Journal of Chromatography A最新文献_第2页

Radiation stability of two extraction chromatography resins containing aza-crown-based diglycolamides used for Am(III) uptake

IF 3.8 2区化学 Q1 BIOCHEMICAL RESEARCH METHODS

Journal of Chromatography A

Pub Date : 2025-02-25 DOI: 10.1016/j.chroma.2025.465822

Piyali Banerjee , Rajesh B. Gujar , Seraj A. Ansari , Rajesh Saini , Anoop Kelkar , Richard J.M. Egberink , Willem Verboom , Prasanta K. Mohapatra

The radiolytic stability of two extraction chromatography resins with multiple diglycolamide arms was investigated by exposing them to gamma radiation and carrying out uptake studies of Am(III) from acidic feeds. The resins contained aza-crown-based diglycolamide (DGA) ligands, viz., triaza-9-crown-3-N,N’,N”-trisdiglycolamide (TAM-3-DGA) and tetraaza-12-crown-4-N,N’,N”,N’”-tetrakisdiglycolamide (TAM-4-DGA), where the DGA moieties were grafted to the ‘N’ atoms of the macrocyclic ring. These two resins showed excellent performance for the separation of Am(III) from radioactive feed solutions and radiation stabilities were evaluated under a reasonably high gamma ray dose of 1000 kGy. The irradiated resins were employed to recover Am(III) from the acidic feeds in order to evaluate the radiation resistance of the sorbent. The irradiated resins yielded large distribution coefficients for the uptake of Am(III) in the acidity range of 0.5 M – 6 M HNO₃. Different physicochemical properties of the irradiated resins vis-à-vis the pristine resins were evaluated to establish their radiation stabilities. Recycling possibility of the resins was ensured in 5 successive cycles of sorption and desorption. Column studies were carried out using an Am(III) tracer spiked feed containing Eu carrier. The results support the possible application of the two TAM-n-DGA resins (n = 3 or 4) for the separation of Am(III) from radioactive waste solutions without any issue of recycling and radiation stability.

{"title":"Radiation stability of two extraction chromatography resins containing aza-crown-based diglycolamides used for Am(III) uptake","authors":"Piyali Banerjee , Rajesh B. Gujar , Seraj A. Ansari , Rajesh Saini , Anoop Kelkar , Richard J.M. Egberink , Willem Verboom , Prasanta K. Mohapatra","doi":"10.1016/j.chroma.2025.465822","DOIUrl":"10.1016/j.chroma.2025.465822","url":null,"abstract":"<div><div>The radiolytic stability of two extraction chromatography resins with multiple diglycolamide arms was investigated by exposing them to gamma radiation and carrying out uptake studies of Am(III) from acidic feeds. The resins contained aza-crown-based diglycolamide (DGA) ligands, <em>viz.</em>, triaza-9-crown-3-<em>N,N’,N”</em>-trisdiglycolamide (TAM-3-DGA) and tetraaza-12-crown-4-<em>N,N’,N”,N’”</em>-tetrakisdiglycolamide (TAM-4-DGA), where the DGA moieties were grafted to the ‘<em>N</em>’ atoms of the macrocyclic ring. These two resins showed excellent performance for the separation of Am(III) from radioactive feed solutions and radiation stabilities were evaluated under a reasonably high gamma ray dose of 1000 kGy. The irradiated resins were employed to recover Am(III) from the acidic feeds in order to evaluate the radiation resistance of the sorbent. The irradiated resins yielded large distribution coefficients for the uptake of Am(III) in the acidity range of 0.5 M – 6 M HNO<sub>3</sub>. Different physicochemical properties of the irradiated resins <em>vis-à-vis</em> the pristine resins were evaluated to establish their radiation stabilities. Recycling possibility of the resins was ensured in 5 successive cycles of sorption and desorption. Column studies were carried out using an Am(III) tracer spiked feed containing Eu carrier. The results support the possible application of the two TAM-n-DGA resins (<em>n</em> = 3 or 4) for the separation of Am(III) from radioactive waste solutions without any issue of recycling and radiation stability.</div></div>","PeriodicalId":347,"journal":{"name":"Journal of Chromatography A","volume":"1748 ","pages":"Article 465822"},"PeriodicalIF":3.8,"publicationDate":"2025-02-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143562417","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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

