Analytical Chemistry最新文献

Profiling of Biofluid Metabolites with a Kinetically Differentiated Binary Biosensing Platform

IF 7.4 1区化学

Analytical Chemistry Pub Date : 2025-02-26 DOI: 10.1021/acs.analchem.4c03404

Bing Qi, Ziyun Miao, Jiahui Tan, Yingqian Wang, Jie Wang

{"title":"Profiling of Biofluid Metabolites with a Kinetically Differentiated Binary Biosensing Platform","authors":"Bing Qi, Ziyun Miao, Jiahui Tan, Yingqian Wang, Jie Wang","doi":"10.1021/acs.analchem.4c03404","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c03404","url":null,"abstract":"Biofluid metabolites have a crucial linkage with the health of the human body, and developing a universal method for metabolite monitoring is imperative for disease diagnosis and health management. Herein, we report a kinetically differentiated binary biosensing platform that is specifically responsive to NAD(P)H for profiling diverse biofluid metabolites. The kinetically differentiated binary biosensing platform comprises a cyanine derivative dye with fast reaction kinetics and a quinolinium derivative dye with slow reaction kinetics. Compared to the traditional unitary strategy for NAD(P)H detection, the linear range of the binary biosensing platform is widened by up to 20 times. NAD(P)H are ubiquitous cofactors in living systems, and metabolite production generally involves the consumption or generation of NAD(P)H. Thus, biofluid metabolites can be easily quantified by measuring the variation of NAD(P)H concentration during biochemical reactions with the binary biosensing platform. In this study, serum sorbitol, 2-hydroxybutyric acid (2HB), and α-ketoglutarate (AKG) were all quantified by the binary biosensing platform with accuracies higher than 93%. The kinetically differentiated binary biosensing platform can be extended to the analysis of any molecule that can react directly or indirectly with NAD(P)H. In addition, we constructed a paper-based assay with the binary biosensing platform, and the test papers showed good promise in the point-of-care (POC) profiling of biofluid metabolites. This study proposes a simple strategy to expand the calibration range of traditional unitary detection systems and further provides a universal paradigm for high throughput profiling of disease-associated biomolecules, which offers good promise in disease diagnosis and health management.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"10 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-02-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143496116","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

Single-Use Electrochemical Aptamer-Based Sensors for Calibration-Free Measurements in Human Saliva via Dual-Frequency Approaches: Prospects and Challenges

IF 7.4 1区化学

Analytical Chemistry Pub Date : 2025-02-26 DOI: 10.1021/acs.analchem.4c06802

Yasmin Liu, Rishi Pandey, Mary Jane McCarthy, Onyekachi Raymond

{"title":"Single-Use Electrochemical Aptamer-Based Sensors for Calibration-Free Measurements in Human Saliva via Dual-Frequency Approaches: Prospects and Challenges","authors":"Yasmin Liu, Rishi Pandey, Mary Jane McCarthy, Onyekachi Raymond","doi":"10.1021/acs.analchem.4c06802","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c06802","url":null,"abstract":"Despite the rapid growth in aptamer-based biosensor research, there remains a significant demand for aptasensors that operate without the need for sample preparation and calibration, to better facilitate real-world applications. Electrochemical aptamer-based (EAB) sensors, particularly those utilizing a dual-frequency, calibration-free approach, have shown promising advances toward commercialization. Single-use, disposable sensors represent a cost-effective solution for at-home and on-site point-of-care (POC) diagnostics. However, the development of these sensors presents unique challenges compared to in vivo monitoring and reusable platforms, with pronounced variations across sensors and batches. Motivated by these challenges, we have comprehensively investigated the dual-frequency, calibration-free approach, focusing on sensor-to-sensor and batch-to-batch variations. Our research explored the use of a nonresponsive frequency-based ratiometric method for detecting cocaine with laser-ablated, disposable EAB sensors. Additionally, to overcome the absence of nonresponsive frequencies in some aptasensors, we developed strategies to modify the aptamer structure and optimize operational conditions, effectively tailoring nonresponsive frequencies to allow for rapid result turnover. Moreover, we assessed the effects of various filter types on saliva pretreatment using liquid chromatography with tandem mass spectrometry (LCMS/MS) and developed a saliva collection workflow using an oral swab. This workflow and the disposable aptasensors developed herein achieved low μM sensitivity in saliva, with results obtainable in under 5 min, including saliva collection and processing. Furthermore, our findings indicate that certain food and drink residues in saliva can compromise sensor accuracy, highlighting an area for future refinement.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"6 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-02-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143496120","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

