Analytical Chemistry最新文献_第2页

Dual-Enhanced Lateral Flow Immunoassay: Synergizing Oriented Antibody Anchoring and Nanozyme Catalytic Amplification for Ultrasensitive Cancer Detection. 双增强横向流动免疫测定：协同定向抗体锚定和纳米酶催化扩增用于超灵敏癌症检测。

IF 7.4 1区化学

Analytical Chemistry Pub Date : 2025-07-31 DOI: 10.1021/acs.analchem.5c02403

Qing Yang,Wanchao Zuo,Jiaren Song,Siqi Zeng,Xiangming Meng,Zhipeng Ding,Qiannan Hu,Xuhui Tan,Donghui Zhang,Jianjun Dai,Yanmin Ju

{"title":"Dual-Enhanced Lateral Flow Immunoassay: Synergizing Oriented Antibody Anchoring and Nanozyme Catalytic Amplification for Ultrasensitive Cancer Detection.","authors":"Qing Yang,Wanchao Zuo,Jiaren Song,Siqi Zeng,Xiangming Meng,Zhipeng Ding,Qiannan Hu,Xuhui Tan,Donghui Zhang,Jianjun Dai,Yanmin Ju","doi":"10.1021/acs.analchem.5c02403","DOIUrl":"https://doi.org/10.1021/acs.analchem.5c02403","url":null,"abstract":"Conventional lateral flow immunoassays (LFIAs) suffer from limited sensitivity in detecting low-abundance tumor biomarkers, primarily attributed to inefficient antibody utilization and insufficient signal intensity of nano-immunoprobes. Here, we propose a dual-enhanced LFIA integrating oriented antibody anchoring and nanozyme catalytic amplification for ultrasensitive visual detection of tumor biomarkers, denoted as DEOAN-LFIA. Bimetallic catalyst gold-platinum nanoparticles (Au@Pt NPs) were functionalized with phenylboronic acid to selectively orient antibodies via fragment crystallizable (Fc) glycans for improving antibody utilization efficiency, thereby enriching target-probe complexes on the test line (T line), realizing the first-step signal amplification. Subsequently, the elevated local concentration of Au@Pt NPs efficiently catalyzed the conversion of chromogenic substrates into colored products, further amplifying the signal from enriched probes on the T line for the second-step signal amplification. Using common tumor markers alpha-fetoprotein (AFP) and carcinoembryonic antigen (CEA) as model targets, DEOAN-LFIA achieved ultrasensitive detection of picogram-level targets (50 pg/mL for AFP and 10 pg/mL for CEA) with rapid analysis within 25 min. Clinical validation with 36 human serum samples demonstrated favorable concordance with the standard clinical assay. This DEOAN-LFIA platform provides a robust ultrasensitive point-of-care tool for the early diagnosis of malignant diseases.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"27 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-07-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144747801","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}

引用次数: 0

Multiscale Synergistic SERS Chiral Detection: Gold Nanoclusters-Mediated Enantioselective Molecular Discrimination on the Self-Assembly of Gold Nanoparticles. 多尺度协同SERS手性检测：金纳米团簇介导的金纳米粒子自组装对映选择性分子识别。