Integration of QSAR models with high throughput screening to accelerate the development of polishing chromatography unit operations

IF 3.8 2区化学 Q1 BIOCHEMICAL RESEARCH METHODS

Journal of Chromatography A

Pub Date : 2025-02-25 DOI: 10.1016/j.chroma.2025.465818

Michael Hartmann , Michael Rauscher , Julie Robinson , John Welsh , David Roush

The development of robust polishing chromatographic processes is a critical step in downstream bioprocess development that can be time-consuming and resource intensive. Recently, there has been an increase in diverse protein constructs that are not amenable to platform approaches, increasing the need for novel processes to be developed for effective purification. High throughput screening (HTS) is an important tool to parse chromatographic design space and identify promising conditions to continue development. Despite its utility, HTS capabilities are challenged by tight development timelines, material scarcity, and an increasingly complex pipeline of biotherapeutics. Predictive modeling can augment HTS by leveraging historical screening data to rapidly explore and prioritize process design space, effectively expanding the range of conditions considered without the need for additional experimental screening. Here we present the development of a quantitative structure activity relationship (QSAR) model, trained from internal HTS data, that predicts protein partitioning as a function of resin and mobile phase conditions. The training dataset contains a diverse collection of screening data and has more than 8000 datapoints, covering 29 therapeutic proteins and 44 resins. The model encodes partitioning by building descriptors of the mobile phase, parameters that describe the resin, and biophysical properties of the protein. Overall, the regression model has an R²=0.92 and shows 95% and 93% classification accuracy for predicting elution and strong binding conditions, respectively. Here, we highlight the model predictiveness and describe how in silico screening can be used as a first step in the HTS workflow to reduce design space and accelerate process development.

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引用次数: 0

RT-Pred: A web server for accurate, customized liquid chromatography retention time prediction of chemicals

IF 3.8 2区化学 Q1 BIOCHEMICAL RESEARCH METHODS

Journal of Chromatography A

Pub Date : 2025-02-25 DOI: 10.1016/j.chroma.2025.465816

Mahi Zakir , Marcia A. LeVatte , David S. Wishart

High-performance liquid chromatography (HPLC) together with mass spectrometry (MS) is routinely used to separate, identify and quantify chemicals. HPLC data also provides retention time (RT) which can be aligned with structural data. Recent developments in machine learning (ML) have improved our ability to predict RTs from known or postulated chemical structures, allowing RT data to be used more effectively in LC-MS-based compound identification. However, RT data is highly specific to each chromatographic method (CM) and hundreds of different CMs with interdependent parameters are used in separations. This has limited the application of ML-based RT predictions in compound identification. Here we introduce an easy-to-use RT prediction webserver (called RT-Pred) that predicts RTs for molecules across most chromatographic setups. RT-Pred not only supports its own in-house CM-specific RT predictors, it allows users to easily train a custom RT-Pred model using their own RT data on their own CM and to predict RTs with that custom model. RT-Pred also supports RT and compound searches against its own database of millions of predicted RTs spanning >40 different CMs. RT-Pred is also uniquely capable of accurately identifying compounds that will elute in the void volume or be retained on the column. Including this void/retained/eluted classifier significantly improves RT-Pred's performance. Tests indicate that RT-Pred had an average coefficient of determination (R²) of 0.95 over 20 different CMs. Comparisons of RT-Pred against other RT predictors showed that RT-Pred achieved lower mean absolute errors and higher R² scores than any other published RT predictor. RT-Pred is freely available at https://rtpred.ca.