Trends in Pharmaceutical Analysis: The Evolving Role of Liquid Chromatography

IF 7.4 1区化学

Analytical Chemistry Pub Date : 2025-02-26 DOI: 10.1021/acs.analchem.4c06662

Valentina D’Atri, Rodell C. Barrientos, Gioacchino Luca Losacco, Serge Rudaz, Arnaud Delobel, Erik L. Regalado, Davy Guillarme

引用次数: 0

GLASSR-Net: Glass Substrate Spectral Restoration Neural Network for Fourier Transform Infrared Microspectroscopy in the Fingerprint Region

IF 7.4 1区化学

Analytical Chemistry Pub Date : 2025-02-26 DOI: 10.1021/acs.analchem.4c06805

Xiangyu Zhao, Jingzhu Shao, Yudong Tian, Zhiqiang Gui, Ping Tang, Qinyu Li, Zhihong Wang, Chongzhao Wu

{"title":"GLASSR-Net: Glass Substrate Spectral Restoration Neural Network for Fourier Transform Infrared Microspectroscopy in the Fingerprint Region","authors":"Xiangyu Zhao, Jingzhu Shao, Yudong Tian, Zhiqiang Gui, Ping Tang, Qinyu Li, Zhihong Wang, Chongzhao Wu","doi":"10.1021/acs.analchem.4c06805","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c06805","url":null,"abstract":"Fourier transform infrared (FTIR) microspectroscopy has emerged as a pivotal pathological tool, offering informative spectral biomarkers for numerous diseases. However, the dependency on specialized infrared (IR) substrates limits effective and widespread clinical translation. IR transparent bases like calcium/barium fluoride (CaF2/BaF2) are costly and fragile, while IR reflective bases cannot be used for microscopic screening due to their opacity to visible light. In comparison, 1 mm thick pathological glass substrates are cost-effective, reliable, and widely utilized in clinical pathology. Therefore, establishing a methodology for collecting high-quality FTIR spectra on glass substrates is highly desired and beneficial. Here, we develop a glass substrate spectral restoration neural network (GLASSR-Net) to restore the fingerprint absorbance spectra from glass-based spectra spanning the wavenumbers from 1800 to 1000 cm–1. The model is trained and validated by acquiring input glass-based spectra and ground truth spectra, respectively, through FTIR raster scanning on contiguous tissue sections of papillary thyroid carcinoma (PTC) mounted on glass and CaF2 substrates. The GLASSR-Net successfully restores the sample absorbance and accurately reconstructs the biochemical distribution in both the spatial and spectral domains. Furthermore, the biochemical signatures of PTC are effectively extracted and analyzed from the restored spectra with traditional spectral histology, indicating a decrease in amide I/II absorption and an accumulation of lipids and nucleic acids in cancerous regions. The proposed GLASSR-Net presents a novel framework for data collection, spectral restoration, and integration of traditional methodology in glass-based IR microspectroscopy, which facilitates the incorporation of FTIR microspectroscopy into clinical histological scenarios.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"31 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-02-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143496121","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

Development of a Near-Infrared Probe for Enhancing Cancer Therapy by Mitigating Pyroptosis-Induced Inflammation

IF 7.4 1区化学

Analytical Chemistry Pub Date : 2025-02-26 DOI: 10.1021/acs.analchem.4c07048

Bin Li, Weikang Peng, Zhihang Jin, Shusheng Zhang, Lei Yang, Mingming Yu, Zhanxian Li

{"title":"Development of a Near-Infrared Probe for Enhancing Cancer Therapy by Mitigating Pyroptosis-Induced Inflammation","authors":"Bin Li, Weikang Peng, Zhihang Jin, Shusheng Zhang, Lei Yang, Mingming Yu, Zhanxian Li","doi":"10.1021/acs.analchem.4c07048","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c07048","url":null,"abstract":"Pyroptosis, a specialized cell death mechanism crucial in cancer therapy, is distinct from apoptosis and primary necrosis. It is linked to inflammation and reactive oxygen species, particularly peroxynitrite (ONOO–), which is implicated in disease. Monitoring pyroptosis is challenging due to its connection with cellular polarity and the tumor environment. In this research, we developed a near-infrared probe, PBQI, which is highly sensitive and responsive to polarity and ONOO– fluctuations. PBQI targets mitochondria and lipid droplets, enabling real-time tracking of pyroptosis-associated subcellular alterations. It was found to differentiate between normal and cancer cells during pyroptosis triggered by cisplatin and metformin. To mitigate pyroptosis-induced inflammation, disulfiram was used as an inhibitor, significantly alleviating excessive inflammation. This study highlights PBQI’s utility in studying the interplay between polarity, ONOO–, and pyroptosis, and contributes to the development of more targeted cancer therapies that optimize pyroptosis’s antitumor benefits while minimizing inflammatory side effects.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"51 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-02-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143496124","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 FT-ICR MS and Machine Learning to Forecast Acid Content Across Boiling Cuts

