Pub Date : 2024-11-21DOI: 10.1021/acs.analchem.4c05288
Xiaojun Li, Xiulei Qi, Xingguo Liu, Jun Zhu, Lianghai Hu
Outer membrane vesicles (OMVs) secreted by bacteria are emerging diagnostic markers for bacterial infection or disease detection due to their carriage of various signaling molecules. However, actual biological samples of patients are extremely complex, and applying OMVs to clinical diagnosis remains a major challenge. One of the major challenges is that there are still great difficulties in the enrichment of OMVs including tedious steps and lower concentration. And some commonly used exosome enrichment methods, such as ultracentrifugation, still have some shortcomings. Herein, we introduce lipopolysaccharide (LPS) molecularly imprinted polymer (MIP) for efficient capturing and analyzing OMVs, enabling a novel approach to bacterial disease diagnosis based on biorecognition materials. LPS, as a unique structure of Gram-negative bacteria, also widely expressed on the surface of OMVs, which will form cyclic hydrogen bonds with functional monomers of MIP with affinity interactions. The prepared MIP efficiently can isolate OMVs from 100 μL of culture broth via specific affinity LPS in less than 40 min with a recovery rate of over 95%. Moreover, MIP exhibits good reusability, with almost identical enrichment performance after 5 repeated cycles, contributing to reducing experimental costs in both time and economy. The captured OMVs can be detected using Western blotting with target protein antibodies or in combination with proteomic analysis, providing a proteomic biomarker platform for early bacteria disease diagnosis.
{"title":"Lipopolysaccharide Imprinted Polymers for Specific Recognition of Bacterial Outer Membrane Vesicles","authors":"Xiaojun Li, Xiulei Qi, Xingguo Liu, Jun Zhu, Lianghai Hu","doi":"10.1021/acs.analchem.4c05288","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c05288","url":null,"abstract":"Outer membrane vesicles (OMVs) secreted by bacteria are emerging diagnostic markers for bacterial infection or disease detection due to their carriage of various signaling molecules. However, actual biological samples of patients are extremely complex, and applying OMVs to clinical diagnosis remains a major challenge. One of the major challenges is that there are still great difficulties in the enrichment of OMVs including tedious steps and lower concentration. And some commonly used exosome enrichment methods, such as ultracentrifugation, still have some shortcomings. Herein, we introduce lipopolysaccharide (LPS) molecularly imprinted polymer (MIP) for efficient capturing and analyzing OMVs, enabling a novel approach to bacterial disease diagnosis based on biorecognition materials. LPS, as a unique structure of Gram-negative bacteria, also widely expressed on the surface of OMVs, which will form cyclic hydrogen bonds with functional monomers of MIP with affinity interactions. The prepared MIP efficiently can isolate OMVs from 100 μL of culture broth via specific affinity LPS in less than 40 min with a recovery rate of over 95%. Moreover, MIP exhibits good reusability, with almost identical enrichment performance after 5 repeated cycles, contributing to reducing experimental costs in both time and economy. The captured OMVs can be detected using Western blotting with target protein antibodies or in combination with proteomic analysis, providing a proteomic biomarker platform for early bacteria disease diagnosis.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"15 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2024-11-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142684917","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}
Pub Date : 2024-11-21DOI: 10.1021/acs.analchem.4c04284
Tong Wang, Shu Li, Run Mu, Zhengwei Lu, Jie Su, Jing Chen, Jinhua Zhan
Microplastics and nanoplastics are emerging contaminants that pose a threat to the environment and human. Spectroscopic technologies are advantageous in analyzing nanoplastics, but it is challenging to selectively detect nanoplastics with different size thresholds. In this work, the hyphenated method of electrosorption and surface-enhanced Raman spectroscopy (ES-SERS) was developed for the simple, rapid, and size-resolved analysis of trace polystyrene (PS) nanoplastics from 20 to 300 nm. A rough silver was used as both the working electrode for electrosorption and the substrate for the SERS response. By applying a positive electric potential to the rough silver, the PS nanoplastics accelerated toward the silver surface and were adsorbed tightly at the SERS “hot spot” inside the rough silver nanostructure. The proposed ES-SERS method achieved a detection limit of 100 ng/L for 300 and 100 nm PS, 50 ng/L for 50 nm PS, and 30 ng/L for 20 nm PS nanoplastics. It is worth noting that smaller nanoplastics typically exhibit larger analytical enhancement factor values in ES-SERS. According to the difference in electromigration behavior of PS in various sizes, PS nanoplastics under a certain size can be selectively enriched and detected by controlling the electrosorption time. The ES-SERS method was successfully demonstrated for detecting nanoplastics released from the lids of disposable beverage cups. This work opens up new possibilities for size-resolved analysis of nanoplastics.