IF 7.4 1区化学

Analytical Chemistry Pub Date : 2025-07-31 DOI: 10.1021/acs.analchem.5c02859

Yanan Wu,Yuqing Yang,Rui Wang,Haifeng Yang,Xinling Liu

{"title":"Multiscale Synergistic SERS Chiral Detection: Gold Nanoclusters-Mediated Enantioselective Molecular Discrimination on the Self-Assembly of Gold Nanoparticles.","authors":"Yanan Wu,Yuqing Yang,Rui Wang,Haifeng Yang,Xinling Liu","doi":"10.1021/acs.analchem.5c02859","DOIUrl":"https://doi.org/10.1021/acs.analchem.5c02859","url":null,"abstract":"Surface-enhanced Raman scattering (SERS), despite its high sensitivity in molecular fingerprint detection, typically lacks chiral specificity. Chiral metal nanoclusters (CMNCs) with sub-3 nm cores hold promise for chiral molecular sensing, yet their application in SERS-based chiral recognition remains largely unexplored. In this study, two-dimensional self-assembly of Au nanoparticles (NPs, 30 ∼ 50 nm) functionalized with D- or L-penicillamine (Pen) stabilized sub-3 nm Au nanoclusters (NCs) were constructed as SERS-active substrates. On these substrates, distinct SERS signals were observed for L- versus D-phenylalanine (Phe) enantiomers, with a signal intensity difference of approximately 5-fold at a low concentration of 10-6 mol/L, suggesting a good enantiomeric discrimination effect and detection sensitivity. Similar chiral discrimination phenomena were also found by using propranolol enantiomers or chiral Cu NCs. These findings demonstrate the significant potential of the integration of CMNCs into plasmonic SERS substrates for developing sensitive chiral sensing strategies based on nonchiral vibrational Raman spectroscopy and advancing the fundamental studies of metal nanocluster-molecule chiral interactions.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"27 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-07-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144748090","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}

引用次数: 0

Advanced Extracellular Vesicle Isolation: A Hybrid Electrokinetic-Tangential Flow Filtration Approach for Improved Yield, Purity, and Scalability. 先进的细胞外囊泡分离：一种混合电动-切向流过滤方法，以提高产量，纯度和可扩展性。

IF 6.7 1区化学

Analytical Chemistry Pub Date : 2025-07-30 DOI: 10.1021/acs.analchem.5c01168

YongWoo Kim, SoYoung Jeon, KangMin Lee, Sehyun Shin

{"title":"Advanced Extracellular Vesicle Isolation: A Hybrid Electrokinetic-Tangential Flow Filtration Approach for Improved Yield, Purity, and Scalability.","authors":"YongWoo Kim, SoYoung Jeon, KangMin Lee, Sehyun Shin","doi":"10.1021/acs.analchem.5c01168","DOIUrl":"https://doi.org/10.1021/acs.analchem.5c01168","url":null,"abstract":"As extracellular vesicles (EVs) become increasingly important in diagnostics and therapeutics, achieving both improved purity and yield during isolation remains a critical challenge. Conventional techniques often suffer from the coisolation of nonvesicular particles and soluble proteins, limiting their clinical and research utility. In response, we introduce ExoTFF, a hybrid isolation technology that sequentially integrates electrokinetic filtration (ExoFilter) with size-exclusion tangential flow filtration (TFF) to deliver unprecedented performance gains through an iterative, synergistic mechanism. In the ExoTFF system, the sample is repeatedly circulated through an electrokinetic mesh filter and TFF until the liquid is removed. This recirculating flow gradually eliminates contaminants, while the electrokinetic filter continuously captures EVs as the sample is purified. Finally, any residual impurities in the TFF unit are completely removed via a dead volume elimination process. The complementary actions of these two distinct separation mechanisms double EV recovery rates and reduce impurity levels by 80% compared to conventional TFF, culminating in an impressive 800% improvement in the purity ratio. In proof-of-concept experiments, ExoTFF processed 10 mL of plasma within 10 min, efficiently depleting albumin and high-density lipoprotein (HDL) while achieving superior EV recovery. To further explore scalability, an automated ExoTFF system processed 500 mL of sample in 50 min, maintaining consistent yield and purity. The ability to sustain performance across different scales highlights ExoTFF's potential for both laboratory research and industrial-level EV production. Beyond biological applications, this platform also offers broad applicability for the isolation of negatively charged nanoparticles, demonstrating its potential impact across multiple nanotechnology-driven fields.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":" ","pages":""},"PeriodicalIF":6.7,"publicationDate":"2025-07-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144740622","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}