IF 7.4 1区化学

Analytical Chemistry Pub Date : 2025-02-26 DOI: 10.1021/acs.analchem.4c04522

Jussara V. Roque, Wilson J. Cardoso, Deborah V. A. de Aguiar, Gabriel F. dos Santos, Alexandre de O. Gomes, Iris Medeiros Júnior, Gesiane da S. Lima, Boniek Gontijo

{"title":"Integrating FT-ICR MS and Machine Learning to Forecast Acid Content Across Boiling Cuts","authors":"Jussara V. Roque, Wilson J. Cardoso, Deborah V. A. de Aguiar, Gabriel F. dos Santos, Alexandre de O. Gomes, Iris Medeiros Júnior, Gesiane da S. Lima, Boniek Gontijo","doi":"10.1021/acs.analchem.4c04522","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c04522","url":null,"abstract":"In this study, we introduce a pioneering approach that leverages advanced machine learning and ultrahigh-resolution Fourier transform ion cyclotron mass spectrometry (FT-ICR MS) data to predict the distribution of the total acid number (TAN) in true boiling point (TBP) distillation cuts from crude oil. By employing partial least-squares (PLS) regression and ordered predictor selection (OPS), we achieved robust predictive models with high accuracy, evidenced by low root-mean-square error of calibration (RMSEC) and strong correlation coefficients (Rc). Our analysis of 36 diverse crude oil samples revealed significant variations in chemical composition, with nitrogen- and oxygen-containing compounds playing key roles in influencing TAN values. Through the use of volcano plots, we identified critical molecular classes that drive changes in TAN. The predictive models demonstrated remarkable consistency between predicted and actual TAN values, particularly in samples with a higher TAN, further validating their reliability. Significantly, our method overcomes the limitations of traditional ASTM testing by requiring smaller sample volumes while still providing accurate TAN predictions. This novel approach offers a powerful new tool for the molecular characterization and behavioral forecasting of complex mixtures, enabling a more efficient pathway for sample analysis when resources are limited.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"15 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-02-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143496118","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

Optimization of the Entropy-Based Wavelet Method for Removing Strong RF and AC Interferences in a Charge Detection Linear Ion Trap Mass Spectrometer

IF 7.4 1区化学

Analytical Chemistry Pub Date : 2025-02-26 DOI: 10.1021/acs.analchem.4c06069

Minh Cong Dang, Avinash A. Patil, Thị Khánh Ly Lại, Szu-Wei Chou, Trang Kieu Thi Hoang, Mhar Ian Cua Estayan, Wen-Ping Peng

{"title":"Optimization of the Entropy-Based Wavelet Method for Removing Strong RF and AC Interferences in a Charge Detection Linear Ion Trap Mass Spectrometer","authors":"Minh Cong Dang, Avinash A. Patil, Thị Khánh Ly Lại, Szu-Wei Chou, Trang Kieu Thi Hoang, Mhar Ian Cua Estayan, Wen-Ping Peng","doi":"10.1021/acs.analchem.4c06069","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c06069","url":null,"abstract":"We developed an entropy-based wavelet method to effectively remove interference from strong radio frequency (RF) and auxiliary alternating current (AC) fields in a linear ion trap (LIT) mass spectrometer coupled to a charge sensing particle detector (CSPD). By optimizing the energy-to-Shannon entropy, we identified the optimal mother wavelet family and decomposition level and determined suitable threshold values based on the median of sub-band coefficients at each decomposition level. These thresholds were applied as rigid criteria across all decomposition levels to eliminate noise interferences and avoid the arbitrary choice of the threshold. This entropy wavelet-based method successfully denoised high-mass protein mass spectra, achieving significant improvements in signal-to-noise ratio (S/N) for immunoglobulin G (IgG) and alpha-2-macroglobulin (A2M) ions, with increases of 68.03% and 81.73%, respectively. Our method surpasses previously reported baseline correction techniques, such as orthogonal wavelet packet decomposition (OWPD) filtering, and enhances the sensitivity of LIT mass spectrometry (LIT-MS) in analyzing high-mass protein ions.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"25 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-02-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143496119","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

Structural Annotation Method for Locating sn- and C═C Positions of Lipids Using Liquid Chromatography–Electron Impact Excitation of Ions from Organics (EIEIO)–Mass Spectrometry

