Analytical Chemistry最新文献_第6页

Renal-Clearable Molecular Reporters for Near-Infrared Fluorescence Imaging and Urinalysis of Pulmonary Metastatic Tumor

IF 7.4 1区化学

Analytical Chemistry Pub Date : 2025-04-11 DOI: 10.1021/acs.analchem.5c00392

Ya Zhou, Jiangxian Chen, Yang Zhou, Yi Liu, Xingyue Yang, Xiaoxiao Wang, Wanyi Chen, Weiping Xu, Hui Cai, Jiaguo Huang

{"title":"Renal-Clearable Molecular Reporters for Near-Infrared Fluorescence Imaging and Urinalysis of Pulmonary Metastatic Tumor","authors":"Ya Zhou, Jiangxian Chen, Yang Zhou, Yi Liu, Xingyue Yang, Xiaoxiao Wang, Wanyi Chen, Weiping Xu, Hui Cai, Jiaguo Huang","doi":"10.1021/acs.analchem.5c00392","DOIUrl":"https://doi.org/10.1021/acs.analchem.5c00392","url":null,"abstract":"Despite approximately 40% of all patients with cancer developing pulmonary metastases in the course of their disease, it remains a diagnostic challenge in clinical practice. Herein, we propose a fluorogenic probe (CPRG) with gamma-glutamyl transferase (GGT)-triggered signal turn-on for near-infrared fluorescence imaging (NIRF) and urinalysis of orthotopic pulmonary metastatic tumors in living mice. CPRG comprised four key moieties: a GGT-reactive moiety, a hemicyanine-based signal unit, a polyethylene glycol linker, and an active tumor targeting moiety. Such a tailored probe is intrinsically nonfluorescent and only activates its NIRF signals in the presence of GGT. After intratracheal administration into the lungs of living tumor-bearing mice, CPRG can efficiently accumulate in the pulmonary tumors and sensitively turn-on the NIRF signal for real-time imaging. Relying on the high renal clearance efficiency (∼70% ID), it can be rapidly excreted through kidneys for urinalysis and assessed by the chemotherapeutic efficacy of cisplatin. This study not only reports fluorogenic tracers for imaging of pulmonary metastatic tumors but also provides guidelines for the development of molecular probes for companion diagnosis of metastatic cancer.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"33 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-04-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143822797","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

Chemometrics-Assisted Enhancement of Electrochemical Biosensor Performance toward miRNA Detection 化学计量学辅助提高电化学生物传感器检测 miRNA 的性能

IF 7.4 1区化学

Analytical Chemistry Pub Date : 2025-04-11 DOI: 10.1021/acs.analchem.4c05402

Wanda Cimmino, Simona Esposito, Panagiota M. Kalligosfyri, Nunzia Iaccarino, Stefano Cinti

{"title":"Chemometrics-Assisted Enhancement of Electrochemical Biosensor Performance toward miRNA Detection","authors":"Wanda Cimmino, Simona Esposito, Panagiota M. Kalligosfyri, Nunzia Iaccarino, Stefano Cinti","doi":"10.1021/acs.analchem.4c05402","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c05402","url":null,"abstract":"Chemometrics represents a potent tool for optimizing the experimental setup and subsequently boosting the performance of analytical methods. In particular, design of experiments (DoE) allows the experimental conditions to be optimized with high accuracy and a lower number of experiments when compared with the classical univariate approach, also known as one variable at a time (OVAT), which provides only a partial understanding on how factors affect the response. In this work, DoE was exploited, specifically a D-optimal design was used, to improve the analytical performance of a hybridization-based paper-based electrochemical biosensor, taking as target of the study the miRNA-29c (miR-29c) that is related to triple negative breast cancer. The sensing platform is composed of six variables to be optimized, including both those related to the sensor’s manufacture (i.e., gold nanoparticles, immobilized DNA probe) and those related to the working conditions (i.e., ionic strength, probe-target hybridization, electrochemical parameters). The adoption of DoE allowed us to optimize the device using only 30 experiments with respect to the 486 that would have been required with the OVAT approach, and as a consequence of the more accurate optimal conditions that have been reached, the detection of miRNA was more sensitive and repeatable when compared with previous data reported using the univariate approach for optimization, leading to a 5-fold limit of detection (LOD) improvement toward miRNA. It confirms that chemometrics might be considered a fundamental tool to be used in the development of various kinds of sensors and biosensors.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"17 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-04-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143822516","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

