| 晏浩,孙轶斌,崔洪洋,万祎.Ph4PCl增强电离结合同位素指纹匹配算法的多卤代化合物非靶向鉴定[J].井冈山大学自然版,2023,44(6):22-28 |
| Ph4PCl增强电离结合同位素指纹匹配算法的多卤代化合物非靶向鉴定 |
| NON-TARGETED IDENTIFICATION OF POLYHALOGENATED COMPOUNDS USING THE COMBINATION OF PH4PCL-ENHANCED IONIZATION AND ISOTOPE MATCHING ALGORITHM |
| 投稿时间：2023-08-07 修订日期：2023-10-12 |
| DOI：10.3969/j.issn.1674-8085.2023.06.004 |
| 中文关键词: 多卤代化合物 Ph4PCl增强电离 物质鉴定 |
| 英文关键词: polyhalogenated compounds Ph4PCl-enhanced ionization substance identification |
| 基金项目:国家自然科学基金项目(22206007,22176003,22225601);国家重点研发项目(2021YFC3200803) |
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| 中文摘要: |
| 多卤代化合物是一类典型的有机污染物,具有生物放大性、环境持久性和毒性,对全球生态系统和人类带来健康危害,因此环境中多卤代化合物的鉴定尤为重要。然而在现有分析方法中,多卤代化合物电离效率低、灵敏度差、操作繁琐,导致该类物质的鉴定效率低。本研究首先在液相流动相中添加四苯基氯化鏻(Ph4PCl),能普遍增强多卤化合物的电离和灵敏度,而且为了快速高效对多卤代化合物信号进行鉴定,还开发了快速筛选多卤代化合物分子式的同位素指纹匹配算法。将Ph4PCl氯增强电离和算法结合用于城市污水中多卤代化合物的扫描分析,共鉴定出356个多卤代化合物,包括81个已知多卤代化合物(20个短链氯化石蜡、21个中链氯化石蜡、29个长链氯化石蜡和11个超短链氯化石蜡),以及275个未知多卤代化合物。未知物质通过串级质谱结构分析,包括113个含氧氯化石蜡结构类似物、97个氯化石蜡亚硝酸酯、54个含硫氯化石蜡结构类似物和11个溴代烷烃。可见,Ph4PCl增强电离与同位素指纹匹配算法的结合分析,才能实现环境中已知和未知多卤代化合物的全面快速扫描和鉴定。 |
| 英文摘要: |
| The polyhalogenated compounds are typical organic pollutants known for their bioaccumulation,persistence and toxicity, posing significant health risk to global ecosystems and human. Thus, the identification of the polyhalogenated compounds in environment is very important. However, the current analytical methods for the identification of the polyhalogenated compounds suffer from low ionization efficiency, poor sensitivity, and complex procedures, leading to low identification efficiency. In this study, we firstly introduced tetraphenylphosphonium chloride(Ph4PCl) into the liquid chromatography-mass spectrometry to enhance the ionization of the polyhaloalkyl compounds. Then, a novel isotopic fingerprint-matching algorithm was developed based on the isotopic patterns of the compounds to efficiently identify the polyhalogenated compounds. Based on the combination of Ph4PCl-enhanced ionization and isotopic fingerprint-match method, 356 polyhalogenated compounds were successfully identified in the demostic wastewater samples. Among the identified compounds,81 known polyhalogenated compounds included 20 short-chain, 21 median-chain, 29 long-chain, and 11 very short-chain chlorinated paraffins, and 275 unknown polyhalogenated compounds were consisted of 113 oxygencontaining chlorinated paraffins(CPOxs), 97 chlorinated paraffin nitroesters(CPNO3s), 54 sulfur-containing chlorinated paraffins(CPSxs), and 11 Br-containing alkyl compounds. The established method realized the comprehensive and efficient identification of polyhalogenated compounds in environment. |
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