IF 7.4 1区化学

Analytical Chemistry Pub Date : 2025-02-26 DOI: 10.1021/acs.analchem.4c05560

Yao Chen, Jun Yang, Xinxin Wang, Yuqing Zhang, Yaping Shao, Hang Li, Xiaoyan Dong, Fei Jiang, Chunxiu Hu, Guowang Xu

{"title":"Structural Annotation Method for Locating sn- and C═C Positions of Lipids Using Liquid Chromatography–Electron Impact Excitation of Ions from Organics (EIEIO)–Mass Spectrometry","authors":"Yao Chen, Jun Yang, Xinxin Wang, Yuqing Zhang, Yaping Shao, Hang Li, Xiaoyan Dong, Fei Jiang, Chunxiu Hu, Guowang Xu","doi":"10.1021/acs.analchem.4c05560","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c05560","url":null,"abstract":"Definitive structural elucidation of lipids is pivotal for unraveling the functions of lipids in biological systems. Despite advancements in mass spectrometry (MS) for lipid analysis, challenges in annotation scope and efficiency remain, especially in resolving isomers. Herein, we introduce an optimized method using liquid chromatography coupled with electron impact excitation of ions from organic tandem mass spectrometry (LC-EIEIO-MS/MS) for comprehensive analysis and structural annotation of lipids. This approach integrates a six-step analytical protocol for precise lipid annotation, including (1) extracting MS information, (2) classifying lipids, (3) aligning sum composition, (4) determining sn-positions, (5) locating C═C positions, and (6) ascertaining annotation levels. In analyzing 34 lipid standards spiked into serum, our method achieved 100% and 82.4% annotation accuracy at the sn- and C═C isomer levels, respectively, compared to 26.5% and 0% in the CID mode using MS-DIAL. A total of 1312 sn-positions and 1033 C═C locations of lipids were annotated in quality control plasma pooled from healthy individuals and patients with Alzheimer’s disease. The isomers of lipids revealed more pronounced differences between the healthy and diseased groups compared to the sum compositions of the lipids. Overall, the LC-EIEIO-MS/MS approach provides a comprehensive profiling and efficient annotation method for lipidomics, promising to shed new light on lipid-related biological pathways and disease mechanisms.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"28 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-02-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143496126","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

Measurement of Real-Time Serotonin Dynamics from Human-Derived Gut Organoids

IF 7.4 1区化学

Analytical Chemistry Pub Date : 2025-02-26 DOI: 10.1021/acs.analchem.4c06033

Bettina Bohl, Yuxian Lei, Gavin A. Bewick, Parastoo Hashemi

{"title":"Measurement of Real-Time Serotonin Dynamics from Human-Derived Gut Organoids","authors":"Bettina Bohl, Yuxian Lei, Gavin A. Bewick, Parastoo Hashemi","doi":"10.1021/acs.analchem.4c06033","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c06033","url":null,"abstract":"The importance of the gut in regulating the brain–body immune axis is becoming increasingly evident. Interestingly, the brain and gut share many common signaling molecules, with serotonin being one of the most notable. In fact, the gut is the primary source of serotonin in the body. However, studying serotonin dynamics in a human-specific context remains a challenge. Human stem cell-derived models provide a promising avenue for studying signal transmission in well-controlled, in vitro environments. In this study, we report the first fast-scan cyclic voltammetry (FSCV) measurements of serotonin signaling in a newly developed enterochromaffin cell (ECC)-enriched gut organoid model. First, we characterize the stem cell-derived gut organoids and confirm they are enriched with ECCs, the key cell type responsible for producing and releasing serotonin in the gut. We then optimize an in vitro buffer that maintains cell viability while supporting FSCV measurements. Using this system, we detect spontaneous release events, which increase in frequency and amplitude following stimulation with forskolin (FSK) and 3-isobutyl-1-methylxanthine (IBMX). Finally, we confirm the identity of the signal as serotonin using a selective serotonin reuptake inhibitor (SSRI), which significantly delayed the reuptake profile. Our study introduces the first real-time measurement of serotonin signaling in a human-derived gut model. We believe this system will be essential for future research on serotonin’s role in the gut and for potential novel drug target identification.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"52 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-02-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143496122","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

Analysis of the Human Scent on Fired Cartridge Cases from a Simulated Crime Scene.

IF 6.7 1区化学

Analytical Chemistry Pub Date : 2025-02-25 Epub Date: 2025-02-14 DOI: 10.1021/acs.analchem.4c06231

Ulrika Malá, Václav Vokálek, Pavel Vrbka, Jana Čechová, Petra Pojmanová, Oleksii Kaminskyi, Veronika Škeříková, Štěpán Urban

引用次数: 0