Analytical Chemistry最新文献

{"title":"Bridging Indigenous Ways of Knowing with Western Science Pedagogy in STEM Education.","authors":"Genievieve C Borg,Teresa Kumblathan","doi":"10.1021/acs.analchem.5c02421","DOIUrl":"https://doi.org/10.1021/acs.analchem.5c02421","url":null,"abstract":"","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"138 1","pages":"10097-10098"},"PeriodicalIF":7.4,"publicationDate":"2025-05-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144097825","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Digital SERS Nanostructured Platform for Amplification-free Single-Molecule DNA Detection and Pre-Symptomatic Diagnosis of Kiwifruit Soft Rot.","authors":"Jinai Chen,Yujiao Wei,Liming Wang,Leyi Chen,Shengnan He,Honglin Liu","doi":"10.1021/acs.analchem.5c01686","DOIUrl":"https://doi.org/10.1021/acs.analchem.5c01686","url":null,"abstract":"We present a digital surface-enhanced Raman spectroscopy (SERS) platform enabling enzyme- and amplification-free single-molecule DNA detection through Poisson distribution-driven quantification and geometrically optimized plasmonic nanostructures. Utilizing high-throughput UV lithography, we fabricated large-area nanopillar arrays (1.5 × 1.5 cm) with tunable heights (500-1300 nm) and periodicities (4-10 μm), addressing key limitations in conventional SERS methods via three innovations: (1) dynamic hotspot generation: Target DNA induces plasmonic dimerization between functionalized gold nanoprobes and Au-capped nanopillars, creating spatially resolved SERS enhancement (1326 cm-1 DTNB signal), (2) digital counting algorithms: Compensate Raman intensity variations by quantifying activated pillars as discrete molecular events, and (3) geometric confinement: Spatial confinement effects enabling statistically robust single-molecule occupancy. This platform achieved 10 fM sensitivity for Diaporthe spp. DNA detection, outperforming PCR-electrophoresis (1 pM) by 2 orders of magnitude. Applied to presymptomatic kiwifruit diagnosis, the system identified pathogen DNA in asymptomatic samples prior to visual symptom development, validated by characteristic DTNB peaks (1326 cm-1) absent in negative controls. The modular design permits multiplexed detection through probe diversification, while the absence of enzymatic steps enables field-deployable operation. By integrating single-molecule statistics with plasmonic signal amplification, this work establishes a robust framework for precision molecular diagnostics, demonstrating transformative potential for agricultural pathogen surveillance and low-abundance biomarker analysis. The technology's batch-producible nanopillar architecture and digital quantification strategy overcome longstanding reproducibility challenges in SERS-based detection, positioning it as a versatile tool for next-generation biosensing applications.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"1 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-05-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144103528","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Constructing Built-In Electric Field in Hierarchical-Flower Heterostructure for High-Performance Serum Metabolic Assay.","authors":"Tao Ning,Penglong Cao,Jun Yang,Tianrun Xu,Di Yu,Ting Li,Ting Wang,Chunxiu Hu,Xinyu Liu,Xianzhe Shi,Guowang Xu","doi":"10.1021/acs.analchem.5c01100","DOIUrl":"https://doi.org/10.1021/acs.analchem.5c01100","url":null,"abstract":"Laser desorption ionization mass spectrometry (LDI-MS) is a critical platform for high-throughput nontargeted metabolomics analysis in clinical diagnosis. However, traditional organic matrices inherently suffer from background interference in the low-mass range and exhibit low sensitivity for small molecule detections. Heterostructure has been regarded as an effective structure for high charge carrier mobility and tunable band gaps, which can enhance ion transfer efficiency and photothermal conversion during the LDI-MS process. In this work, Fe3O4/MoS2 nanoparticles with hierarchical-flower heterostructure were facilely synthesized as a novel matrix of LDI-MS to enhance the detection of serum metabolic profilings (SMPs), which was further applied for the early diagnosis of lung cancer. The heterostructure of Fe3O4/MoS2 can construct a built-in electric field to inhibit electron-hole recombination. Additionally, its abundant defect structures synergistically accelerate interfacial charge transfer, thereby promoting desorption and ionization processes. As a result, the newly developed Fe3O4/MoS2 nanomatrix demonstrated exceptional performance in LDI-MS, significantly surpassing the conventional matrices by at least 1 order of magnitude. Subsequently, information-rich SMPs were successfully obtained from merely 1 μL of serum. More than 90% of the metabolic features exhibited RSDs below 30% in quality control samples, highlighting the high reproducibility of our method for clinical applications. Furthermore, hundreds of lung cancer patients and healthy controls can be clearly distinguished based on their SMPs by using appropriate machine learning models. Finally, two key metabolites associated with lung cancer were identified as potential biomarkers, which showed promising diagnostic capability with an AUC value of 0.824 in the validation set. Taken together, Fe3O4/MoS2 nanoparticles emerge as a promising nanomatrix with superior LDI efficiency and the developed LDI-MS platform proves to be a powerful tool for serum metabolic profiling, offering significant potential for lung cancer diagnosis.