{"title":"Size-Resolved SERS Detection of Trace Polystyrene Nanoplastics via Selective Electrosorption","authors":"Tong Wang, Shu Li, Run Mu, Zhengwei Lu, Jie Su, Jing Chen, Jinhua Zhan","doi":"10.1021/acs.analchem.4c04284","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c04284","url":null,"abstract":"Microplastics and nanoplastics are emerging contaminants that pose a threat to the environment and human. Spectroscopic technologies are advantageous in analyzing nanoplastics, but it is challenging to selectively detect nanoplastics with different size thresholds. In this work, the hyphenated method of electrosorption and surface-enhanced Raman spectroscopy (ES-SERS) was developed for the simple, rapid, and size-resolved analysis of trace polystyrene (PS) nanoplastics from 20 to 300 nm. A rough silver was used as both the working electrode for electrosorption and the substrate for the SERS response. By applying a positive electric potential to the rough silver, the PS nanoplastics accelerated toward the silver surface and were adsorbed tightly at the SERS “hot spot” inside the rough silver nanostructure. The proposed ES-SERS method achieved a detection limit of 100 ng/L for 300 and 100 nm PS, 50 ng/L for 50 nm PS, and 30 ng/L for 20 nm PS nanoplastics. It is worth noting that smaller nanoplastics typically exhibit larger analytical enhancement factor values in ES-SERS. According to the difference in electromigration behavior of PS in various sizes, PS nanoplastics under a certain size can be selectively enriched and detected by controlling the electrosorption time. The ES-SERS method was successfully demonstrated for detecting nanoplastics released from the lids of disposable beverage cups. This work opens up new possibilities for size-resolved analysis of nanoplastics.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"57 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2024-11-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142678848","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}
Pub Date : 2024-11-21DOI: 10.1021/acs.analchem.4c05728
Shuang Mu, Zhaowei Tian, Wei Ren, Chenghui Liu
Surface-enhanced Raman scattering (SERS) has emerged as a powerful tool for contamination detection. Fabricating efficient nanostructures with hotspots for signal enhancement and concentrating diluted target analyte molecules to the hotspots are critical for ultrasensitive SERS detection, which generally requires advanced instruments and intricate manipulations. Herein, we report a simple, low-cost, and high-efficiency paper device that can simultaneously concentrate the analytes and generate SERS hotspots rapidly with the assistance of laser-induced thermophoresis. After dropping the target- and plasmonic nanoparticle-containing solution on a paper substrate, the evaporative gradient created by the laser-induced thermophoresis can promote the delivery of the analytes and plasmonic nanoparticles simultaneously to the tiny area of the laser spot, forming compact SERS hotspots to significantly amplify the analyte’s Raman scattering signals. This convenient thermophoretic strategy can be accomplished rapidly within ∼4 min and exhibits more than 104-times higher sensitivity than that without the assistance of laser-based thermophoresis. This elegant paper device is successfully applied to the detection of contaminants such as pesticides and nanoplastics in fruit and water samples, holding the potential to provide a simple, fast, and cost-effective approach for on-site detection of environmental contaminants.