{"title":"RT-Pred: A web server for accurate, customized liquid chromatography retention time prediction of chemicals","authors":"Mahi Zakir , Marcia A. LeVatte , David S. Wishart","doi":"10.1016/j.chroma.2025.465816","DOIUrl":"10.1016/j.chroma.2025.465816","url":null,"abstract":"<div><div>High-performance liquid chromatography (HPLC) together with mass spectrometry (MS) is routinely used to separate, identify and quantify chemicals. HPLC data also provides retention time (RT) which can be aligned with structural data. Recent developments in machine learning (ML) have improved our ability to predict RTs from known or postulated chemical structures, allowing RT data to be used more effectively in LC-MS-based compound identification. However, RT data is highly specific to each chromatographic method (CM) and hundreds of different CMs with interdependent parameters are used in separations. This has limited the application of ML-based RT predictions in compound identification. Here we introduce an easy-to-use RT prediction webserver (called RT-Pred) that predicts RTs for molecules across most chromatographic setups. RT-Pred not only supports its own in-house CM-specific RT predictors, it allows users to easily train a custom RT-Pred model using their own RT data on their own CM and to predict RTs with that custom model. RT-Pred also supports RT and compound searches against its own database of millions of predicted RTs spanning >40 different CMs. RT-Pred is also uniquely capable of accurately identifying compounds that will elute in the void volume or be retained on the column. Including this void/retained/eluted classifier significantly improves RT-Pred's performance. Tests indicate that RT-Pred had an average coefficient of determination (R²) of 0.95 over 20 different CMs. Comparisons of RT-Pred against other RT predictors showed that RT-Pred achieved lower mean absolute errors and higher R² scores than any other published RT predictor. RT-Pred is freely available at <span><span>https://rtpred.ca</span><svg><path></path></svg></span>.</div></div>","PeriodicalId":347,"journal":{"name":"Journal of Chromatography A","volume":"1747 ","pages":"Article 465816"},"PeriodicalIF":3.8,"publicationDate":"2025-02-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143511961","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

New strategies for non-targeted quantification in comprehensive two-dimensional gas chromatography: The potential of reconstructed TIC response factor surfaces

IF 3.8 2区化学 Q1 BIOCHEMICAL RESEARCH METHODS

Journal of Chromatography A

Pub Date : 2025-02-24 DOI: 10.1016/j.chroma.2025.465811

Jason Devers, David I. Pattison, Asger B. Hansen, Jan H. Christensen

Comprehensive two-dimensional gas chromatography (GC × GC) offers unrivaled peak capacity and the ability to resolve and characterize hundreds to thousands of compounds within complex environmental samples. Knowledge of their concentrations is essential in assessing their toxicological and regulatory relevance; however, reliable quantification typically requires concurrent analysis of an authentic standard for each compound. Response factors (RF) may be used to estimate the concentration of a compound without the need for its respective standard, but this is not routinely employed in gas chromatography-mass spectrometry (GC–MS). This study demonstrates that GC × GC offers a new opportunity for the calculation of RFs and estimating a compounds concentration via the creation of 2D total ion current (TIC) response factor surfaces (RFS). A new method, linking a compounds retention time coordinate to its RF using a reconstructed TIC approach, was used to calculate the concentration of 27 compounds in both solvent and effluent wastewater matrix. Using both suspect screening and non-targeted methodologies, average fold change errors of 1.58 and 1.83 respectively were determined for the novel RFS approach. The approach was compared to an RF prediction model utilizing molecular descriptors, using a genetic algorithm, partial least squares regression (GA-PLS) model. The accuracy of the RFS method demonstrates its potential in the fields of suspect screening and non-targeted analysis, where realistic concentration estimates are required. The RFS approach delivers comparable accuracy in concentration prediction compared to computational approaches for determining RFs, but crucially, without the need for generating molecular descriptors or acquiring a reference standard. Additionally, a purely non-targeted approach outlined can allow for the calculation of RF for features without the need for identification or a reference spectrum.