Equivalent and Complementary Variables Screening for the Optimization of Wavelengths in Spectral Multivariate Calibration

IF 7.4 1区化学

Analytical Chemistry Pub Date : 2025-04-11 DOI: 10.1021/acs.analchem.5c00662

Honghong Wang, Shuming Lan, Lingbo Wei, Yunchi Hu, Yan Kang, Ting Wu, Yiping Du

{"title":"Equivalent and Complementary Variables Screening for the Optimization of Wavelengths in Spectral Multivariate Calibration","authors":"Honghong Wang, Shuming Lan, Lingbo Wei, Yunchi Hu, Yan Kang, Ting Wu, Yiping Du","doi":"10.1021/acs.analchem.5c00662","DOIUrl":"https://doi.org/10.1021/acs.analchem.5c00662","url":null,"abstract":"Equivalent variables (EVs) were defined on the basis of a finding that replacing a selected variable with its neighbor variable provided a similar model performance. These are a group of variables having nearly equal modeling effects and can be efficient alternative to each other. Complementary variables (CVs) were defined as different variables screened from different variable selection algorithms that can further improve multivariate calibration by combining CVs with the original selected variables. Three variable selection algorithms, stability competitive adaptive reweighted sampling (SCARS), competitive adaptive reweighted sampling (CARS), and Monte Carlo and uninformative variable elimination (MC-UVE), were used for screening EVs and CVs and verifying the replaceability of EVs and model improvability with CVs. The developed strategy of variable selection based on EVs and CVs was investigated using NIR, MIR, and UV–vis spectra datasets. Seventeen basic variables (BVs) and 54 EVs were screened from the corn NIR spectra by SCARS. The selected EVs and BVs were comparable to one another in terms of modeling, and all models built with replaced variables showed close prediction errors with a RMSEP deviation <0.003. Furthermore, 15 CVs of SCARS were screened from EVs of CARS and MC-UVE. The combination of CVs and BVs of SCARS can significantly improve model performance; RMSEC and RMSEP decreased from 0.0207 and 0.0290 to 0.0109 and 0.0136, respectively. Similar results were obtained for other datasets. Results revealed that screening CVs from EVs of other algorithms and combining BVs could effectively optimize variable selection and improve model performance.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"16 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-04-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143819859","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

Machine Learning-Driven Surface Plasmon-Enhanced Dual Spectroscopies Improve Recognition and Real-Time Monitoring of Hazardous Chemicals

IF 7.4 1区化学

Analytical Chemistry Pub Date : 2025-04-11 DOI: 10.1021/acs.analchem.5c00545

Yanyan Lu, Yu Qiao, Haoming Bao, Kang Chen, Yi Wei, Qian Zhao, Guo Kang Leon, Hongwen Zhang, Xing Yi Ling, Weiping Cai

{"title":"Machine Learning-Driven Surface Plasmon-Enhanced Dual Spectroscopies Improve Recognition and Real-Time Monitoring of Hazardous Chemicals","authors":"Yanyan Lu, Yu Qiao, Haoming Bao, Kang Chen, Yi Wei, Qian Zhao, Guo Kang Leon, Hongwen Zhang, Xing Yi Ling, Weiping Cai","doi":"10.1021/acs.analchem.5c00545","DOIUrl":"https://doi.org/10.1021/acs.analchem.5c00545","url":null,"abstract":"To address the challenges of precise identification and real-time monitoring of hazardous chemicals, this work proposes and develops surface-plasmon-enhanced dual spectroscopies (SPEDS). This technique combines highly recognizable surface-enhanced Raman spectroscopy (SERS) with real-time plasmon-mediated differential ultraviolet–visible spectroscopy (P-DUS). The feasibility of this technique is demonstrated by successfully acquiring SPEDS signals of thiourea with a plasmonic gold colloidal system. By combining SPEDS with machine learning algorithms, we achieve accurate identification and precise quantification of chemicals, with accuracies of 98.2 and 98.6%, respectively, significantly outperforming single P-DUS (63.2 and 95.1%) and SERS (80.3 and 86.5%). Additionally, we demonstrate the universality and expandability of SPEDS through other plasmonic nanostructures of various shapes and surface modifications. Using a CuS-coated Au nanoarray, we demonstrate multiple 8-h monitoring sessions of Hg2+ with good anti-interference and robust quantification, thereby highlighting the practical potential of SPEDS in real-world applications. These results position SPEDS as a cutting-edge and multifunctional chemical sensing platform, unlocking transformative possibilities for advancing environmental monitoring, industrial safety, and public health.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"11 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-04-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143819871","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