{"title":"Laser-Induced Thermophoretic SERS Enhancement on Paper for Facile Pesticide and Nanoplastic Sensing","authors":"Shuang Mu, Zhaowei Tian, Wei Ren, Chenghui Liu","doi":"10.1021/acs.analchem.4c05728","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c05728","url":null,"abstract":"Surface-enhanced Raman scattering (SERS) has emerged as a powerful tool for contamination detection. Fabricating efficient nanostructures with hotspots for signal enhancement and concentrating diluted target analyte molecules to the hotspots are critical for ultrasensitive SERS detection, which generally requires advanced instruments and intricate manipulations. Herein, we report a simple, low-cost, and high-efficiency paper device that can simultaneously concentrate the analytes and generate SERS hotspots rapidly with the assistance of laser-induced thermophoresis. After dropping the target- and plasmonic nanoparticle-containing solution on a paper substrate, the evaporative gradient created by the laser-induced thermophoresis can promote the delivery of the analytes and plasmonic nanoparticles simultaneously to the tiny area of the laser spot, forming compact SERS hotspots to significantly amplify the analyte’s Raman scattering signals. This convenient thermophoretic strategy can be accomplished rapidly within ∼4 min and exhibits more than 10<sup>4</sup>-times higher sensitivity than that without the assistance of laser-based thermophoresis. This elegant paper device is successfully applied to the detection of contaminants such as pesticides and nanoplastics in fruit and water samples, holding the potential to provide a simple, fast, and cost-effective approach for on-site detection of environmental contaminants.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"70 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2024-11-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142685042","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}
Carbohydrate antigen 19-9 is a well-known malignancy biomarker, and its sensitive detection is particularly crucial in the diagnosis and assessment of pancreatic cancer. In this study, an ultrasensitive CA19-9 immunosensor was constructed using the Zn2+-regulated CdSySe1–y (Zn-CdSySe1–y) nanospheres (NSs) as the electrochemiluminescence (ECL) emitter and FeCoS2 nano octahedrons (NOs) as a coreactant enhancer. The microstructure of ternary transition metal chalcogenide CdSySe1–y was precisely tuned by Zn2+ doping to avoid aggregation and thus enable stable and efficient cathodic ECL responses. The bimetallic sulfide FeCoS2 was synthesized using a metal organic framework (MOF) as the template by ion permeation. It was able to catalyze the coreactant efficiently due to the synergistic effect of the Fe2+ and Co2+. The immunosensor exhibited low detection limit (7.6 × 10–5 U mL–1) in the wide linear range of 0.0001–100 U mL–1, offering a sensitive CA19-9 detection method.
{"title":"A Dual-Ion Synergistic Catalysis Utilizing Zn2+-Regulated CdSySe1–y ECL Immunosensor Employed for the Ultrasensitive CA19-9 Detection","authors":"Dawei Fan, Zhengxing Gong, Guangyue He, Hanxiao Liu, Yingli Wang, Hongmin Ma, Dan Wu, Huan Wang, Qin Wei","doi":"10.1021/acs.analchem.4c05034","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c05034","url":null,"abstract":"Carbohydrate antigen 19-9 is a well-known malignancy biomarker, and its sensitive detection is particularly crucial in the diagnosis and assessment of pancreatic cancer. In this study, an ultrasensitive CA19-9 immunosensor was constructed using the Zn<sup>2+</sup>-regulated CdS<sub><i>y</i></sub>Se<sub>1–<i>y</i></sub> (Zn-CdS<sub><i>y</i></sub>Se<sub>1–<i>y</i></sub>) nanospheres (NSs) as the electrochemiluminescence (ECL) emitter and FeCoS<sub>2</sub> nano octahedrons (NOs) as a coreactant enhancer. The microstructure of ternary transition metal chalcogenide CdS<sub><i>y</i></sub>Se<sub>1–<i>y</i></sub> was precisely tuned by Zn<sup>2+</sup> doping to avoid aggregation and thus enable stable and efficient cathodic ECL responses. The bimetallic sulfide FeCoS<sub>2</sub> was synthesized using a metal organic framework (MOF) as the template by ion permeation. It was able to catalyze the coreactant efficiently due to the synergistic effect of the Fe<sup>2+</sup> and Co<sup>2+</sup>. The immunosensor exhibited low detection limit (7.6 × 10<sup>–5</sup> U mL<sup>–1</sup>) in the wide linear range of 0.0001–100 U mL<sup>–1</sup>, offering a sensitive CA19-9 detection method.