{"title":"New strategies for non-targeted quantification in comprehensive two-dimensional gas chromatography: The potential of reconstructed TIC response factor surfaces","authors":"Jason Devers, David I. Pattison, Asger B. Hansen, Jan H. Christensen","doi":"10.1016/j.chroma.2025.465811","DOIUrl":"10.1016/j.chroma.2025.465811","url":null,"abstract":"<div><div>Comprehensive two-dimensional gas chromatography (GC × GC) offers unrivaled peak capacity and the ability to resolve and characterize hundreds to thousands of compounds within complex environmental samples. Knowledge of their concentrations is essential in assessing their toxicological and regulatory relevance; however, reliable quantification typically requires concurrent analysis of an authentic standard for each compound. Response factors (RF) may be used to estimate the concentration of a compound without the need for its respective standard, but this is not routinely employed in gas chromatography-mass spectrometry (GC–MS). This study demonstrates that GC × GC offers a new opportunity for the calculation of RFs and estimating a compounds concentration via the creation of 2D total ion current (TIC) response factor surfaces (RFS). A new method, linking a compounds retention time coordinate to its RF using a reconstructed TIC approach, was used to calculate the concentration of 27 compounds in both solvent and effluent wastewater matrix. Using both suspect screening and non-targeted methodologies, average fold change errors of 1.58 and 1.83 respectively were determined for the novel RFS approach. The approach was compared to an RF prediction model utilizing molecular descriptors, using a genetic algorithm, partial least squares regression (GA-PLS) model. The accuracy of the RFS method demonstrates its potential in the fields of suspect screening and non-targeted analysis, where realistic concentration estimates are required. The RFS approach delivers comparable accuracy in concentration prediction compared to computational approaches for determining RFs, but crucially, without the need for generating molecular descriptors or acquiring a reference standard. Additionally, a purely non-targeted approach outlined can allow for the calculation of RF for features without the need for identification or a reference spectrum.</div></div>","PeriodicalId":347,"journal":{"name":"Journal of Chromatography A","volume":"1747 ","pages":"Article 465811"},"PeriodicalIF":3.8,"publicationDate":"2025-02-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143488510","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Dual-mode monolithic column with zwitterion antifouling and aptamer affinity for online specific recognition of okadaic acid

IF 3.8 2区化学 Q1 BIOCHEMICAL RESEARCH METHODS

Journal of Chromatography A

Pub Date : 2025-02-24 DOI: 10.1016/j.chroma.2025.465819

Qi Peng , Yan Ye , Xinglin Wu , Chenchen Lin , Xucong Lin , Qibiao Weng , Qinai Chen

Developing a functional media for precise identification of trace shellfish toxin would underpin the effective assessment of marine pollution. Herein, a novel monolithic column with a dual-mode strategy integrating antifouling and aptamer bionic affinity recognition was proposed for online specific identification of the marine toxin okadaic acid (OA). The zwitterionic monomer 2-(methacryloyloxy)ethylphosphorylcholine (MPC) and aptamers were synergistically employed to enable efficient reduction of matrix interferences and selective capture of target OA. Preparation optimization, characterization, and fouling-resistant mechanism of the dual-mode bionic monolith were evaluated. The zwitterion phosphorylcholine MPC introduced into the monolith significantly improved the fouling resistance to biomass substrates, meanwhile the aptamers were able to provide a high specific recognition capacity. Coupled with LC-MS, the as-prepared monolith provided an effective approach for highly selective and sensitive identification of OA. Good recovery yields of over 90 % in shellfish tissue extracts and human serum were achieved with a sensitive limit of detection (LOD) as low as 0.1 ng/mL, as well as excellent specificity and low interference from proteins, fatty acids and analogues. Applied to popular shellfishes (such as clams, mussels, and oysters) and serum samples, trace OA toxin was accurately distinguished and quantified with satisfactory recoveries as 93.8 ± 2.2 % – 99.9 ± 1.9 % (n = 3). Compared to the traditional HLB cartridge and other materials in the LC-MS method, the resulting anti-fouling aptamer monolith provided a more advanced online analysis mode with higher sensitivity and better resolution of OA in biological samples. It might provide an attractive access to an online bionic recognition platform with LC-MS for efficient, anti-interference and sensitive specific detection of trace marine toxin OA in biological samples.

