra-high-resolution mass spectrometry has enabled the identification of the molecular composition of dissolved organic matter (DOM), elucidating its molecular structure remains a challenging endeavor. Here, two fulvic acids (FAs), one from river and the other from forest soil, were subjected to reduction using an optimized n-butylsilane (n-BS) reduction method. The reduction products were purified through a combination of liquid-liquid extraction and silica gel column chromatography, resulting in the separation into saturates, aromatics, and polar products. The polar products were analyzed by high-resolution mass spectrometry (HRMS), and the saturates and aromatics were analyzed using gas chromatography-mass spectrometry (GC-MS). HRMS results showed that the number of oxygen atoms and double-bond equivalent (DBE) values of FA decreased after reduction. GC-MS results revealed that a total of 270 hydrocarbon monomers were identified from the reduction products of a single sample, with the highest carbon number of cycloalkanes reaching C<sub>33</sub>. For the first time, steranes and hopanes were detected in the reduction products, potentially serving as evidence for the existence of carboxyl-rich alicyclic molecule (CRAM) precursors. Additionally, a significant number of polycyclic aromatic hydrocarbons were identified, and the potential sources of various compounds were preliminarily inferred based on their isomers. This study extends the knowledge of the possible backbone structure of the DOM and provides a new potential tool for investigating the origin and transformation mechanisms of DOM.</p>","PeriodicalId":462,"journal":{"name":"Analytical and Bioanalytical Chemistry","volume":" ","pages":"6919-6929"},"PeriodicalIF":3.8,"publicationDate":"2024-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142398950","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}
Andrea Fiorani, Claudio Ignazio Santo, Kohei Sakanoue, Donato Calabria, Mara Mirasoli, Francesco Paolucci, Giovanni Valenti, Yasuaki Einaga
{"title":"Electrogenerated chemiluminescence from luminol-labelled microbeads triggered by in situ generation of hydrogen peroxide.","authors":"Andrea Fiorani, Claudio Ignazio Santo, Kohei Sakanoue, Donato Calabria, Mara Mirasoli, Francesco Paolucci, Giovanni Valenti, Yasuaki Einaga","doi":"10.1007/s00216-024-05356-z","DOIUrl":"10.1007/s00216-024-05356-z","url":null,"abstract":"<p><p>We developed a sensing strategy that mimics the bead-based electrogenerated chemiluminescence immunoassay. However, instead of the most common metal complexes, such as Ru or Ir, the luminophore is luminol. The electrogenerated chemiluminescence of luminol was promoted by in situ electrochemical generation of hydrogen peroxide at a boron-doped diamond electrode. The electrochemical production of hydrogen peroxide was achieved in a carbonate solution by an oxidation reaction, while at the same time, microbeads labelled with luminol were deposited on the electrode surface. For the first time, we proved that was possible to obtain light emission from luminol without its direct oxidation at the electrode. This new emission mechanism is obtained at higher potentials than the usual luminol electrogenerated chemiluminescence at 0.3-0.5 V, in conjunction with hydrogen peroxide production on boron-doped diamond at around 2-2.5 V (vs Ag/AgCl).</p>","PeriodicalId":462,"journal":{"name":"Analytical and Bioanalytical Chemistry","volume":" ","pages":"7277-7283"},"PeriodicalIF":3.8,"publicationDate":"2024-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141246896","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}
Luisa Speicher, Hao Song, Norman Ahlmann, Daniel Foest, Simon Höving, Sebastian Brandt, Guanghui Niu, Joachim Franzke, Caiyan Tian
{"title":"Correction to: Soft ionization mechanisms in flexible μ‑tube plasma-from FμTP to closed μ‑tube plasma.","authors":"Luisa Speicher, Hao Song, Norman Ahlmann, Daniel Foest, Simon Höving, Sebastian Brandt, Guanghui Niu, Joachim Franzke, Caiyan Tian","doi":"10.1007/s00216-024-05621-1","DOIUrl":"10.1007/s00216-024-05621-1","url":null,"abstract":"","PeriodicalId":462,"journal":{"name":"Analytical and Bioanalytical Chemistry","volume":" ","pages":"7191"},"PeriodicalIF":3.8,"publicationDate":"2024-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11579189/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142492485","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}
Augusto Juste-Dolz, William Teixeira, Yeray Pallás-Tamarit, Mario Carballido-Fernández, Javier Carrascosa, Ángela Morán-Porcar, María Ángeles Redón-Badenas, María Gracia Pla-Roses, María Dolores Tirado-Balaguer, María José Remolar-Quintana, Jon Ortiz-Carrera, Ethel Ibañez-Echevarría, Angel Maquieira, David Giménez-Romero
{"title":"Real-world evaluation of a QCM-based biosensor for exhaled air.","authors":"Augusto Juste-Dolz, William Teixeira, Yeray Pallás-Tamarit, Mario Carballido-Fernández, Javier Carrascosa, Ángela Morán-Porcar, María Ángeles Redón-Badenas, María Gracia Pla-Roses, María Dolores Tirado-Balaguer, María José Remolar-Quintana, Jon Ortiz-Carrera, Ethel Ibañez-Echevarría, Angel Maquieira, David Giménez-Romero","doi":"10.1007/s00216-024-05407-5","DOIUrl":"10.1007/s00216-024-05407-5","url":null,"abstract":"<p><p>The biosensor, named \"virusmeter\" in this study, integrates quartz crystal microbalance technology with an immune-functionalized chip to distinguish between symptomatic patients with respiratory diseases and healthy individuals by analyzing exhaled air samples. Renowned for its compact design, rapidity, and noninvasive nature, this device yields results within a 5-min timeframe. Evaluated under controlled conditions with 54 hospitalized symptomatic COVID-19 patients and 128 control subjects, the biosensor demonstrated good overall sensitivity (98.15%, 95% CI 90.1-100.0) and specificity (96.87%, 95% CI 92.2-99.1). This proof-of-concept presents an innovative approach with significant potential for leveraging piezoelectric sensors to diagnose respiratory diseases.</p>","PeriodicalId":462,"journal":{"name":"Analytical and Bioanalytical Chemistry","volume":" ","pages":"7369-7383"},"PeriodicalIF":3.8,"publicationDate":"2024-12-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11584482/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141449282","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}