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"61 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2024-11-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142684918","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}
Pub Date : 2024-11-20DOI: 10.1021/acs.analchem.4c04510
Min Shi, Yun Zhang, Jia-Xing Chen, Yanyuan Wu, Zongping Wang, Peng-Fei Shi, Xudong Jin, Xue-Qiang Wang
Peroxynitrite (ONOO–) is a critical biomarker associated with a wide array of diseases including cancer, inflammatory conditions, and neurodegenerative disorders. This study introduces an innovative chemiluminescence nanoprobe (CLNP) based on a bicyclic dioxetane structure, designed for highly sensitive and specific in vivo imaging of ONOO–. Our CLNP demonstrates exceptional capabilities in generating high-contrast imaging of disease lesions, with applications verified across tumor models, acute inflammation, and acute liver injury scenarios. Key findings highlight the probe’s rapid response to oxidative species, superior tissue penetration, and high signal-to-noise ratio, underscoring its potential for real-time diagnostic applications. This work represents an important advance in the field of diagnostic imaging using CL probes, offering promising avenues for the early detection and treatment of ONOO–-related pathologies.
{"title":"A Bicyclic Dioxetane Chemiluminescence Nanoprobe for Peroxynitrite Imaging in Vivo","authors":"Min Shi, Yun Zhang, Jia-Xing Chen, Yanyuan Wu, Zongping Wang, Peng-Fei Shi, Xudong Jin, Xue-Qiang Wang","doi":"10.1021/acs.analchem.4c04510","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c04510","url":null,"abstract":"Peroxynitrite (ONOO<sup>–</sup>) is a critical biomarker associated with a wide array of diseases including cancer, inflammatory conditions, and neurodegenerative disorders. This study introduces an innovative chemiluminescence nanoprobe (CLNP) based on a bicyclic dioxetane structure, designed for highly sensitive and specific in vivo imaging of ONOO<sup>–</sup>. Our CLNP demonstrates exceptional capabilities in generating high-contrast imaging of disease lesions, with applications verified across tumor models, acute inflammation, and acute liver injury scenarios. Key findings highlight the probe’s rapid response to oxidative species, superior tissue penetration, and high signal-to-noise ratio, underscoring its potential for real-time diagnostic applications. This work represents an important advance in the field of diagnostic imaging using CL probes, offering promising avenues for the early detection and treatment of ONOO<sup>–</sup>-related pathologies.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"1 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2024-11-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142678924","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}
Pub Date : 2024-11-20DOI: 10.1021/acs.analchem.4c05127
Zhaowei Meng, Amir Ata Saei, Hezheng Lyu, Massimiliano Gaetani, Roman A. Zubarev
The proteome integral solubility alteration (PISA) assay is widely used for identifying drug targets, but it is labor-intensive and time-consuming and requires a substantial amount of biological sample. Aiming at enabling automation and greatly reducing the sample amount, we developed one-pot time-induced (OPTI)-PISA. Here, we demonstrate OPTI-PISA performance on identifying targets of multiple drugs in cell lysate and scaling down the sample amount to sub-microgram levels, making the PISA method suitable for NanoProteomics. OPTI-PISA can be implemented using only the standard equipment of a proteomics lab.