Anionic Cyanine Membrane Probes for Live Cells and In Vivo Fluorescence Imaging 用于活细胞和体内荧光成像的阴离子蓝膜探针

IF 7.4 1区化学

Analytical Chemistry Pub Date : 2025-04-11 DOI: 10.1021/acs.analchem.4c05795

Dmytro I. Danylchuk, Igor Khalin, Yelisetty V. Suseela, Severin Filser, Nikolaus Plesnila, Andrey S. Klymchenko

{"title":"Anionic Cyanine Membrane Probes for Live Cells and In Vivo Fluorescence Imaging","authors":"Dmytro I. Danylchuk, Igor Khalin, Yelisetty V. Suseela, Severin Filser, Nikolaus Plesnila, Andrey S. Klymchenko","doi":"10.1021/acs.analchem.4c05795","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c05795","url":null,"abstract":"Molecular probes for cell plasma membranes are indispensable for fluorescence imaging. Herein, we present an array of five anionic cyanine-based turn-on plasma membrane probes with emission spanning from green to near infrared. They are analogous to the commonly used MemBright probe family, where two zwitterionic anchor groups are replaced with anionic sulfonates with dodecyl chains. The developed probes provide selective wash-free staining of plasma membranes of live cells in vitro, featuring improved brightness and slower internalization inside the cells. In comparison to protein-based (wheat germ agglutinin) membrane markers, new membrane probes provide better staining in poorly accessible cell–cell contacts. A key challenge is to stain cell plasma membranes directly in vivo. During in vivo brain tissue imaging in living mice by two-photon microscopy, the anionic cyanine probes allowed us to visualize in detail the pyramidal neurons with high image quality, clearly resolving neuron soma, dendrites with dendritic spines, and axons with axonal boutons. The developed anionic cyanine-based plasma membrane probes constitute an important extension of the toolbox for plasma membrane research.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"42 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-04-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143822800","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

Ion Mobility Gas-Phase Separation Enhances Top-Down Mass Spectrometry of Heavily Modified Guide RNA

IF 7.4 1区化学

Analytical Chemistry Pub Date : 2025-04-11 DOI: 10.1021/acs.analchem.5c00705

Luis A. Macias, Jamie Lowther, Eric L. Tillotson, Ellen Rohde, James A. Madsen

{"title":"Ion Mobility Gas-Phase Separation Enhances Top-Down Mass Spectrometry of Heavily Modified Guide RNA","authors":"Luis A. Macias, Jamie Lowther, Eric L. Tillotson, Ellen Rohde, James A. Madsen","doi":"10.1021/acs.analchem.5c00705","DOIUrl":"https://doi.org/10.1021/acs.analchem.5c00705","url":null,"abstract":"As gene editing technologies enter the clinic, state-of-the-art characterization methods have been developed in parallel to assess the components of these paradigm-shifting medicines. One such component, the guide RNA (gRNA) element of CRISPR-based drugs, is a large synthetic heavily modified oligonucleotide that programs for the desired gene edit. Conventional oligonucleotide sequencing technologies can inform gRNA composition, but these methods may not completely capture the chemical modifications that are introduced during synthesis. Circumventing these challenges, mass spectrometry has demonstrated use in oligonucleotide analyses and has been combined here with ion mobility to deepen its characterization power. The use of ion mobility enabled us to perform gas-phase separation of the fragment ions produced by top-down mass spectrometry, yielding a significant increase in fragment identifications for a highly modified 100-mer gRNA by uncovering high-confidence assignments for heavily modified regions and for the important spacer region. Furthermore, the high-confidence fragment assignments empowered simultaneous de novo sequencing and chemical modification localization for the 5′-end spacer region as well as for 15 nucleotides on the heavily modified 3′-end. Overall, a total sequence coverage of 95% was achieved for the heavily modified 100-mer, ushering near complete sequence and chemical modification confirmation by top-down mass spectrometry.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"248 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-04-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143822798","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

Spatial–Temporal Cube Denoising for Real-Time Digital PCR Melting Analysis to Improve the Accuracy of Multiplex Detection 用于实时数字 PCR 熔解分析的时空立方体去噪技术可提高多重检测的准确性