{"title":"Dual-mode monolithic column with zwitterion antifouling and aptamer affinity for online specific recognition of okadaic acid","authors":"Qi Peng , Yan Ye , Xinglin Wu , Chenchen Lin , Xucong Lin , Qibiao Weng , Qinai Chen","doi":"10.1016/j.chroma.2025.465819","DOIUrl":"10.1016/j.chroma.2025.465819","url":null,"abstract":"<div><div>Developing a functional media for precise identification of trace shellfish toxin would underpin the effective assessment of marine pollution. Herein, a novel monolithic column with a dual-mode strategy integrating antifouling and aptamer bionic affinity recognition was proposed for online specific identification of the marine toxin okadaic acid (OA). The zwitterionic monomer 2-(methacryloyloxy)ethylphosphorylcholine (MPC) and aptamers were synergistically employed to enable efficient reduction of matrix interferences and selective capture of target OA. Preparation optimization, characterization, and fouling-resistant mechanism of the dual-mode bionic monolith were evaluated. The zwitterion phosphorylcholine MPC introduced into the monolith significantly improved the fouling resistance to biomass substrates, meanwhile the aptamers were able to provide a high specific recognition capacity. Coupled with LC-MS, the as-prepared monolith provided an effective approach for highly selective and sensitive identification of OA. Good recovery yields of over 90 % in shellfish tissue extracts and human serum were achieved with a sensitive limit of detection (LOD) as low as 0.1 ng/mL, as well as excellent specificity and low interference from proteins, fatty acids and analogues. Applied to popular shellfishes (such as clams, mussels, and oysters) and serum samples, trace OA toxin was accurately distinguished and quantified with satisfactory recoveries as 93.8 ± 2.2 % – 99.9 ± 1.9 % (<em>n</em> = 3). Compared to the traditional HLB cartridge and other materials in the LC-MS method, the resulting anti-fouling aptamer monolith provided a more advanced online analysis mode with higher sensitivity and better resolution of OA in biological samples. It might provide an attractive access to an online bionic recognition platform with LC-MS for efficient, anti-interference and sensitive specific detection of trace marine toxin OA in biological samples.</div></div>","PeriodicalId":347,"journal":{"name":"Journal of Chromatography A","volume":"1747 ","pages":"Article 465819"},"PeriodicalIF":3.8,"publicationDate":"2025-02-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143528765","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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

Effective extraction and sensitive detection of aflatoxins in wheat by polymeric ionic liquid-based magnetic adsorbent with multiple interactions

IF 3.8 2区化学 Q1 BIOCHEMICAL RESEARCH METHODS

Journal of Chromatography A

Pub Date : 2025-02-23 DOI: 10.1016/j.chroma.2025.465813

Yong Man , Juan An , Chenxi Liu , Yaming Sun , Xuemeng Xu , Chenchen Song , Renyong Zhao , Lijun He

In this study, polymeric ionic liquids (PILs) modified magnetic nanoparticles were used to extract four aflatoxins (AFs) from wheat samples, providing a convenient and cost-effective sample preparation technique for AFs detection in the complex food matrix. The extraction parameters were optimized in terms of the amount of adsorbent, adsorption time, type and volume of desorption solvent, desorption time, and salt addition. The results showed that the proposed method had high sensitivity, good repeatability, and wide linear range. The limits of detection (S/N=3) of four AFs were 0.05-0.41 μg kg^-1. The accuracy was also evaluated using spiked wheat samples and acceptable relative recovery of four AFs at different fortification levels were obtained, ranging from 50.3 %-110.4 %. It was indicated that both the anion species and the alkyl chain length of cation in PILs significantly affected the extraction efficiency. Meanwhile, multiple interactions, including hydrogen bonding, π-π and p-π, and hydrophobic interactions between the adsorbent and the AFs, were responsible for the effective extraction.

