João Flávio da Silveira Petruci, Danielle da Silva Sousa, Boris Mizaikoff
{"title":"Advanced Mid-Infrared Sensors for Molecular Analysis","authors":"João Flávio da Silveira Petruci, Danielle da Silva Sousa, Boris Mizaikoff","doi":"10.1021/acs.analchem.4c06799","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c06799","url":null,"abstract":"Published as part of <i>Analytical Chemistry</i> special issue “Fundamental and Applied Reviews in Analytical Chemistry 2025”. Figure 1. (a) Representation of a typical setup of an ATR-based spectrometer. Panels (b–d) shows schematics of a planar waveguide composed of a layer of sample (e.g., analyte-containing solution, solid, etc.) (nc), a waveguiding layer (nwg), and a substrate layer (ns) (i.e., in case of a thin-film substrate-supported waveguide structure) with nwg > ns, nc: (b) the guided radiation propagates via total internal reflections along a zigzag path through the waveguide; (c) as the thickness of the waveguide decreases, the number of internal reflections increases; and (d) if the thickness is on the order of magnitude of the wavelength, individual reflections no longer adequately describe the propagation behavior of the wavefront. The evanescent field appears continuously along the entire waveguide surface. [Reproduced from ref (9). Copyright 2016, American Chemical Society, Washington, DC.] Figure 2. Illustration of common thin-film waveguide geometries: (a) slab waveguide, (b) strip waveguide, (c) rib waveguide, (d) slab waveguide, (e) ridge waveguide, and (f) embedded/buried waveguide. The same functional layers are marked with the same colors: green = waveguide layer (nc), pink = optical buffer layer (nb), and yellow = substrate (ns). [Adapted from ref (50). Copyright 2022, MDPI.] Figure 3. Panels (a–h) show scanning electronic microscopy (SEM) images of some representative hollow-core photonic crystal fibers (HC-PCFs). (a) Commercially available hollow core photonic bandgap fiber (HC-PBGF): HC-1550–02 was from NKT Photonics. [Reproduced (b) HC-PCF designed for the guiding in the MIR region; (c) hollow core Bragg fiber; (d) Kagome lattice HC-PCF; (e) hollow core antiresonant fibers (HC-ARF); (f) nodeless HC-ARF; (g) hollow fiber with negative curvature of the core wall]; and (h) double antiresonant hollow square core fiber. [Panel (a) was reproduced with permission from ref (101). Copyright 2020, MDPI.] (i) Schematic diagram of the proposed HC-PBGF based gas sensor. [Reprinted with permission from ref (100). Copyright 2021.] Figure 4. (a) Schematic illustration of the experimental setup for a broadband MIR femtosecond laser system (red line: laser source beam; yellow dashed line: globar radiation; OAPM: off-axis parabolic mirror; orange line: attenuated light after sample interaction MCT detector: mercury cadmium telluride detector). (b and c) Linear correlation between the integrated peak area and the concentration ranging from 0.08 to 10% of two independent ethanol measurements with their calculated linear regression equation, coefficient of determination (<i>R</i><sup>2</sup>), and LOD and LOQ values. [Reproduced from ref (106). Copyright 2023, American Chemical Society, Washington, DC.] Figure 5. Cross-sectional view of (a) iHWG and (b) the MOX gas cell. IR absorption spectra of 1000 and 100 ppm of CH<sub>4</sub> with ","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"25 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-03-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143723637","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}
Jing Li, Jiao Hu, An-An Liu, Cui Liu, Dai-Wen Pang
{"title":"Quantum Dots for Chemical Metrology","authors":"Jing Li, Jiao Hu, An-An Liu, Cui Liu, Dai-Wen Pang","doi":"10.1021/acs.analchem.4c06794","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c06794","url":null,"abstract":"This article has not yet been cited by other publications.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"4 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-03-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143723638","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":"Correction to “A Nanofluorescent Probe for Evaluating the Fluctuation of Aminopeptidase N in Nonalcoholic Fatty Liver Disease and Hepatic Fibrosis”","authors":"Xiao Sun, Xinlei Wang, Lili Fu, Xiaoyan Wang, Lingxin Chen, Yan Huang","doi":"10.1021/acs.analchem.5c01684","DOIUrl":"https://doi.org/10.1021/acs.analchem.5c01684","url":null,"abstract":"Figure 6. (a) Establishment process of hepatic fibrosis model mice. (b) Imaging APN levels in mouse models of hepatic fibrosis. Control group: no treatment for 6 weeks. 3-week group: no treatment for the first 3 weeks, and subcutaneous injection of oil solution (CCl<sub>4</sub>:olive oil = 1:4) with 20% CCl<sub>4</sub> by volume fraction at 5 mL/kg body weight every 3 days for 3 weeks. 