Analytica Chimica Acta最新文献

{"title":"A magnetic SERS-imprinted sensor for the determination of cardiac troponin I based on proteolytic peptide technology","authors":"Shuqian Wang ,&nbsp;Jinli Qin ,&nbsp;Yin Liang ,&nbsp;Youai Ye ,&nbsp;Yamei Guo ,&nbsp;Shushu Li ,&nbsp;Xiao Yang ,&nbsp;Yong Liang","doi":"10.1016/j.aca.2024.343316","DOIUrl":"10.1016/j.aca.2024.343316","url":null,"abstract":"<div><div>Acute myocardial infarction is a sudden and high-mortality disease that can be accurately diagnosed by measuring the level of cardiac troponin I in the blood. Currently, cTnI commonly used clinical detection methods usually have excellent sensitivity and are suitable for large-scale sample detection analysis. However, most of these methods are operated through multiple steps of fixation, incubation, reaction and separation, and most of them require professionals to operate complex instruments, which greatly limits their applicability in real-time rapid detection. Therefore, a method that requires low professional skills and can perform rapid detection is necessary. We presents an alternative strategy to quantify cTnI in clinical serum samples using a combination of SERS and magnetic molecularly imprinted polymers (MMIP). MMIPs was synthesized under Polyvinyl Pyrrolidone (PVP) conditions without vinyl modification using characteristic peptide as template, MAA and DMAm as functional monomers. The internal Raman probe 4-MBA was connected through Ag-SH bonds in MMIPs to solve the problem that the target object had no Raman characteristic peak. MMIPs with high magnetic and adsorptive properties showed characteristic absorption peaks at the Raman shift of 1582 cm⁻¹ after specific capture of the target templates. The Raman signals of the 4-MBA were reduced due to shielding effects and the detection range of this method was 0.001–100 ng mL⁻¹. The recoveries and relative standard deviations (RSDs) of the spiked experiments were 103.1%–106.3 % and 3.54 %–7.38 %, respectively. In summary, this work had appropriate sensitivity and specificity, and there was no significant difference in detection results after ELISA verification. It provided a flexible and practical analysis method for detecting cTnI based on SERS technology. In addition, the imprinting materials of other disease markers can be prepared by changing the template molecules, which provides a new idea for the detection of other biomarkers.</div></div>","PeriodicalId":240,"journal":{"name":"Analytica Chimica Acta","volume":"1332 ","pages":"Article 343316"},"PeriodicalIF":5.7,"publicationDate":"2024-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142444454","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":"Detection of factor Xa activity using giant magnetoresistive biosensors","authors":"Yulhwa Lee ,&nbsp;Songeun Kim ,&nbsp;Tae-Jin Song ,&nbsp;Shan X. Wang ,&nbsp;Jung-Rok Lee","doi":"10.1016/j.aca.2024.343347","DOIUrl":"10.1016/j.aca.2024.343347","url":null,"abstract":"<div><h3>Background</h3><div>As anticoagulants are widely used to treat patients with atrial fibrillation (AF) and other thrombotic conditions, it is necessary for physicians to determine whether the medication has been taken in emergencies. Among many anticoagulants, rivaroxaban has attracted attention due to its safety and convenience. Since rivaroxaban inhibits activated coagulation factor X (factor Xa), measuring factor Xa activity can determine the presence of rivaroxaban.</div></div><div><h3>Results</h3><div>We report a magnetic biosensing platform capable of measuring the activity of factor Xa using peptide substrates conjugated with magnetic nanoparticles (MNPs). Due to the size of factor Xa, a new method of solution-phase assays was proposed for magnetic biosensing platforms to address issues with immobilized peptides on the sensors. This method was validated with factor Xa and trypsin, both of which are serine proteases. In the solution-phase assays, samples with either the enzymes of interest or no enzyme were simultaneously measured, and the activity of the enzyme was estimated using the difference between the measurements. Unlike conventional optical methods, our platform was capable of detecting the activity of factor Xa at 2 μg mL⁻¹ with a 30 min sample incubation.</div></div><div><h3>Significance</h3><div>The assay using giant magnetoresistive biosensors outperformed conventional optical techniques. This platform can facilitate the determination of the presence of rivaroxaban and assist physicians in deciding on appropriate treatments for patients.