引用次数: 0

Integrating Fluorogenic DNAzymes with Photonic Crystals for Bacterial Detection on a Microfluidic Biochip. 集成荧光DNAzymes与光子晶体的微流控生物芯片细菌检测。

IF 7.4 1区化学

Analytical Chemistry Pub Date : 2025-07-30 DOI: 10.1021/acs.analchem.5c02447

Rui Zhang,Chen An,Jiuxing Li,Xiaozheng Li,Qiang Zhang,Qing'an Li,Shen Li,Bo Wang,Xiaoqian Li,Yangyang Chang,Zijie Zhang,Meng Liu

引用次数: 0

Adduct-Induced Variability in Tandem Mass Spectrometry. 串联质谱法中加合物诱导的变异。

IF 7.4 1区化学

Analytical Chemistry Pub Date : 2025-07-30 DOI: 10.1021/acs.analchem.5c02792

Botao Liu,Zhifeng Tang,Tao Huan

{"title":"Adduct-Induced Variability in Tandem Mass Spectrometry.","authors":"Botao Liu,Zhifeng Tang,Tao Huan","doi":"10.1021/acs.analchem.5c02792","DOIUrl":"https://doi.org/10.1021/acs.analchem.5c02792","url":null,"abstract":"Tandem mass spectrometry (MS/MS) provides essential structural information and plays a central role in compound annotation in metabolomics. While different precursor ion types are expected to influence the generation of MS/MS spectra, systematic investigations into precursor ion type-dependent MS/MS variability have been limited. To address this gap, we analyzed over half a million MS/MS spectra of 24,686 unique compounds from the NIST 20 spectral library, covering a broad range of precursor ion types and collision energies (CEs). Using [M + H]+ and [M - H]- spectra as references, we found that alkali cation adducted species such as [M + Na]+ and [M + K]+ exhibited distinct fragmentation behavior and low spectral similarity, likely due to the distinct nature of the alkali charge carriers, which do not promote protonated fragmentation pathways but instead stabilize the precursor ion through coordination. In contrast, [M + NH4]+, [2M + H]+, [M + H - H2O]+, [M + Cl]-, [2M - H]-, and [M - H - H2O]- showed moderate to high similarity to their references, as they often undergo neutral losses that generate [M + H]+ or [M - H]-, or are themselves derived from these ions. Our study also observed that fragmentation is structure-driven at lower CE and energy-driven at higher CE. This pattern allows for a higher spectral similarity among different precursor ion types at high CE. However, [2M + H]+ or [2M - H]- showed reduced similarity at higher CE, likely because the same amount of energy is distributed across more bonds in these larger precursor ions, resulting in less energy per bond. Finally, we demonstrated that ignoring precursor ion types can compromise compound annotation, including spectral library searches, molecular networking, and machine learning model development. Overall, this study underscores the critical influence of precursor ion types on MS/MS spectra and highlights the need for precursor-ion-type-aware strategies in metabolite annotation, which has been largely overlooked in the metabolomics field.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"6 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-07-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144737238","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}

引用次数: 0

Reconstructing Super-Resolution Raman Spectral Image Using a Generative Adversarial Network-Based Algorithm. 基于生成对抗网络的超分辨率拉曼光谱图像重建算法。

IF 7.4 1区化学

Analytical Chemistry Pub Date : 2025-07-30 DOI: 10.1021/acs.analchem.5c02934

Jie Xu,Haorui An,Xiangtao Kong,Zixuan Zhang,Qidong Liu,Jie Li,Jie Qin,Ivan A Bratchenko,Shuang Wang