{"title":"Effective extraction and sensitive detection of aflatoxins in wheat by polymeric ionic liquid-based magnetic adsorbent with multiple interactions","authors":"Yong Man , Juan An , Chenxi Liu , Yaming Sun , Xuemeng Xu , Chenchen Song , Renyong Zhao , Lijun He","doi":"10.1016/j.chroma.2025.465813","DOIUrl":"10.1016/j.chroma.2025.465813","url":null,"abstract":"<div><div>In this study, polymeric ionic liquids (PILs) modified magnetic nanoparticles were used to extract four aflatoxins (AFs) from wheat samples, providing a convenient and cost-effective sample preparation technique for AFs detection in the complex food matrix. The extraction parameters were optimized in terms of the amount of adsorbent, adsorption time, type and volume of desorption solvent, desorption time, and salt addition. The results showed that the proposed method had high sensitivity, good repeatability, and wide linear range. The limits of detection (S/N=3) of four AFs were 0.05-0.41 μg kg<sup>-1</sup>. The accuracy was also evaluated using spiked wheat samples and acceptable relative recovery of four AFs at different fortification levels were obtained, ranging from 50.3 %-110.4 %. It was indicated that both the anion species and the alkyl chain length of cation in PILs significantly affected the extraction efficiency. Meanwhile, multiple interactions, including hydrogen bonding, π-π and p-π, and hydrophobic interactions between the adsorbent and the AFs, were responsible for the effective extraction.</div></div>","PeriodicalId":347,"journal":{"name":"Journal of Chromatography A","volume":"1747 ","pages":"Article 465813"},"PeriodicalIF":3.8,"publicationDate":"2025-02-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143511959","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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

3D microporous metal-organic framework Ca-TCPB as a fiber coating for headspace solid-phase microextraction of polycyclic aromatic hydrocarbons

IF 3.8 2区化学 Q1 BIOCHEMICAL RESEARCH METHODS

Journal of Chromatography A

Pub Date : 2025-02-23 DOI: 10.1016/j.chroma.2025.465814

Jiaomei Yang , Huina Zhou , Yingge Hao , Shufang Tian , Ling Yan , Minghua Lu

Polycyclic aromatic hydrocarbons (PAHs) as a type of persistent organic pollutants in environment can pose serious threat to ecosystem and human health. Herein, a microporous metal-organic framework (MOF) material namely Ca-TCPB [H₄TCPB: 1,2,4,5-tetrakis(4-carboxyphenyl)-benzene] with three-dimensional (3D) structure was synthesized via simple solvothermal method. The Ca-TCPB served as fiber coating of solid-phase microextraction (SPME) to extract and enrich PAHs prior to gas chromatography analysis. The results showed that the established method has a wide linear range (0.005–40 ng⋅mL^-1), high coefficient of determination (R²>0.9961), low detection limit (0.0017–0.003 ng⋅mL^-1), and high enrichment factor (7504–13,932), respectively. In addition, the analytical method was successful detected trace target PAHs in pond water with recoveries in the range of 83.3–114.1 %. The excellent extraction ability of this Ca-TCPB crystalline material for target PAHs can be attributed to strong interactions between Ca-TCPB and PAHs, including π-π stacking interactions and hydrogen bonding interactions. It was shown that Ca-TCPB material as fiber coating material possessed the merits of facile and eco-friendly synthesis process, high enrichment multiples, superior thermal stability (470 °C), and high number of reuse times (75 times). Furthermore, the biocompatible Ca-TCPB is alternative material that are green, safe and sustainable. Therefore, the innovative use of Ca-TCPB material as a fiber coating for HP-SPME in this work opens new horizons for sample preparation and environmental analysis.