IF 7.4 1区化学

Analytical Chemistry Pub Date : 2025-04-11 DOI: 10.1021/acs.analchem.5c00906

Peilin Zang, Jinze Li, Dongshu Li, Qi Yang, Zhiqi Zhang, Yan Gao, Runhu Huang, Yueye Zhang, Wei Zhang, Chuanyu Li, Jia Yao, Lianqun Zhou

{"title":"Spatial–Temporal Cube Denoising for Real-Time Digital PCR Melting Analysis to Improve the Accuracy of Multiplex Detection","authors":"Peilin Zang, Jinze Li, Dongshu Li, Qi Yang, Zhiqi Zhang, Yan Gao, Runhu Huang, Yueye Zhang, Wei Zhang, Chuanyu Li, Jia Yao, Lianqun Zhou","doi":"10.1021/acs.analchem.5c00906","DOIUrl":"https://doi.org/10.1021/acs.analchem.5c00906","url":null,"abstract":"Real-time digital melting curves combine highly sensitive real-time digital polymerase chain reaction (PCR) with high-resolution melting curve analysis to achieve multiplex detection, which optimizes PCR efficiency and improves identification capability. However, due to the noise interference during the experiment, it is challenging to accurately obtain the melting temperature by extracting the microwell signal only from a single image at each temperature, further affecting the accuracy and resolution of multiplex detection. In this work, a spatial–temporal cube denoising model (STCDM) was established, which explicitly integrates the spatial and temporal dimensions to address the noise inherent in melting images. By constructing a three-dimensional spatial–temporal cube, the STCDM performs block denoising to effectively mitigate noise across both dimensions, leading to more accurate and reliable multiplex detection. The correction results demonstrated an improvement in melting temperature accuracy from 92% to 98%, with a resolution within 0.6 °C and good repeatability. Therefore, on the basis of the real-time dPCR platform, using the STCDM can significantly enhance the accuracy, driving the advancement of multiplex detection technology.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"17 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-04-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143822801","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

Dual Desalting Electrospray Strategy for In-Cell Mass Spectrometry to Reveal Novel Sphingolipid Metabolism in an Epithelial–Mesenchymal Transition

IF 7.4 1区化学

Analytical Chemistry Pub Date : 2025-04-11 DOI: 10.1021/acs.analchem.4c06669

Huimin Liu, Tianhong Wu, Hongbin He, Rongbin Zhou, Jia Zhao, Liujuan Zhan, Zhuanghao Hou, Guangming Huang

{"title":"Dual Desalting Electrospray Strategy for In-Cell Mass Spectrometry to Reveal Novel Sphingolipid Metabolism in an Epithelial–Mesenchymal Transition","authors":"Huimin Liu, Tianhong Wu, Hongbin He, Rongbin Zhou, Jia Zhao, Liujuan Zhan, Zhuanghao Hou, Guangming Huang","doi":"10.1021/acs.analchem.4c06669","DOIUrl":"https://doi.org/10.1021/acs.analchem.4c06669","url":null,"abstract":"The metabolome offers a direct snapshot of cell function and can respond to external changes within a very brief time scale of seconds or minutes. In situ in-cell mass spectrometry, with minimal pretreatment, enables direct analysis in a nonvolatile salt environment. However, it is challenging to obtain abundant metabolomes due to the inherent incompatibility of nonvolatile salts with mass spectrometry. Here, we developed a dual desalting electrospray ionization mass spectrometry (dd-ESI MS) technology for in-cell MS measurement to obtain a comprehensive and native cellular metabolome in nonvolatile salt buffers. The salt ions and metabolites were initially separated through the mild electrophoretic effect of induced nanoelectrospray ionization (InESI). In the following electrospray process, the complex interactions between aqueous droplets and methanol droplets further enhanced the desalting effect. Compared with nanoESI, dd-ESI MS exhibited stronger salt tolerance and higher sensitivity for cell metabolome analysis in PBS buffer. Interestingly, we observed a significant enrichment of the sphingolipid metabolism pathway during the epithelial–mesenchymal transition, a metabolic pathway not previously confirmed by metabolomics techniques. In addition, the transcriptome analysis also revealed consistent gene changes, further confirming the validity of our findings. dd-ESI MS enabled the acquisition of a more comprehensive and native metabolome, providing novel insights into complex physiological processes.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"29 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-04-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143819844","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