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"14 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-05-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144103829","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"A Robust Biosensor Based on Dual Loop Constrained Antifouling Peptide for Electrochemical Detection of Human Insulin like Growth Factor 1 in Blood.","authors":"Baoping Zhu,Yang Li,Wenqing Wang,Shujie Cheng,Rui Han,Xiliang Luo","doi":"10.1021/acs.analchem.5c01274","DOIUrl":"https://doi.org/10.1021/acs.analchem.5c01274","url":null,"abstract":"Human insulin-like growth factor 1 (IGF-1) levels in human blood serve as a reliable biomarker for assessing endogenous growth hormone secretion and are also implicated in the pathogenesis of various cancers, highlighting their broad clinical diagnostic value. However, the direct detection of IGF-1 in complex blood samples with electrochemical biosensors is challenging due to the severe biofouling and the enzymes in the blood that may cause degradation of biomolecules functionalized on the sensor surfaces. Herein, a dual-loop constrained antifouling peptide (DLC-AP) was designed and constructed through the covalent cyclization of linear antifouling peptides, and it was further used for the development of an antifouling electrochemical biosensor. The DLC-AP exhibited exceptional antifouling properties in complex biological media, and its structural stability against enzymatic degradation by proteolytic enzymes in blood significantly enhanced the stability and antifouling performance of the biosensor. The DLC-AP-based biosensor demonstrated high sensitivity for IGF-1 detection in human blood samples, achieving a linear response range of 0.1 pM to 100.0 nM with a low limit of detection (7.0 fM), and its assay results of IGF-1 levels in clinical blood samples showed agreement with the ELISA results. This strategy of peptide and biosensor design offers a promising avenue for the construction of antifouling biosensing devices for biomarker monitoring in complex human blood.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"131 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-05-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144103802","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Pericyte Biomarkers for Ischemic Stroke: Potential and Prospects.","authors":"Wendi Wang,Qing Han,Tianwei Wang,Jian Liu,Qingbin Ni,Jingyi Sun,Ying Wang,Baoliang Sun","doi":"10.1021/acs.analchem.5c00142","DOIUrl":"https://doi.org/10.1021/acs.analchem.5c00142","url":null,"abstract":"Ischemic stroke (IS) has a high mortality rate. Multiplexed detection of IS core biomarkers is of great significance to early diagnosis and personalized treatment of IS patients. Whether pericytes, a key component of the neurovascular unit and blood-brain barrier located on the capillary wall, could serve as a promising biomarker for IS is to be explored. Herein, we observed a significant upregulation of inflammatory and apoptotic factors, such as MMP9, in pericytes subjected to in vitro ischemia. By transfecting pericytes with ASK1-shRNA to inhibit ASK1 expression, we noted reduced levels of inflammatory and apoptotic markers, including MMP9, as well as enhanced pericyte contraction and migration, thereby preserving the integrity of the blood-brain barrier. Additionally, ELISA assays conducted using plasma samples from patients with varying NIHSS scores revealed statistically significant concentrations of PDGFRβ and MMP9. Furthermore, we developed a highly sensitive and specific quantitative detection method for PDGFRβ and MMP9 based on fluorescence sensor technology. This novel detector exhibits high sensitivity, repeatability, and stability, enabling precise dual detection. Thus, the results suggest the great potential of the detection of PDGFRβ and MMP9 for early diagnosis of IS and prognosis prediction of the disease.