{"title":"3D microporous metal-organic framework Ca-TCPB as a fiber coating for headspace solid-phase microextraction of polycyclic aromatic hydrocarbons","authors":"Jiaomei Yang , Huina Zhou , Yingge Hao , Shufang Tian , Ling Yan , Minghua Lu","doi":"10.1016/j.chroma.2025.465814","DOIUrl":"10.1016/j.chroma.2025.465814","url":null,"abstract":"<div><div>Polycyclic aromatic hydrocarbons (PAHs) as a type of persistent organic pollutants in environment can pose serious threat to ecosystem and human health. Herein, a microporous metal-organic framework (MOF) material namely Ca-TCPB [H<sub>4</sub>TCPB: 1,2,4,5-tetrakis(4-carboxyphenyl)-benzene] with three-dimensional (3D) structure was synthesized via simple solvothermal method. The Ca-TCPB served as fiber coating of solid-phase microextraction (SPME) to extract and enrich PAHs prior to gas chromatography analysis. The results showed that the established method has a wide linear range (0.005–40 ng⋅mL<sup>-1</sup>), high coefficient of determination (R<sup>2</sup>>0.9961), low detection limit (0.0017–0.003 ng⋅mL<sup>-1</sup>), and high enrichment factor (7504–13,932), respectively. In addition, the analytical method was successful detected trace target PAHs in pond water with recoveries in the range of 83.3–114.1 %. The excellent extraction ability of this Ca-TCPB crystalline material for target PAHs can be attributed to strong interactions between Ca-TCPB and PAHs, including π-π stacking interactions and hydrogen bonding interactions. It was shown that Ca-TCPB material as fiber coating material possessed the merits of facile and eco-friendly synthesis process, high enrichment multiples, superior thermal stability (470 °C), and high number of reuse times (75 times). Furthermore, the biocompatible Ca-TCPB is alternative material that are green, safe and sustainable. Therefore, the innovative use of Ca-TCPB material as a fiber coating for HP-SPME in this work opens new horizons for sample preparation and environmental analysis.</div></div>","PeriodicalId":347,"journal":{"name":"Journal of Chromatography A","volume":"1747 ","pages":"Article 465814"},"PeriodicalIF":3.8,"publicationDate":"2025-02-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143510652","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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 procedure based on dispersive solid phase extraction and LC-MS/MS for the analysis of perfluoroalkyl and polyfluoroalkyl substances in food contact materials 开发一种基于分散固相萃取和 LC-MS/MS 的程序，用于分析食品接触材料中的全氟烷基和多氟烷基物质

IF 3.8 2区化学 Q1 BIOCHEMICAL RESEARCH METHODS

Journal of Chromatography A

Pub Date : 2025-02-23 DOI: 10.1016/j.chroma.2025.465815

Yang Yang , Jin Wang , Jia Qiu , Yan Luo , Chun Yang , Shali Tang , Hui Cao , Qian Wang , Xiaojing Lai

To monitor per- and polyfluoroalkyl substances (PFAS) in food contact materials (FCMs), an LC-MS/MS method for the simultaneous detection of 35 PFAS was developed and validated in paper and plastic products. Chromatographic and mass spectrometry parameters, extraction solvents, matrix effects in details were studied. The impact of matrix effects on PFAS concentration was analyzed, revealing that the matrix enhancement effect was more significant for some PFAS with low concentrations. In order to eliminate the matrix effect and enhance detection accuracy, a straightforward pretreatment method combining methanol ultrasonic extraction with dispersive solid-phase extraction (d-SPE) was established. PFHpA, PFDA, PFTriDA, PFTeDA, PF-3,7-DMOA, HFPO-DA, PFHxS, PFHpS, PFOS, 4:2 FTS, 6:2 FTS, 8:2 FTS, 10:2 FTS, and 6:2 diPAP required further d-SPE extraction with PSA, and other substances could be directly extracted by methanol ultrasonic treatment. The recoveries of the established method for all compounds ranged from 62.40 to 135.80%, with a relative standard deviation (RSD) of 0.15% to 16.81%. The limit of quantitation was between 0.005 and 0.02 mg·kg⁻¹. The method was applied to detect PFAS in 119 FCMs, resulting in the identification of 15 PFAS.