6-week group of mice were stimulated with CCl<sub>4</sub> for 6 weeks consecutively in the same way as the 3-week group. Mice in the CCl<sub>4</sub> + bestatin group were stimulated with After 6 weeks of continuous stimulation with CCl<sub>4</sub>, mice in the CCl<sub>4</sub> + bestatin group were pretreated with bestatin (100 μmol/L in saline) for 1 h prior to incubation of the probes. (c) Isolated organ fluorescence imaging (heart, liver, spleen, kidneys, and lungs). (d) Pathology of H&E in different test groups. (e) The images’ mean fluorescence intensity (b). (f) Body-weight changes. (****<i>p</i> < 0.0001.) Scale bar = 20 μm. This article has not yet been cited by other publications.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"36 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-03-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143723880","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":"On-Chip Isolation and Reciprocal Signal Amplification Detection of Tumor-Derived Exosomes in Dual-Control Microfluidic Device","authors":"Junhe Ma, Kexin Li, Zhaofan Duan, Xuexin Yang, Guodong Zhou, Sujuan Ye","doi":"10.1021/acs.analchem.5c00426","DOIUrl":"https://doi.org/10.1021/acs.analchem.5c00426","url":null,"abstract":"The detection of exosomes is critical for health monitoring and disease diagnosis. However, their small size and low concentration present significant challenges. In this study, we designed a dual-control microchip integrated with a surface-enhanced Raman scattering (SERS) signal amplification detection method. By employing separate chambers for isolation and detection, this method achieves magnetic separation control and DNA cascade signal amplification with electrokinetic enrichment detection. The magnetic separation step captures and isolates exosomes in a magnetic-controlled reaction chamber, releasing a signal-switching strand that translates exosome recognition into a DNA signal amplification process. The DNA cascade reciprocal signal amplification reaction is performed in an electrokinetic enrichment reaction chamber, significantly improving detection efficiency and signal intensity. In addition, absolute-value coupled data processing reduces background interference. These unique merits enable precise and highly efficient assay of exosomes. This dual-control microchip signal amplification sensor exhibits remarkable sensitivity, rapid detection times, with a detection limit of 10.9 particles/μL and a reaction time of 35 min, and successful application to real sample analysis. The platform offers a viable, accurate, and portable solution for medical point-of-care testing.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"130 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-03-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143723762","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":"Needle Trap Devices in Analytical Chemistry: A Critical Review of Development, Applications, and Future Perspectives","authors":"Nassiba Baimatova, Emanuela Gionfriddo","doi":"10.1021/acs.analchem.4c06984","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c06984","url":null,"abstract":"This article has not yet been cited by other publications.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"36 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-03-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143723772","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}
Shirou Feng, Hongyi Liu, Cong Zhou, Xiyue Xiong, Yingzhuang Chen, Ming Ma, Bo Chen
{"title":"Direct Corona Charging: A New Strategy for Enhancing Sensitivity and Stability in Charged Aerosol Detection","authors":"Shirou Feng, Hongyi Liu, Cong Zhou, Xiyue Xiong, Yingzhuang Chen, Ming Ma, Bo Chen","doi":"10.1021/acs.analchem.4c05557","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c05557","url":null,"abstract":"The charged aerosol detector (CAD) is widely used for detecting nonvolatile compounds without UV absorption due to its high sensitivity, stability, and consistent response. However, the traditional plasma collision charging mode (PCCM) suffers from issues such as sample dilution, gas flow back-mixing, and disturbances, which reduce sensitivity and repeatability. To address these limitations, this study introduces the direct corona charging mode (DCCM), which eliminates the charging gas route by using a high-voltage corona needle to directly charge the dried aerosol. This approach avoids mixing collisions, simplifies the instrument structure, and reduces nitrogen consumption. Comparative analyses using samples like caffeine demonstrated that DCCM significantly improves sensitivity and stability over PCCM. The response under DCCM fits a quadratic curve with a correlation coefficient above 0.99 across 3 orders of magnitude. Direct injection of 22 analytes showed that DCCM achieved a peak area relative standard deviation below 10%, with better response consistency than PCCM. Gradient analysis of complex samples further confirmed DCCM’s superior repeatability and sensitivity. Real-sample analysis highlighted DCCM-CAD’s practical potential. In summary, DCCM enhances CAD performance, reduces costs, and simplifies design, paving the way for more efficient and reliable commercial CAD systems.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"183 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-03-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143723769","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}