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"18 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-05-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144103803","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Dual-Signal Probing of Molecular Subtypes of Breast Cancer: Synergistic Chirality and Charge-Transfer Effect Enable Enhanced Accuracy.","authors":"Xiaomei Mo,Huacheng Li,Xiang Zhong,Meng Li,Menghui Jia,Hongwei Wu,Xiaoran Li,Tao Yi,Chunyan Li,Xiang Lan","doi":"10.1021/acs.analchem.5c01620","DOIUrl":"https://doi.org/10.1021/acs.analchem.5c01620","url":null,"abstract":"Tumor molecular subtyping is essential for guiding personalized treatment strategies. However, existing detection methods are constrained by complex procedures, prolonged processing times, and high costs. Therefore, the development of rapid and straightforward detection methods remains a critical unmet need. Here, we employed DNA nanotechnology to construct a series of fluorophore-coupled pairs (a chiral BODIPY (cBDP) and a cyanine), revealing intermolecular interactions via various spectroscopic measurements and identifying a pair with unique charge and chirality transfer properties. By the integration of the fluorophore pair as a probe into DNA circuit systems, it can achieve amplification of dual optical signals of circular dichroism (CD) and fluorescence through DNA cascade reaction-controlled dissociation and the formation of the probe. For the practical implementation, we applied this dual-signal detection system for breast cancer molecular subtyping, which proved to successfully detect key biomarkers, estrogen receptor (ER), and human epidermal growth factor receptor 2 (HER2), within 1 h. The receptor-specific spectral responses enabled the rapid classification of four breast cancer molecular subtypes. Particularly, the synergistic effect of charge and chirality transfer proved to contribute to the enhancement of the detection accuracy. Given its versatility and precision, this platform shows significant promise for tumor molecular subtyping and offers potential applications in clinical biomarker detection and personalized therapy.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"44 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-05-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144097814","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Multiplexed Detection of Pancreatic-Specific Nucleic Acids and Protein Biomarkers Using a Logic Nanofluidic Platform.","authors":"Lina Wang,Yixin Jia,Jin Wang,Xing-Hua Xia,Chen Wang","doi":"10.1021/acs.analchem.5c01978","DOIUrl":"https://doi.org/10.1021/acs.analchem.5c01978","url":null,"abstract":"Early detection of pancreatic cancer is vital for patient survival. However, current diagnostic approaches remain constrained by insufficient precision and specificity inherent to single-biomarker detection strategies. Herein, we develop a nanochannel biosensing platform implementing cooperative dual-signal detection of pancreatic-specific biomarkers CA19-9 and miRNA-196a. Using liquid-liquid interface self-assembly, we constructed anodic aluminum oxide (AAO)-Au hybrid nanochannels integrated with a surface-modified double-key DNA nanolock (DDN). The conformational switch of DDN logic gating triggered by miRNA-196a exposes the CA19-9-aptamer, enabling specific target recognition and consequent ion current signal attenuation. Simultaneously, released miRNA-196a is quantified by catalytic hairpin assembly and hybridization chain reaction-mediated cascade amplification. Experiments show that the present DDN-based logic nanofluidic platform could achieve an ultralow detection limit of 0.000027 U·mL-1 for CA19-9 and 4.74 aM for miRNA-196a, which is 2-3 orders of magnitude higher than traditional ELISA/qPCR methods. Finally, clinical sample analysis confirms the high specificity of this platform in distinguishing pancreatic cancer and acute pancreatitis from healthy individuals. This DDN-functionalized nanofluidic biosensor provides valuable insights into designing precision detection platforms for pancreatic cancer, highlighting its significant potential for clinical diagnostics.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"17 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-05-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144087761","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Detection of Protein Polysulfidation Using a β-(4-Hydroxyphenyl)ethyl Iodoacetamide-Derived Biotin Tag HPB.","authors":"Yuping Xin,Xinyue Zhang,Qingda Wang,Longyang Dian,Yongzhen Xia,Luying Xun,Huaiwei Liu","doi":"10.1021/acs.analchem.5c00712","DOIUrl":"https://doi.org/10.1021/acs.analchem.5c00712","url":null,"abstract":"Protein polysulfidation (Pr-SnH, n ≥ 2) is a type of post-translational modification that plays multiple physiological functions. Detecting Pr-SnH remains challenging due to the high reactivity of -SnH groups and their similarity to other thiol-based modifications. Here, we report the development of a new biotinylated tag, HPB, which is derived from β-(4-hydroxyphenyl)ethyl iodoacetamide (HPE-IAM). HPB demonstrates superior performance over the traditional iodoacetamide (IAM)-derived biotin tag IAB, especially in minimizing off-target alkylation and preserving polysulfide chains. After protocol optimization, we achieved a 73.3% accuracy rate in proteomic scale Pr-SnH detection. Further, we found that polysulfides can modify other amino acids besides cysteine, including histidine, phenylalanine, and tryptophan, by introducing -SH or -SSH groups into their heterocyclic/phenyl rings. This leads to the detection accuracy rate of all current methods being less than 100%. Nonetheless, this study provides a reliable tool for detecting protein polysulfidation from complex cellular backgrounds.