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引用次数: 0

Quantification of Gd species in a tetrameric Gd-based contrast agent using HPLC-ICP-MS

IF 3.8 2区化学 Q1 BIOCHEMICAL RESEARCH METHODS

Journal of Chromatography A

Pub Date : 2025-02-21 DOI: 10.1016/j.chroma.2025.465808

Sonja Weishaupt , Wiebke Holkenjans , Sandra Balzer , Anne Jeremias , Michael Sperling , Martin Vogel , Uwe Karst

This study presents a newly developed high-performance liquid chromatography-inductively coupled plasma-mass spectrometry (HPLC-ICP-MS) method for quantification of Gd complexes in a tetrameric, macrocyclic Gd-based MRI contrast agent (GBCA). Since for the multimeric GBCA Gadoquatrane, currently in Phase III clinical development, mainly multinuclear Gd complexes are expected as by-products from the route of synthesis, HPLC-ICP-MS is suitable for the quantitative determination of these Gd species. The developed HPLC-ICP-MS method offers high sensitivity and accurate quantification based on external calibration with a generic Gd standard and is thus a powerful alternative to routinely used HPLC-UV in the pharmaceutical industry. The method allows for quantitatively detecting six different multimeric Gd-containing by-products in a Gadoquatrane sample taken from the early process development. A limit of quantification (LOQ) of 38 nmol/L is achieved for monomeric Gd complexes, which allows the quantitative determination of Gd species at levels as low as 0.004 mass% in the product. With this method, unknown Gd-containing by-products in GBCAs even at trace levels can be well assessed regarding their relevance in the further synthesis process optimization and in the drug substance control strategy. The elaborative synthesis of reference compounds for quantification of unknowns may be omitted, which can significantly accelerate the synthesis process optimization.

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引用次数: 0

Strategy for identification of characteristic components from multiphase of Sanwu Huangqin Decoction via UHPLC‒Q-TOF‒MS and UHPLC-QQQ-MS combined with multivariate statistical analysis

IF 3.8 2区化学 Q1 BIOCHEMICAL RESEARCH METHODS

Journal of Chromatography A

Pub Date : 2025-02-21 DOI: 10.1016/j.chroma.2025.465809

Shiqi Wang , Tongyun Wang , Jiang He , Wenyi Mao , Puyang Gong , Jianhua He , Xuecheng Xiao , Shan Lu , Yi Hong , Yujie Guo

Sanwu Huangqin Decoction (SHD), a classic prescription for nourishing yin and clearing heat, is commonly used to treat febrile diseases, erythromelalgia, autoimmune liver diseases, and skin diseases. However, research on the quality standard of SHD is still in its infancy and has focused mainly on single Chinese herbs, with few systematic studies. Currently, traditional Chinese medicine decoctions, as a complex polydisperse system, have attracted widespread attention. It is necessary to establish an integrated and rapid identification strategy for evaluating and controlling the quality of multiphase of SHD. The ingredients in the three phases of SHD were first isolated via the centrifugation‒dialysis technique, and an method was established via ultrahigh-performance liquid chromatography quadrupole time-of-flight mass spectrometry (UHPLC‒Q-TOF‒MS) for discrimination. The identification results and multivariate statistical analysis revealed that the SHD and three phases were clearly clustered, whereas the composition difference between the nanophase state and SHD was the smallest. Moreover, 34 significantly common differential markers were screened out by variable importance for projection (VIP) > 1 and P < 0.05 to construct the orthogonal partial least squares-discriminant analysis (OPLS-DA) regression prediction model. Furthermore, a strategy for potential effective phase identification and quality evaluation index was established based on the absolute quantitative analysis of the 13 characteristic ingredients via ultrahigh-performance liquid chromatography triple quadrupole mass spectrometry (UHPLC-QQQ-MS). The comprehensive strategy of qualitative analysis combined with absolute quantitative analysis may be an effective tool for the identification and discrimination of SHD and the potential effective phase state. These findings could provide a significative reference for further revealing the material basis and determining the quality control indicators of SHD.

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引用次数: 0