</div></div>","PeriodicalId":240,"journal":{"name":"Analytica Chimica Acta","volume":"1331 ","pages":"Article 343347"},"PeriodicalIF":5.7,"publicationDate":"2024-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142444272","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":"Microcolumn and coelution hydration of oil seal blood spot for efficient screening of newborn α-thalassemia via chip isoelectric focusing","authors":"Genhan Zha ,&nbsp;Xuan Xiao ,&nbsp;Youli Tian ,&nbsp;Hengying Zhu ,&nbsp;Ping Chen ,&nbsp;Qiang Zhang ,&nbsp;Changjie Yu ,&nbsp;Honggen Li ,&nbsp;Yuxing Wang ,&nbsp;Chengxi Cao","doi":"10.1016/j.aca.2024.343342","DOIUrl":"10.1016/j.aca.2024.343342","url":null,"abstract":"<div><h3>Background</h3><div>The global prevalence of α-thalassemia necessitates effective newborn screening strategies due to its severe clinical consequences. Traditional methods such as liquid chromatography (LC), capillary electrophoresis (CE), and isoelectric focusing (IEF) face limitations, including low separation efficiency, poor sensitivity for detecting Hb Bart's, and time-intensive operations, particularly with dried blood spots (DBS). These limitations hinder timely and accurate screening. This study addresses the need for a more efficient, sensitive, and rapid method for detecting Hb Bart's in newborns.</div></div><div><h3>Results</h3><div>We enhanced IEF separation and sensitivity by designing a microfluidic IEF (mIEF) system with shortened columns and employing a coelution sample loading technique using oil-sealed blood spots for rapid sample pretreatment. Our experiments demonstrated significant improvements: the total analysis time was reduced from 1110 min (IPG IEF) and 46 min (LC) per batch to 36 min per batch. For individual samples, the focusing time decreased from 6 min (previous mIEF) to 3 min, with the microcolumn length shortened by 50 %, from 30 mm to 15 mm. The developed method showed excellent consistency with clinical Bart's detection and PCR diagnosis, achieving 100 % sensitivity and 98 % specificity for α-thalassemia screening.</div></div><div><h3>Significance and novelty</h3><div>Our novel mIEF method provides an efficient, sensitive, and rapid tool for screening newborns for α-thalassemia. This advancement addresses the limitations of traditional techniques, improving early diagnosis and intervention strategies and ultimately enhancing health outcomes for at-risk newborns.</div></div>","PeriodicalId":240,"journal":{"name":"Analytica Chimica Acta","volume":"1331 ","pages":"Article 343342"},"PeriodicalIF":5.7,"publicationDate":"2024-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142439999","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":"Residence time prediction in magnetically controlled biomolecular local rebinding-dissociation kinetics","authors":"Can Zuo,&nbsp;Yumei Wen,&nbsp;Dongyu Chen,&nbsp;Jihai Ouyang,&nbsp;Ping Li","doi":"10.1016/j.aca.2024.343341","DOIUrl":"10.1016/j.aca.2024.343341","url":null,"abstract":"<div><div>The residence time of drug-target conjugates is a critical factor in drug screening and efficacy prediction. The local rebinding-dissociation kinetics gives insights into in-vivo drug-target interactions. A magnetic torque system (MTS) is designed to observe rebinding-dissociation kinetics for predicting residence time. The system utilizes an alternating magnetic field (AMF) to manipulate the magnetization motion of magnetically labeled biomolecules and the forces acting upon biomolecular bonds. The motion, sensed by a quartz crystal microbalance (QCM), reflects biomolecular interactions occurring at the particle surface. Meanwhile, the motion facilitates the separation of dissociated molecules from the surface, thereby obviating the necessity for fixed and mobile phases in common kinetics observations. The constant and static solution environment minimizes reagent consumption. The MTS was utilized to observe the local rebinding-dissociation of antibodies (PAB and MAB) to magnetic beads (MB) and to HER2 receptors. The residence times recorded by the MTS were larger than the results obtained via SPR method, due to the occurrences of rebinding-dissociation kinetics. Interaction behaviours can be meticulously regulated for varying affinities by modulating the intensity of magnetic field. A high intensity field (400 Oe) was applied for strong binding between antibody-MB (biotin-streptavidin), and a low intensity field (300 Oe) was applied for weak antigen-antibody interactions. An increase in AMF strength enhanced dissociation, with a shift from 300 Oe to 400 Oe resulting in a 1 ∼ 4-fold reduction in residence time. Overall, the MTS provides an interactive and customizable perspective on kinetics observations.