Identification of novel halogenated naturally occurring compounds in marine biota by high-resolution mass spectrometry and combined screening approaches.
Identification of novel halogenated naturally occurring compounds in marine biota by high-resolution mass spectrometry and combined screening approaches.
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通过高分辨率质谱和组合筛选方法鉴定海洋生物群中新型卤代天然化合物。
DOI：
10.1016/j.envpol.2021.117933
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发表时间：
2021
影响因子：
8.9
通讯作者：
Covaci A
中科院分区：
文献类型：
--
作者：
Belova L;Fujii Y;Cleys P;Smielowska M;Haraguchi K;Covaci A
海洋动物、植物或细菌是天然存在的生物活性卤化化合物（NHCs）的来源，如溴酚（bp）、溴苯醚（BAs）和多溴联苯醚（HO-PBDEs、MeO-PBDEs）和溴联苯（HO-BBs、MeO-BBs）的羟基化或甲氧基化类似物。本研究采用液相色谱高分辨率质谱综合筛选方法，结合靶筛选、可疑筛选和非靶筛选，旨在鉴定常用气相色谱方法可能遗漏的新的羟基化NHCs。筛选藻类样品24份，海绵样品4份，其他无脊椎动物样品7份。靶标筛选基于19个可用的bp、（di）OH-BDEs和diOH-BBs参考标准，得到7个明确鉴定的化合物。6-OH-BDE47是检测频率最高的化合物，检测频率为31%。可疑筛选获得了另外两种在藻类样品中鉴定的化合物以及在flamellodysideasp海绵样品中鉴定的17和8种化合物。和Callyspongia sp.。本文提出的可疑筛选结果证实了先前对flamellodysideasp海绵样品进行的研究结果。andCallyspongiasp。此外,inLamellodysideasp。andCallyspongiasp。报道了13种和4种新发现的NHCs，包括七溴化diOH-BDE、单氯化五溴化diOH-BDE、六溴化OH-MeO-BDE等。通过非靶筛选，鉴定出31种和20种多卤化化合物。andCallyspongiasp。样本,分别。根据得到的碎片化光谱，可以在这两个物种中鉴定出多溴化二羟基化二苯氧苯（diOH-PBDPBs），如七-、八-和非溴化diOH-BDPBs。据我们所知，这项研究是关于OH-PBDPBs在环境中存在的第一份报告。
Marine animals, plants or bacteria are a source of bioactive naturally-occurring halogenated compounds (NHCs) such as bromophenols (BPs), bromoanisoles (BAs) and hydroxylated or methoxylated analogues of polybrominated diphenyl ethers (HO-PBDEs, MeO-PBDEs) and bromobiphenyls (HO-BBs, MeO-BBs). This study applied a comprehensive screening approach using liquid chromatography high-resolution mass spectrometry and combining target, suspect and non-target screening with the aim to identify new hydroxylated NHCs which might be missed by commonly applied gas chromatographic methods. 24 alga samples, 4 sea sponge samples and 7 samples of other invertebrates were screened. Target screening was based on 19 available reference standards of BPs, (di)OH-BDEs and diOH-BBs and yielded seven unequivocally identified compounds. 6-OH-BDE47 was the most frequently detected compound with a detection frequency of 31%. Suspect screening yielded two additional compounds identified in alga samples as well as 17 and 8 compounds identified in sea sponge samples ofLamellodysideasp. and Callyspongia sp., respectively. The suspect screening results presented here confirmed the findings of previous studies conducted on sea sponge samples ofLamellodysideasp. andCallyspongiasp. Additionally, inLamellodysideasp. andCallyspongiasp. 13 and 4 newly identified NHCs are reported including heptabrominated diOH-BDE, monochlorinated pentabrominated diOH-BDE, hexabrominated OH–MeO-BDE and others. Non-target screening allowed the identification of 31 and 20 polyhalogenated compounds inLamellodysideasp. andCallyspongiasp. samples, respectively. Based on the obtained fragmentation spectra, polybrominated dihydroxylated diphenoxybenzenes (diOH-PBDPBs), such as hepta-, octa- and nonabrominated diOH-BDPBs, could be identified in both species. To our knowledge, this study is the first report on the environmental presence of OH-PBDPBs.