{"title":"Reconstructing Super-Resolution Raman Spectral Image Using a Generative Adversarial Network-Based Algorithm.","authors":"Jie Xu,Haorui An,Xiangtao Kong,Zixuan Zhang,Qidong Liu,Jie Li,Jie Qin,Ivan A Bratchenko,Shuang Wang","doi":"10.1021/acs.analchem.5c02934","DOIUrl":"https://doi.org/10.1021/acs.analchem.5c02934","url":null,"abstract":"Raman imaging utilizes molecular fingerprint information to visualize the spatial distribution of a substance within the scanned area. Subject to its scanning mechanism, it usually costs a prolonged data acquisition duration for achieving high-resolution Raman images. In this study, we propose a generative adversarial network (GANs) based algorithm to significantly enhance both the Raman spectral imaging speed and spatial resolution. The proposed method was trained and evaluated on 186 hyperspectral Raman datasets acquired from unlabeled cells, and its reconstruction performance was quantitatively evaluated by the parameters of peak signal-to-noise ratio (PSNR), structural similarity index (SSIM), and root-mean-square error (RMSE). Univariate imaging and K-means clustering analysis (KCA) were both adopted to evaluate the preservation of biochemical information after image reconstructing. The results demonstrated that the proposed method effectively enhances spatial resolution by a factor of 2-4 while accelerating imaging speed by a factor of 4-16. Furthermore, transfer learning was utilized to adapt the pretrained model to different objects, validating its generalization capabilities and extending its universalities. This study highlighted the potential of deep learning for super-resolution Raman imaging, providing a promising pathway for high-throughput and real-time biochemical analysis.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"68 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-07-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144737239","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}

引用次数: 0

Top-Down Proteomics for the Characterization and Quantification of Calreticulin Arginylation. 自上而下蛋白质组学用于钙网蛋白精氨酸化的表征和定量。

IF 6.7 1区化学

Analytical Chemistry Pub Date : 2025-07-29 Epub Date: 2025-06-26 DOI: 10.1021/acs.analchem.4c04141

Richard M Searfoss, Xingyu Liu, Benjamin A Garcia, Zongtao Lin

{"title":"Top-Down Proteomics for the Characterization and Quantification of Calreticulin Arginylation.","authors":"Richard M Searfoss, Xingyu Liu, Benjamin A Garcia, Zongtao Lin","doi":"10.1021/acs.analchem.4c04141","DOIUrl":"10.1021/acs.analchem.4c04141","url":null,"abstract":"Arginylation installed by arginyltransferase 1 (ATE1) features an addition of arginine (Arg) to the reactive amino acids (e.g., Glu and Asp) at the protein N-terminus or side chain. Systemic removal of arginylation after ATE1 knockout (KO) in mouse models resulted in heart defects leading to embryonic lethality. The biological importance of arginylation has motivated the discovery of arginylation sites on proteins using bottom-up approaches. While bottom-up proteomics is powerful in localizing peptide arginylation, it lacks the ability to quantify proteoforms at the protein level. Here we developed a top-down proteomics workflow for characterizing and quantifying calreticulin (CALR) arginylation. To generate fully arginylated CALR (R-CALR), we have inserted an R residue after the signaling peptide (AA1-17). Upon overexpression in ATE1 KO cells, CALR and R-CALR were purified by affinity purification and analyzed by LCMS in positive mode. Both proteoforms showed charge states ranging from 27 to 68 with charge 58 as the most intense charge state. Their MS2 spectra from electron-activated dissociation (EAD) showed preferential fragmentation at the protein N-terminals which yielded sufficient c ions facilitating precise localization of the arginylation sites. The calcium-binding domain (CBD) gave minimum characteristic ions possibly due to the abundant presence of >100 D and E residues. Ultraviolet photodissociation (UVPD) compared with EAD and ETD significantly improved the sequence coverage of CBD. This method can identify and quantify CALR arginylation at absence, endogenous (low), and high levels. To our knowledge, our work is the first application of top-down proteomics in characterizing post-translational arginylation in vitro and in vivo.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":" ","pages":"15562-15569"},"PeriodicalIF":6.7,"publicationDate":"2025-07-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144493143","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}

引用次数: 0

From Spectra to Structure: AI-Powered ³¹P NMR Interpretation. 从光谱到结构：人工智能驱动的31P核磁共振解释。