</div></div>","PeriodicalId":240,"journal":{"name":"Analytica Chimica Acta","volume":"1331 ","pages":"Article 343341"},"PeriodicalIF":5.7,"publicationDate":"2024-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142439998","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 decision confidence in AI using Monte Carlo dropout for Raman spectra classification","authors":"Jhonatan Contreras ,&nbsp;Thomas Bocklitz","doi":"10.1016/j.aca.2024.343346","DOIUrl":"10.1016/j.aca.2024.343346","url":null,"abstract":"<div><h3>Background</h3><div>Machine learning algorithms for bacterial strain identification using Raman spectroscopy have been widely used in microbiology. During the training phase, existing datasets are augmented and used to optimize model architecture and hyperparameters. After training, it is presumed that the models have reached their peak performance and are used for inference without being further enhanced. Our methodology combines Monte Carlo Dropout (MCD) with convolutional neural networks (CNNs) by utilizing dropout during the inference phase, which enables to measure the model uncertainty, a critical but often ignored aspect in deep learning models.</div></div><div><h3>Results</h3><div>We categorize unseen input data into two subsets based on the uncertainty of their prediction by employing MCD and defining the threshold using the Gaussian Mixture Model (GMM). The final prediction is obtained on the subset of testing data that exhibits lower model uncertainty, thereby enhancing the reliability of the results. To validate our method, we applied it to two Raman spectra datasets. As a result, we have observed an increase in accuracy of 9 % for Dataset 1 (from 83.10 % to 92.10 %) and 12.82 % for Dataset 2 (from 83.86 % to 96.68 %). These improvements were observed within specific subsets of the data: 826 out of 1206 spectra in Dataset 1 and 1700 out of 3000 spectra in Dataset 2. This demonstrates the effectiveness of our approach in improving prediction accuracy by focusing on data with lower uncertainty.</div></div><div><h3>Significance</h3><div>Different from routine prediction based on mere probabilities, we believe this uncertainty-guided prediction is more effective to ensure a high prediction rate rather than the prediction on the entire dataset. By guiding the decision-making of a model on higher-confidence subsets, our methodology can enhance the accuracy of classification in critical areas like disease diagnosis and safety monitoring. This targeted approach is to advance microbial identification and produces more trustworthy predictions.</div></div>","PeriodicalId":240,"journal":{"name":"Analytica Chimica Acta","volume":"1332 ","pages":"Article 343346"},"PeriodicalIF":5.7,"publicationDate":"2024-10-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142444273","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}

{"title":"Simultaneous determination of somatic cell count and total plate count in raw milk based on ATP bioluminescence assay","authors":"Longrui Yang ,&nbsp;Xiaoyun Sun ,&nbsp;Jiaci Chen ,&nbsp;Juan Zhang ,&nbsp;Xiaoyu Li ,&nbsp;Song Qu ,&nbsp;Kai Wu ,&nbsp;Fengchun Huang ,&nbsp;Ailiang Chen","doi":"10.1016/j.aca.2024.343338","DOIUrl":"10.1016/j.aca.2024.343338","url":null,"abstract":"<div><div>The somatic cell count (SCC) and total plate count (TPC) are essential quality indicators for raw milk. Traditional detection methods require separate measurements and rely on complex, large-scale instruments or cultivation techniques, which are both time-consuming and laborious. To address these challenges, this study developed a novel method for the simultaneous detection of SCC and TPC in the same raw milk sample using the ATP bioluminescence assay. This method utilizes oxy-ethylated iso-nonyl phenol (Neonol-10) and cetyltrimethylammonium bromide (CTAB) to selectively lyse somatic cells and microorganisms, respectively. This technique is straightforward to operate and can be completed within 2.5 h, with detection ranges of 1 × 10⁴ to 3 × 10⁶ cells/mL for SCC and 1 × 10⁵ to 5 × 10⁷ CFU/mL for TPC. Importantly, this technique meets the requirements of detection standards in China, European Union, Canada, United States, etc. For SCC or TPC in raw milk. Overall, this innovative approach does not rely on expensive equipment or facilities and the stepwise reagent addition procedure can be easily developed into an automated high-throughput system for rapid on-site testing of SCC and TPC in raw milk.</div></div>","PeriodicalId":240,"journal":{"name":"Analytica Chimica Acta","volume":"1331 ","pages":"Article 343338"},"PeriodicalIF":5.7,"publicationDate":"2024-10-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142439636","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":"Towards high throughput analysis using 96-well plate solid phase extraction to determine sedatives and β-blocker residues in food control monitoring","authors":"Ane Arrizabalaga-Larrañaga,&nbsp;Dieke van Doorn,&nbsp;Saskia S. Sterk","doi":"10.1016/j.aca.2024.343335","DOIUrl":"10.1016/j.aca.2024.343335","url":null,"abstract":"<div><h3>Background</h3><div>Veterinary drugs are widely used in animal production to prevent infections and treat diseases but, this may cause a risk to consumers. Due to the high number of food samples required to monitor yearly, simple, fast, sensitive and selective analytical methods are needed in control laboratories to ensure consumers safety. Nevertheless, many analytical methodologies available in these laboratories include multiple steps and therefore are time-consuming and hinder the analysis throughput requiring significant amounts of solvents and reagents.