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"53 89 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-05-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144087763","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"A Digital Microfluidic Platform for the Microscale Production of Functional Immune Cell Therapies.","authors":"Samuel R Little, Niloufar Rahbari, Mehri Hajiaghayi, Fatemeh Gholizadeh, Fanny-Mei Cloarec-Ung, Joel Phillips, Hugo Sinha, Alison Hirukawa, David J H F Knapp, Peter J Darlington, Steve C C Shih","doi":"10.1021/acs.analchem.4c06911","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c06911","url":null,"abstract":"<p><p>Genetically engineering human immune cells has been shown to be an effective approach for developing novel cellular therapies to treat a wide range of diseases. To expand the scope of these cellular therapies while solving persistent challenges, extensive research and development is still required. Here we use a digital microfluidic enabled electroporation system (referred to as triDrop) specifically designed to mitigate harm during electroporation procedures and compare against two state-of-the-art commercially available systems for the engineering of primary human T cells. We describe the ability to use triDrop for highly efficient transfection with minimal reagent consumption while preserving a healthy transcriptomic profile. Finally, we show for the first time the ability to use a digital microfluidic platform for the miniaturized production of Chimeric Antigen Receptor (CAR) T cell therapies demonstrating how this novel system can lead to a 2-fold improvement in immunotherapeutic functionality compared to gold standard methods while providing up to a 20-fold reduction in cost. These results highlight the potential power of this system for automated, rapid, and affordable next-generation cell therapy R&D.</p>","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":" ","pages":""},"PeriodicalIF":6.7,"publicationDate":"2025-05-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144100966","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Electrochemiluminescence Biosensor Based on an Efficient Antifouling Cell Membrane Hydrogel for the Direct Detection of Alkaline Phosphatase in Human Serum and Cell Lysate.","authors":"Qiongwei Wu,Zhengjun Dong,Fan Geng,Jia Wang,Xianzhen Song,Caifeng Ding","doi":"10.1021/acs.analchem.5c00432","DOIUrl":"https://doi.org/10.1021/acs.analchem.5c00432","url":null,"abstract":"Electrochemiluminescence (ECL) biosensors are an ideal choice for the real-time and sensitive detection of biomarkers. However, there are many interfering biomolecules in human serum or cell lysate that can affect the ECL signal through nonspecific interface adsorption. To solve this issue, an efficient ECL antifouling biosensor based on a red blood cell membrane (RBCM) hydrogel was developed for the direct detection of alkaline phosphatase (ALP) in human serum and cell lysate. Among them, the RBCM hydrogel was prepared by embedding the purified RBCM vesicles into [1,2-distearoyl-sn-glycerol-3-phosphoethanolamine]-[polyethylene]-[acrylamide] (DSPE-PEG-AM), which endowed the antifouling interface with high stability and biocompatibility. Meanwhile, compared to RBCM, the constructed RBCM hydrogel improved the electron transfer rate of the antifouling interface. Furthermore, luminescent copper nanosheets (Cu NSs) and quencher MnO2 NSs were encapsulated in the RBCM hydrogel, which greatly reduced the distance between Cu NSs and MnO2 NSs, thereby effectively improving the signal quenching efficiency. In the presence of ALP, l-ascorbic acid 2-phosphate trisodium salt was hydrolyzed to ascorbic acid, thus disrupting the structure of MnO2 NSs to restore the ECL signal. Based on the above sensing strategies, the constructed ECL biosensor achieved an ultrasensitive detection of ALP with a wide linear range (10-5 to 104 U·L-1) and a detection limit as low as 3.4 × 10-6 U·L-1 (3δ/k), demonstrating potential application value in clinical diagnosis.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"8 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-05-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144087764","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}