Wenkang Zhang, Xingyi Qi, Zhuo Mi, Han Wang, Shaojuan Lv, Yongfeng Song, Ping Su, Jiayi Song, Yi Yang
{"title":"A New Phosphorylated Protein Analysis Strategy based on Trypsin Encapsulated in Metal–Organic Frameworks with High Efficiency and a Simplified Workflow","authors":"Wenkang Zhang, Xingyi Qi, Zhuo Mi, Han Wang, Shaojuan Lv, Yongfeng Song, Ping Su, Jiayi Song, Yi Yang","doi":"10.1021/acs.analchem.5c00324","DOIUrl":"https://doi.org/10.1021/acs.analchem.5c00324","url":null,"abstract":"Phosphoproteomics research is crucial for clinical diagnosis. However, due to the self-hydrolysis of natural proteases and the complex typical pretreatment protocol, the traditional bottom-up method is not enough to achieve rapid analysis of phosphorylated proteins. In this work, we encapsulate trypsin (Try) in the ZIF-L(Co) to develop a new strategy that simplifies the phosphorylated protein analysis process and achieves rapid analysis. Try is encapsulated in the mesoporous ZIF-L(Co) to allow the proteins to be accessible to the enzymes. The hydrophobic ZIF-L(Co) can cause the unfolding of proteins and accelerates the digestion process. The Co(II) nodes enhance the affinity toward phosphorylated proteins and capture phosphopeptides selectively. Compared to the traditional denaturation, digestion, and enrichment method, which costs 20 h at least, our strategy simplifies the pretreatment workflow and yields phosphopeptides in just 3.4 h. This strategy is further applied in the analysis of phosphorylated proteins in biosamples such as nonfat milk, egg yolk, and human serum. The results show equivalent performance with the traditional method and exhibit great potential in bioanalysis. This new phosphorylated protein analysis strategy provides a powerful tool for proteomics analysis and promotes research in the field of biomedicine.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"212 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-03-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143713701","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":"Iridium Isotope Tag-Assisted LC-MS Method for Global Profiling and Quantification of Nonvolatile Serum Fatty Acids in Nonalcoholic Fatty Liver Mice","authors":"Yongcheng Dai, Beicheng Zhu, Xueting Yan, Xiaobo Xie, Zixuan Zhan, Yi Lv","doi":"10.1021/acs.analchem.4c05310","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c05310","url":null,"abstract":"Highly accurate and sensitive measurements of fatty acids (FAs) in biological samples are essential for advancing our understanding of their diverse biofunctions. In this work, based on the characteristic isotope pattern of iridium (<sup>191/193</sup>Ir), we employed an iridium-encoded amine (Ir-NH<sub>2</sub>) as the derivatization reagent to establish a selective and sensitive liquid chromatography–mass spectrometry (LC-MS) method for rapid identification and accurate quantification of FAs in biological samples. Upon derivatization, nonvolatile FAs were transformed into amide derivatives tagged with a charged iridium tag, exhibiting improved sensitivity and selectivity in the electrospray ionization (ESI) positive ion mode. By leveraging the unique 2.002 Da mass shift and the 3:5 peak intensity ratio from the natural <sup>191</sup>Ir and <sup>193</sup>Ir isotopes, we can rapidly and efficiently screen the potential carboxyl-containing metabolites from biological samples. Compared to other existing methods, our technique offers higher sensitivity, better signal-to-noise ratio, lower detection limit (1.2–8.4 pg/mL), and easier quantification due to the clear identification of iridium-tagged derivatives. With this method, a total of 58 FAs, including both saturated and unsaturated types, were detected in mice serum lipid extracts, with carbon chain lengths varying from C9 to C24. More importantly, this method was successfully employed for global profiling of nonvolatile serum FAs from mice with nonalcoholic fatty liver disease (NAFLD), providing a novel means for detecting them and offering new avenues for exploring their functional roles and disease associations.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"1 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-03-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143723768","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}
Roberto Rodriguez-Moncayo, Stephanie Pons, Luciana P. Tavares, Hyungkook Jeon, John-Alexander Preuss, Janina Bahnemann, Jongyoon Han, Bruce D. Levy, Joel Voldman