</div></div><div><h3>Results</h3><div>This work developed a 96-well plate solid phase extraction (SPE) method for the extraction of seven sedatives and a β-blocker in animal kidney by ultra-high-performance liquid chromatography coupled to tandem mass spectrometry (UHPLC−MS/MS). The developed method was validated based on Implementing Regulation (EU) 2021/808 in kidney, meat and fish. The performance characteristics of the validation (1–5 μg kg⁻¹) showed good linearity (R² &gt; 0.998) while decision limits (CCα) were between 1 and 1.2 μg kg⁻¹. Trueness and precision were determined at three levels (n = 7) and the results showed values ranging from 85 to 103 % and from 1 to 9 %, respectively. The feasibility of the method was demonstrated for the residue control requirement established by EU. Method was applied to 201 samples of kidney, meat and fish.</div></div><div><h3>Significance</h3><div>This study is the first to present an optimized and validated holistic method for sedatives and β-blocker using 96-well plate SPE and UHPLC−MS/MS. The method showed good performance in kidney, meat and fish samples being an universal method for any species along the same type of sample. The fast, easy, efficient, reliable and universal method showed high throughput and so reduced the analysis time by nine-fold and the required solvent amount by four times fulfilling the green chemistry principals.</div></div>","PeriodicalId":240,"journal":{"name":"Analytica Chimica Acta","volume":"1331 ","pages":"Article 343335"},"PeriodicalIF":5.7,"publicationDate":"2024-10-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142431802","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}

{"title":"Integrated strategy for high-confident global profiling of the histidine phosphoproteome","authors":"Shiyi Li ,&nbsp;Lei Li ,&nbsp;Mengran Ma ,&nbsp;Meining Xing ,&nbsp;Xiaohong Qian ,&nbsp;Wantao Ying","doi":"10.1016/j.aca.2024.343336","DOIUrl":"10.1016/j.aca.2024.343336","url":null,"abstract":"<div><h3>Background</h3><div>Histidine phosphorylation (pHis) plays a key role in signal transduction in prokaryotes and regulates tumour initiation and progression in mammals. However, the pHis substrates and their functions are rarely known due to the lack of effective analytical strategies.</div></div><div><h3>Results</h3><div>Herein, we provide a strategy for unbiased enrichment and assignment of the pHis peptides. First, the entire procedure was designed under alkaline conditions to maintain the stability of the N–P bond of pHis and high-pH reverse-phase chromatography was used to efficiently separate the pHis peptides. Second, exploiting the coelution benefits of diethyl labelling, the ratios of light- and heavy-labelled peptides were accurately quantified, and the sites of phosphorylated histidine were assigned. Finally, Cu-IDA bead enrichment and data-independent acquisition mass spectrometry analysis were used to improve the coverage of the histidine phosphoproteome. With this novel strategy, 768 and 1125 potential pHis peptides were identified from lysates of <em>E. coli</em> and HeLa cells, respectively. And these values represent the highest coverage of the histidine phosphoproteome for both cell types.</div></div><div><h3>Significance</h3><div>These data strongly support the presumption that pHis modifications are widely present in bacteria. The study provides an efficient strategy and can lead to a better understanding of pHis-modified substrates and their biological functions.</div></div>","PeriodicalId":240,"journal":{"name":"Analytica Chimica Acta","volume":"1331 ","pages":"Article 343336"},"PeriodicalIF":5.7,"publicationDate":"2024-10-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142430449","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":"High-precision analysis of toxic metals in lithium-ion battery materials across various complex media","authors":"Tianyu Qi ,&nbsp;Xuezhi Yang ,&nbsp;Ya Liu ,&nbsp;Haonan Wen ,&nbsp;Feiyang Liu ,&nbsp;Ziqi Yue ,&nbsp;Ziyuan Qi ,&nbsp;Haiyan Zhang ,&nbsp;Jianjie Fu ,&nbsp;Qian Liu ,&nbsp;Guibin Jiang","doi":"10.1016/j.aca.2024.343334","DOIUrl":"10.1016/j.aca.2024.343334","url":null,"abstract":"<div><h3>Background</h3><div>Present regulations regarding the management and recycling of spent Lithium-ion batteries (LIBs) are inadequate, which may lead to the pollution of lithium (Li) and heavy metals in water and soil during the informal disposal of such batteries. To comprehend the distribution of toxic metals within spent LIBs and contaminated environmental media, precise analytical methods for toxic metals in these materials are crucial. However, due to the chemical complexity of LIBs materials (e.g., lithium iron phosphate, graphite, separators, and electrolytes), there is still a lack of research on developing and validating analytical techniques for toxic metals in LIB materials across various environmental media.