IF 6.7 1区化学

Analytical Chemistry Pub Date : 2025-07-29 Epub Date: 2025-07-16 DOI: 10.1021/acs.analchem.5c01460

Marvin Alberts, Nina Hartrampf, Teodoro Laino

引用次数: 0

Prioritizing Chemical Candidates from Non-targeted Analysis Using Metadata, Spectral Similarity, and Hazard Scoring within INTERPRET NTA. 在INTERPRET NTA中使用元数据、光谱相似性和危险评分对非目标分析中的候选化学物质进行优先排序。

IF 6.7 1区化学

Analytical Chemistry Pub Date : 2025-07-29 Epub Date: 2025-07-16 DOI: 10.1021/acs.analchem.5c02223

Alex Chao, Jeffrey M Minucci, Troy M Ferland, E Tyler Carr, Greg Janesch, Safia Rizwan, Heather D Whitehead, Tommy Cathey, Shirley Pu, Laura D Brunelle, Angela L Batt, Jon R Sobus, Antony J Williams

{"title":"Prioritizing Chemical Candidates from Non-targeted Analysis Using Metadata, Spectral Similarity, and Hazard Scoring within INTERPRET NTA.","authors":"Alex Chao, Jeffrey M Minucci, Troy M Ferland, E Tyler Carr, Greg Janesch, Safia Rizwan, Heather D Whitehead, Tommy Cathey, Shirley Pu, Laura D Brunelle, Angela L Batt, Jon R Sobus, Antony J Williams","doi":"10.1021/acs.analchem.5c02223","DOIUrl":"10.1021/acs.analchem.5c02223","url":null,"abstract":"New approach methodologies like non-targeted analysis (NTA) are increasingly relevant for identifying and monitoring emerging contaminants. Utilizing high-resolution mass spectrometry (HRMS), NTA methods can detect and annotate chemicals without prior knowledge. Yet, NTA results often have associated uncertainties owing, in part, to a lack of standardized methods. To address this challenge, the US Environmental Protection Agency (US EPA) developed the Interface for Processing, Reviewing, and Translating NTA data (\"INTERPRET NTA\") to support NTA research within its Office of Research and Development (ORD). Previous work demonstrated INTERPRET NTA's capabilities for reviewing and reporting NTA data quality. The current work highlights additional functionalities for retrieving and interpreting chemical results. INTERPRET NTA accesses chemical data from multiple US EPA resources, including (1) chemical metadata from US EPA's Analytical Methods and Open Spectra (AMOS) database, (2) predicted spectra for ∼1.2 million chemical substances within US EPA's DSSTox database, and (3) hazard values from US EPA's Cheminformatics Hazard Module (CHM). De facto water reuse study data with 77 known chemicals were used to demonstrate INTERPRET NTA functions and capabilities. Known chemicals showed higher values for metadata, MS2, and hazard scores in 99.0%, 80.5%, and 92.0% of cases, respectively, compared to false positives. Interactive visualizations within INTERPRET NTA facilitate the visual integration of chemical results, highlighting chemical candidates of greatest interest, and allowing review of underlying data. INTERPRET NTA is being prepared for public release, offering researchers a tool for defensible and efficient review and reporting of NTA study results.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":" ","pages":"15904-15912"},"PeriodicalIF":6.7,"publicationDate":"2025-07-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144647961","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}

引用次数: 0

Correction to "Nanoconfined Electrokinetic Chromatography (NEC): Gradient Separation and Sensing of Short DNA Fragments at the Single-Molecule Level". 修正“纳米限电色谱法（NEC）：单分子水平上短DNA片段的梯度分离和传感”。

IF 6.7 1区化学

Analytical Chemistry Pub Date : 2025-07-29 Epub Date: 2025-07-18 DOI: 10.1021/acs.analchem.5c03864

Jian Lv, Xue Wu, Mansha Wu, Xiaoyuan Wang, Lijuan Gong, Dawei Li, Ruocan Qian

引用次数: 0