{"title":"One-Pot Time-Induced Proteome Integral Solubility Alteration Assay for Automated and Sensitive Drug–Target Identification","authors":"Zhaowei Meng, Amir Ata Saei, Hezheng Lyu, Massimiliano Gaetani, Roman A. Zubarev","doi":"10.1021/acs.analchem.4c05127","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c05127","url":null,"abstract":"The proteome integral solubility alteration (PISA) assay is widely used for identifying drug targets, but it is labor-intensive and time-consuming and requires a substantial amount of biological sample. Aiming at enabling automation and greatly reducing the sample amount, we developed one-pot time-induced (OPTI)-PISA. Here, we demonstrate OPTI-PISA performance on identifying targets of multiple drugs in cell lysate and scaling down the sample amount to sub-microgram levels, making the PISA method suitable for NanoProteomics. OPTI-PISA can be implemented using only the standard equipment of a proteomics lab.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"3 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2024-11-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142679138","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}
Pub Date : 2024-11-20DOI: 10.1021/acs.analchem.4c03823
Kaineng Huang, Yi He, Xingyu Li, Yuanjiang Pan, Yuanji Gao
Herein, a new strategy is employed to build a controllable thermal-coupled charge ionization (TCCI) device to elucidate the desorption–ionization mechanism of plasma ion sources. Efficient synergistic desorption and ionization are achieved within the TCCI device by independently controlling the desorption temperature and plasma charges. The TCCI device efficiently ionizes samples using abundant free electrons, charges, and active species from arc plasma. The coexistence of free electrons and hydroxide radicals confers redox capability to the TCCI system, implying the presence of a unified redox mechanism even when the arc plasma is transmitted through a metal conductor over a distance. In addition, molecular ions of the analytes facilitate the differentiation between primary and secondary amines during their analysis. Notably, the TCCI device enables a switch between hard and soft ionization by adjusting the thermal desorption temperature. At high temperatures (>400 °C), the TCCI device exhibits hard ionization characteristics, producing fragment ions beneficial for isomer discrimination. The TCCI mass spectrometry exhibits robust performance in terms of sensitivity and accuracy for detecting antibiotics and sterols in saline solutions, achieving linearity with correlation coefficients ≥0.99 and excellent reproducibility. The successful analysis of seven pharmaceuticals and four sterols in complex matrices using the TCCI device demonstrates its excellent salt and matrix tolerance. Overall, the TCCI device, with its independent control over thermal desorption and arc plasma, achieves efficient synergistic desorption and ionization, overcoming limitations in existing ionization technologies and contributing to the study of gas-phase ion dynamics and mechanisms.
{"title":"Unlocking the Mysteries of the Desorption–Ionization Mechanism via Separate Thermal and Charge Strategies","authors":"Kaineng Huang, Yi He, Xingyu Li, Yuanjiang Pan, Yuanji Gao","doi":"10.1021/acs.analchem.4c03823","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c03823","url":null,"abstract":"Herein, a new strategy is employed to build a controllable thermal-coupled charge ionization (TCCI) device to elucidate the desorption–ionization mechanism of plasma ion sources. Efficient synergistic desorption and ionization are achieved within the TCCI device by independently controlling the desorption temperature and plasma charges. The TCCI device efficiently ionizes samples using abundant free electrons, charges, and active species from arc plasma. The coexistence of free electrons and hydroxide radicals confers redox capability to the TCCI system, implying the presence of a unified redox mechanism even when the arc plasma is transmitted through a metal conductor over a distance. In addition, molecular ions of the analytes facilitate the differentiation between primary and secondary amines during their analysis. Notably, the TCCI device enables a switch between hard and soft ionization by adjusting the thermal desorption temperature. At high temperatures (>400 °C), the TCCI device exhibits hard ionization characteristics, producing fragment ions beneficial for isomer discrimination. The TCCI mass spectrometry exhibits robust performance in terms of sensitivity and accuracy for detecting antibiotics and sterols in saline solutions, achieving linearity with correlation coefficients ≥0.99 and excellent reproducibility. The successful analysis of seven pharmaceuticals and four sterols in complex matrices using the TCCI device demonstrates its excellent salt and matrix tolerance. Overall, the TCCI device, with its independent control over thermal desorption and arc plasma, achieves efficient synergistic desorption and ionization, overcoming limitations in existing ionization technologies and contributing to the study of gas-phase ion dynamics and mechanisms.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"84 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2024-11-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142678922","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}