</div></div><div><h3>Results</h3><div>This study establishes a comprehensive and highly precise analytical method for assessing toxic metal constituents in LIBs across various complex media, including sewage, soil, and biological matrices. We assessed the selection of digestion solutions for different LIB materials and identified the most suitable internal standard elements in the mass spectrometric analysis workflow. The devised digestion schemes for all components of LIBs are as follows: aqua regia for all cathode materials (excluding LiMn_0.6Fe_0.4PO₄ (LMFP)), nitric acid for diaphragm materials, aqua regia with hydrofluoric acid for the anode material Li₄Ti₅O₁₂ (LTO), and NaOH fusion for graphite and LMFP. LiPF₆ electrolyte can be directly dissolved in ultrapure water. By employing this method, the analysis of cathode materials of LIBs within diverse environmental matrices (sewage, soil, plants, animals) yields recovery rates ranging from 83.6 % to 115.5 %. Furthermore, this research reveals the remarkable accumulation of Li and heavy metals in anode (graphite) of spent LIBs.</div></div><div><h3>Significance</h3><div>This is the first to develop and validate analytical techniques for toxic metals in LIB materials across various environmental media, incorporating both acid digestion and alkaline fusion techniques. This methodology offers comprehensive support for conducting environmental risk assessments of spent LIBs. Using this method, the research elucidates the occurrence characteristics of toxic metals within different parts of commercial spent LIBs, providing valuable insights to enhance recycling efforts and facilitate risk management of spent LIBs.</div></div>","PeriodicalId":240,"journal":{"name":"Analytica Chimica Acta","volume":"1331 ","pages":"Article 343334"},"PeriodicalIF":5.7,"publicationDate":"2024-10-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142430470","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":"Mass-tagged self-assembled nanoprobe reveals the transport of PD-L1 from cancer cells to tumor-educated platelets","authors":"Jianhua Zhu ,&nbsp;Wenjun Zhang ,&nbsp;Zhongcheng Wang ,&nbsp;Yan Wang ,&nbsp;Jiapu Li ,&nbsp;Yunjing Wang ,&nbsp;Feifei Xu ,&nbsp;Yun Chen","doi":"10.1016/j.aca.2024.343312","DOIUrl":"10.1016/j.aca.2024.343312","url":null,"abstract":"<div><h3>Background</h3><div>The expression level of immune checkpoint proteins detected by tissue biopsy is currently used as a predictive biomarker for immune checkpoint blockade (ICB) therapy. However, tissue biopsy is susceptible to invasive sample collection procedures, significant sampling heterogeneity, and the difficulty of repeated sampling. Therefore, liquid biopsy of blood samples is becoming an alternative choice for immune checkpoint protein detection. Among various vesicles in blood, platelets can obtain cancer information to form a specific group called tumor-educated platelets (TEPs). The platelet-derived proteins in TEPs may have a predictive potential in ICB therapy.</div></div><div><h3>Results</h3><div>In this study, a photo-cleavable mass-tagged self-assembled (SAMT) nanoprobe with signal amplification was developed for the quantitative detection of PD-L1. The SAMT probe was assembled by photo-cleavable mass tags, PD-L1 aptamer, and amphiphilic polymer. After binding with PD-L1 on the platelet, the probe can release mass tags with UV light exposure. The amount of the mass tag, representing that of PD-L1, was subsequently determined by mass spectrometry. The assay sensitivity can be greatly improved by up to four orders of magnitude, achieving a detection limit of 10 fM. This assay was subsequently applied to cancer cells and platelet samples from non-small cell lung cancer (NSCLC) patients. The patients with higher tumor stages, higher degrees of lymph node invasion, and better ICB response had higher PD-L1 levels on platelets. Further investigation revealed that PD-L1 on the platelets was transported from cancer cells, providing evidence for the existence of TEPs.</div></div><div><h3>Significance</h3><div>The SAMT probe can amplify the signal of the target molecule into that of multiple mass tags, achieving ultrasensitive ICB protein quantitative detection in platelets. Moreover, the employed SAMT assay not only revealed PD-L1 transport from cancer cells to platelets but also confirmed the presence of TEPs.</div></div>","PeriodicalId":240,"journal":{"name":"Analytica Chimica Acta","volume":"1331 ","pages":"Article 343312"},"PeriodicalIF":5.7,"publicationDate":"2024-10-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142405415","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}