Development of sample extraction and clean-up strategies for target and non-target analysis of environmental contaminants in biological matrices
Development of sample extraction and clean-up strategies for target and non-target analysis of environmental contaminants in biological matrices
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DOI：
10.1016/j.chroma.2015.11.040
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发表时间：
2015-12-24
影响因子：
4.1
通讯作者：
Ramos, Maria Jose Gomez
中科院分区：
文献类型：
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作者：
Baduel, Christine;Mueller, Jochen F.;Ramos, Maria Jose Gomez
最近，作为增加监测分析物数量的手段，多靶分析和非靶筛选方法的趋势越来越大。以前的研究已经开发了生物监测方法，专门专注于只有少数具有相似的物理化学性质的分析物。在本文中，我们提出了一个简单，快速的多残留物的方法，同时提取极性和非极性有机化学品的生物基质，含有高达5%的脂质含量。我们的方法结合了使用气相色谱三重四极杆质谱（GC-QqQ-MS/MS）的靶向多残留分析和使用液相色谱耦合四极杆飞行时间质谱（LC-QTOF-MS/MS）的非靶向筛选补充的多靶向分析。优化的化学提取程序和不同的清洁方法的有效性进行了评估两种生物基质：鱼肌肉（脂质含量类似于2%）和母乳（类似于4%）。为了提取广泛的化学品，用于QuEChERS（快速，简单，便宜，有效，坚固和安全）方法的分配/提取程序作为提取涵盖广泛化合物域的77种目标化合物的初始步骤进行了测试。所有目标分析物都具有不同的物理化学性质（log Kow从-0.3到10不等），并涵盖广泛的活性范围：从极性农药、药品、个人护理产品（PPCPs）到高亲脂性化学品，如多溴二苯醚（PBDE）、多氯联苯（PCB）、多环芳烃（PAH）和有机氯农药（OCP）。探索了多种清除基质中存在的脂质、蛋白质和其他杂质的选择。基于氧化锆的吸附剂作为分散固相萃取（d-SPE）和蛋白质-脂质去除滤筒（Captiva ND Lipids）分别为GC-MS和LC-MS分析提供了最佳结果。通过评价回收率、基质效应、定量限、线性和精密度（日间和日内），对鱼肉和母乳样品的方法进行了充分验证。平均回收率（n = 5）为70和120%之间的相对标准偏差（RSD）小于20%，在大多数情况下。GC-MS/MS LOQ范围为0.08 - 3 μ g/kg，LC-QTOF-MS/MS LOQ范围为0.2 - 9 μ g/kg。所开发的策略被成功地应用于真实的样品的分析;在母乳样品中发现了22种目标分析物，在鱼样品中发现了10种。非目标分析允许检测和鉴定样品中的另外14种污染物和代谢物。(C)2015 Elsevier B. V.版权所有。
Recently, there has been an increasing trend towards multi-targeted analysis and non-target screening methods as a means to increase the number of monitored analytes. Previous studies have developed biomonitoring methods which specifically focus on only a small number of analytes with similar physicochemical properties. In this paper, we present a simple and rapid multi-residue method for simultaneous extraction of polar and non-polar organic chemicals from biological matrices, containing up to 5% lipid content. Our method combines targeted multi-residue analysis using gas chromatography triple quadrupole mass spectrometry (GC-QqQ-MS/MS) and a multi-targeted analysis complemented with nontarget screening using liquid chromatography coupled to a quadrupole time of flight mass spectrometry (LC-QTOF-MS/MS). The optimization of the chemical extraction procedure and the effectiveness of different clean-up methods were evaluated for two biological matrices: fish muscle (lipid content similar to 2%) and breast milk (similar to 4%). To extract a wide range of chemicals, the partition/extraction procedure used for the QuEChERS (Quick, Easy, Cheap, Effective, Rugged and Safe) approach was tested as the initial step for the extraction of 77 target compounds covering a broad compound domain. All the target analytes have different physico-chemical properties (log Kow ranges from -0.3 to 10) and cover a broad activity spectrum: from polar pesticides, pharmaceuticals, personal care products (PPCPs) to highly lipophilic chemicals such as polybrominated diphenyl ethers (PBDEs), polychlorinated biphenyls (PCBs), polycyclic aromatic hydrocarbons (PAHs) and organochloride pesticides (OCPs). A number of options were explored for the clean-up of lipids, proteins and other impurities present in the matrix. Zirconium dioxide-based sorbents as dispersive solid-phase extraction (d-SPE) and protein-lipid removal filter cartridges (Captiva ND Lipids) provided the best results for GC-MS and LC-MS analysis respectively. The method was fully validated for samples of fish muscle and breast milk through the evaluation of recoveries, matrix effects, limit of quantification, linearity and precision (inter-day and intra-day). Mean recoveries (n = 5) were between 70 and 120% with relative standard deviations (RSD) less than 20% in most of the cases. GC-MS/MS LOQs ranged from 0.08 to 3 mu g/kg and LC-QTOF-MS/MS LOQs ranged from 0.2 to 9 mu g/kg. The developed strategy was successfully applied for analysis of real samples; 22 target analytes were found in the breast milk samples and 10 in the fish samples. Non-target analysis allowed the detection and identification of an additional 14 contaminants and metabolites in the samples. (C) 2015 Elsevier B.V. All rights reserved.