Pub Date : 2024-11-20DOI: 10.1021/acs.analchem.4c03633
Hao Zhang, Jingde Fang, Kaiqin Chu, Zachary J. Smith
Lipid droplets (LDs) are highly dynamic organelles, undertaking many important functions such as maintaining lipid metabolism and cellular homeostasis. Traditional methods to analyze LD dynamics focus on morphological changes, while chemical dynamics cannot be easily probed with traditional analytical chemistry techniques. To overcome this challenge, we show here how our phase-guided Raman sampling method, where high-resolution phase microscopy images direct a Raman sampling beam, can perform label-free, multimodal characterization of LD dynamics in living cells at both the single-cell and single-LD levels with submicron accuracy and high temporal resolution. We demonstrate the study of the morphological–compositional dynamics of human hepatocellular carcinoma cells (PLC cells) under different environmental conditions and with and without fatty acid supplementation, providing insight into LD heterogeneity and heterogeneity of response. Finally, we introduce a measurement method for the dynamics of cell-average LD composition, which can quickly and accurately characterize the lipid dynamics at the single-cell level with <30 s temporal resolution. The results here show the promise of the phase-guided Raman sampling method for dynamic morpho-chemical profiling of organelle populations.
{"title":"Real-Time Analysis of Lipid Droplet Morpho-Chemical Dynamics in Living Human Hepatocytes via Phase-Guided Raman Sampling","authors":"Hao Zhang, Jingde Fang, Kaiqin Chu, Zachary J. Smith","doi":"10.1021/acs.analchem.4c03633","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c03633","url":null,"abstract":"Lipid droplets (LDs) are highly dynamic organelles, undertaking many important functions such as maintaining lipid metabolism and cellular homeostasis. Traditional methods to analyze LD dynamics focus on morphological changes, while chemical dynamics cannot be easily probed with traditional analytical chemistry techniques. To overcome this challenge, we show here how our phase-guided Raman sampling method, where high-resolution phase microscopy images direct a Raman sampling beam, can perform label-free, multimodal characterization of LD dynamics in living cells at both the single-cell and single-LD levels with submicron accuracy and high temporal resolution. We demonstrate the study of the morphological–compositional dynamics of human hepatocellular carcinoma cells (PLC cells) under different environmental conditions and with and without fatty acid supplementation, providing insight into LD heterogeneity and heterogeneity of response. Finally, we introduce a measurement method for the dynamics of cell-average LD composition, which can quickly and accurately characterize the lipid dynamics at the single-cell level with <30 s temporal resolution. The results here show the promise of the phase-guided Raman sampling method for dynamic morpho-chemical profiling of organelle populations.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"7 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2024-11-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142678849","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}
Flow injection analysis and liquid chromatography are frequently combined with electrochemiluminescence (ECL) for flow analysis. Almost all electrochemistry flow analyses employ traditional three-electrode electrochemical flow cells which have working electrode, counter electrode, and reference electrode; however, it is expensive and difficult to fabricate a traditional three-electrode electrochemical flow cell and inconvenient to renew the electrode. In this study, we have developed a single-electrode flow cell using commercially available conductive polyethylene film as the only electrode through potential differences induced by the electrode resistance for the first time. The single-electrode flow cell features a simple structure, easy renewal of the electrode, and low cost compared to the traditional three-electrode electrochemical flow cells. Taking the typical Ru(bpy)32+/oxalate ECL system as the analytical model, flow analysis of clinically important oxalate was achieved using single-electrode flow cell. A regression linear equation was obtained over the oxalate concentration ranges from 1 to 200 μM, with a detection limit of 0.92 μM. The single-electrode flow cell is promising for ECL flow analysis.