Self-Cascade of the Cu/Ce-MOF-808 Nanozyme for One-Step Colorimetric Sensing

IF 7.4 1区化学

Analytical Chemistry Pub Date : 2025-04-11 DOI: 10.1021/acs.analchem.5c00433

Yuan Qin, Huimei Liang, Jia Wu, Zheyang Chi, Shulin Zhao, Fanggui Ye

{"title":"Self-Cascade of the Cu/Ce-MOF-808 Nanozyme for One-Step Colorimetric Sensing","authors":"Yuan Qin, Huimei Liang, Jia Wu, Zheyang Chi, Shulin Zhao, Fanggui Ye","doi":"10.1021/acs.analchem.5c00433","DOIUrl":"https://doi.org/10.1021/acs.analchem.5c00433","url":null,"abstract":"Natural enzyme cascades, including the same and different kinds of enzymes, have been widely used in biosensing. However, it is still a challenge for nanozymes, the mimics of natural enzymes, to achieve biosensing with different types of enzyme-like activities based on cascade reactions, such as hydrolase and oxidoreductase. Considering the characteristics of the multienzyme-like activity of some nanozymes, as a proof of concept, this study demonstrates a Cu/Ce-MOF-808 nanozyme as a self-cascade catalyst with hydrolase-like and catechol oxidase-like activities. Taking organophosphorus pesticides as an example, we constructed a self-cascade catalytic reaction for the one-step colorimetric detection of isocarbophos. Specifically, the hydrolase-like activity of Cu/Ce-MOF-808 can hydrolyze isocarbophos to produce colorless isopropyl salicylate, which is further oxidized by the catechol oxidase-like activity of Cu/Ce-MOF-808 and complexed with 4-aminoantipyrine (4-AAP) to produce red quinoneimine under neutral conditions with illumination. Thus, a colorimetric strategy for sensitive isocarbophos analysis is developed, with a linear range of 0.90–400.00 μg·mL–1 and a detection limit of 0.42 μg·mL–1. This research presents a new approach to the design and synthesis of nanozymes and has great application potential in the field of nanozyme cascade biosensing.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"21 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-04-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143819873","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

Quantification of Brominated Flame Retardants in Synthetic Polymers via Direct Mass Spectrometric Analysis

IF 7.4 1区化学

Analytical Chemistry Pub Date : 2025-04-11 DOI: 10.1021/acs.analchem.5c00946

Ville H. Nissinen, Krista Grönlund, Nea Heilala, Ilkka Rytöluoto, Milad Mosallaei, Kirsi Korpijärvi, Paavo Auvinen, Mika Suvanto, Jarkko J. Saarinen, Janne Jänis

{"title":"Quantification of Brominated Flame Retardants in Synthetic Polymers via Direct Mass Spectrometric Analysis","authors":"Ville H. Nissinen, Krista Grönlund, Nea Heilala, Ilkka Rytöluoto, Milad Mosallaei, Kirsi Korpijärvi, Paavo Auvinen, Mika Suvanto, Jarkko J. Saarinen, Janne Jänis","doi":"10.1021/acs.analchem.5c00946","DOIUrl":"https://doi.org/10.1021/acs.analchem.5c00946","url":null,"abstract":"Brominated flame retardants (BFRs) are persistent organic pollutants commonly encountered in plastics. Herein, we report on the quantification of BFRs directly from plastic samples via direct insertion probe mass spectrometry (DIP-MS). The study was conducted using model polymer samples comprising either acrylonitrile butadiene styrene copolymer (ABS) or high impact polystyrene (HIPS) and a BFR, namely decabromodiphenyl ether (decaBDE), hexabromocyclododecane (HBCD), or tetrabromobisphenol A (TBBPA). DIP-MS enabled direct quantification of decaBDE and TBBPA from both ABS and HIPS matrices. A linear correlation between BFR signal intensity and bromine (Br) content of the samples, as determined by X-ray fluorescence, was established over a Br concentration range of 0–7 wt %, or even higher. While DIP-MS showed potential for HBCD analysis as well, its effectiveness for quantitative HBCD determination remains partly uncertain due to the observed reactivity of HBCD during sample preparation. The detection limits for all studied BFRs were below 500 mg Br/kg. Additionally, the study shed light on matrix effects related to additive analysis by DIP-MS, revealing that the polymer and other additives can affect BFR volatilization and reactivity. Overall, DIP-MS demonstrated significant potential for the rapid quantification of BFRs from plastic samples with minimal sample preparation, which is imperative for promoting more efficient plastic recycling.","PeriodicalId":27,"journal":{"name":"Analytical Chemistry","volume":"25 1","pages":""},"PeriodicalIF":7.4,"publicationDate":"2025-04-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143822803","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