{"title":"Inertial Microfluidics Enables Functional Analysis of Neutrophils Isolated from Ultralow Blood Volume Samples","authors":"Roberto Rodriguez-Moncayo, Stephanie Pons, Luciana P. Tavares, Hyungkook Jeon, John-Alexander Preuss, Janina Bahnemann, Jongyoon Han, Bruce D. Levy, Joel Voldman","doi":"10.1021/acs.analchem.5c00102","DOIUrl":"https://doi.org/10.1021/acs.analchem.5c00102","url":null,"abstract":"Monitoring immune cell function is increasingly being recognized as a more relevant biomarker than traditional white blood cell counts, yet the need for repeated relatively large blood volumes still continues to pose a significant challenge. To overcome this, we developed a sample-sparing platform using inertial microfluidics that can process as little as 10 μL of blood to isolate leukocytes for downstream functional analysis. Our platform isolates leukocytes with ∼80% purity, >90% in-device recovery, and >95% viability. Neutrophils were our primary focus due to their sensitivity to external stimuli and their critical role in immune responses. Neutrophils isolated through our new method did not show inadvertent activation, as evidenced by unchanged expression of activation markers CD62L and CD11b, with phenotypes comparable to control cells in whole blood. We conducted a range of functional assays, including phagocytosis, ROS production, and NETosis with all tests confirming that neutrophils maintained their functionality after isolation. These assays were performed using standard laboratory workflows, demonstrating the platform’s compatibility with techniques such as flow cytometry and cell culture assays. Furthermore, we showed the versatility of our platform by successfully isolating leukocytes from challenging samples, including mouse blood from the vena cava or tail vein, as well as human capillary blood obtained by fingerstick. This adaptability highlights the potential of this platform for clinical and research applications, particularly in frequent immune monitoring or cases where sample volume is limited.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"183 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-03-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143713699","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}
Xingzhi Che, An T. H. Le, Maria Orlando, Svetlana M. Krylova, Vasily G. Panferov, Nikita A. Ivanov, Erez Freud, R. Shayna Rosenbaum, Sergey N. Krylov
{"title":"Addressing Hemolysis-Induced Loss of Sensitivity in Lateral Flow Assays of Blood Samples with Platinum-Coated Gold Nanoparticles and Machine Learning","authors":"Xingzhi Che, An T. H. Le, Maria Orlando, Svetlana M. Krylova, Vasily G. Panferov, Nikita A. Ivanov, Erez Freud, R. Shayna Rosenbaum, Sergey N. Krylov","doi":"10.1021/acs.analchem.4c07057","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c07057","url":null,"abstract":"Gold nanoparticles (GNPs), which appear red, are widely used as labels in lateral flow assays (LFAs) for visual detection. However, in blood-derived samples, hemolysis─caused by the rupture of red blood cells and the release of hemoglobin─creates a red-colored background that obscures the test line, significantly raising the limit of detection (LOD) and reducing the diagnostic sensitivity of LFAs. The degree of hemolysis can vary across samples due to differences in blood collection techniques, such as varying finger prick pressure, leading to inconsistent sensitivity. A practical solution to hemolysis-induced sensitivity loss should be easy for LFA manufacturers to implement without complicating the assay’s use. We propose modifying the color of GNPs from red to black by coating the nanoparticles with platinum, creating a platinum shell around a gold core (GNPs@Pt). This simple and cost-effective modification produces black nanoparticles, enhancing the contrast between the test line and background in hemolyzed samples. Using manual threshold-based image analysis, (scanning test strips and calculating the signal-to-noise ratio as a reference technique), we found that GNPs@Pt improved the LOD in LFAs of hemolyzed samples, with greater relative improvements observed at higher levels of hemolysis. In experiments assessing visual detection by human subjects, GNPs@Pt significantly outperformed standard GNPs; however, human accuracy in recognizing the test line was consistently lower than that achieved with threshold-based image analysis. To address the impracticality of manual threshold-based image analysis and the unreliability of visual detection, we developed a machine learning (ML) model for analyzing images of the LFA test strips. The integration of GNPs@Pt with ML-based image analysis achieved an assay LOD performance comparable to manual threshold-based image analysis, demonstrating 100% sensitivity and 100% specificity when benchmarked against the latter as a reference standard. Given the ease of substituting GNPs with GNPs@Pt, we recommend adopting this modification for assays involving blood samples. Additionally, we advocate using ML models, which can be integrated into mobile applications, as a standard readout tool for LFAs.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"41 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-03-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143723434","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}