{"title":"Single-Electrode Flow Cell for Electrochemiluminescent Flow Analysis","authors":"Zhiyong Dong, Yequan Chen, Shiyu Xia, Ala’a Mhmoued Abdllh Alboull, Altaf Hussain, Yu Tian, Guobao Xu","doi":"10.1021/acs.analchem.4c04322","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c04322","url":null,"abstract":"Flow injection analysis and liquid chromatography are frequently combined with electrochemiluminescence (ECL) for flow analysis. Almost all electrochemistry flow analyses employ traditional three-electrode electrochemical flow cells which have working electrode, counter electrode, and reference electrode; however, it is expensive and difficult to fabricate a traditional three-electrode electrochemical flow cell and inconvenient to renew the electrode. In this study, we have developed a single-electrode flow cell using commercially available conductive polyethylene film as the only electrode through potential differences induced by the electrode resistance for the first time. The single-electrode flow cell features a simple structure, easy renewal of the electrode, and low cost compared to the traditional three-electrode electrochemical flow cells. Taking the typical Ru(bpy)<sub>3</sub><sup>2+</sup>/oxalate ECL system as the analytical model, flow analysis of clinically important oxalate was achieved using single-electrode flow cell. A regression linear equation was obtained over the oxalate concentration ranges from 1 to 200 μM, with a detection limit of 0.92 μM. The single-electrode flow cell is promising for ECL flow analysis.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"1 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2024-11-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142673056","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}
Pub Date : 2024-11-20DOI: 10.1021/acs.analchem.4c04416
Tao Tang, Fushou Liu, Biao Huang, Hao Li, Wen-Ping Lin, Zhi-Jun Sun, Mingxi Zhang, Ran Cui
Hepatic ischemia-reperfusion injury (HIRI) and induced systemic inflammation is a time-dependent multistage process which poses a risk of causing direct hepatic dysfunction and multiorgan failure. Real-time in situ comprehensive visualization assessment is important and scarce for imaging-guided therapeutic interventions and timely efficacy evaluation. Here, a logically activatable nanoreporter (termed QD@IR783-TK-FITC) is developed for time-phase imaging quantification of HIRI and induced systemic inflammation. The nanoreporters could be used for in vivo ratiometric NIR-IIb fluorescence sensing of reactive oxygen species (ROS), which can depict the in situ hepatic ROS fluctuation for the early diagnosis of HIRI in the initial 3 h. Meanwhile, the ROS-specific reaction releases renal-clearable fluorophore fragments from nanoreporters for monitoring the systematic inflammation induced by HIRI via longitudinal urinalysis. In addition, a functional relationship between digitized signal outputs (NIR-IIb ratios, urinary fluorescence) with hepatic injury scores has been established, realizing precise prediction of HIRI severity and preassessment of therapeutic efficacy. Such a time-phased modular toolbox can dynamically report HIRI-induced systemic inflammation in vivo, providing an efficient approach for HIRI treatment.
肝脏缺血再灌注损伤（HIRI）和诱发的全身炎症是一个时间依赖性的多阶段过程，有直接导致肝功能障碍和多器官功能衰竭的风险。实时原位综合可视化评估对于成像引导的治疗干预和及时的疗效评估非常重要，也非常稀缺。在此，我们开发了一种逻辑上可激活的纳米报告器（称为 QD@IR783-TK-FITC），用于对 HIRI 和诱导的全身炎症进行时相成像量化。同时，ROS 特异性反应可从纳米孔释放出肾脏可清除的荧光团片段，通过纵向尿液分析监测 HIRI 诱导的系统性炎症。此外，还建立了数字化信号输出（近红外-IIb 比率、尿液荧光）与肝损伤评分之间的功能关系，实现了对 HIRI 严重程度的精确预测和疗效的预先评估。这种分时模块化工具箱可以动态报告 HIRI 引起的体内全身炎症，为 HIRI 治疗提供了一种有效的方法。
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