Nontarget and Target Screening of Organohalogen Compounds in Mussels and Sediment from Hiroshima Bay, Japan: Occurrence of Novel Bioaccumulative Substances

Nontarget and Target Screening of Organohalogen Compounds in Mussels and Sediment from Hiroshima Bay, Japan: Occurrence of Novel Bioaccumulative Substances
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DOI:
10.1021/acs.est.9b06998
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发表时间:
2020-05-05
影响因子:
11.4
通讯作者:
Kunisue, Tatsuya
Kunisue, Tatsuya
中科院分区:
环境科学与生态学1区
文献类型:
--
作者:
Goto, Akitoshi;Nguyen Minh Tue;Kunisue, Tatsuya

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最近的筛选调查表明,海洋环境中存在的未知卤化化合物的含量与持久性有机污染物相当。然而,其在海洋生物中的接触水平和分布以及生物累积潜力仍不清楚。本研究采用二维气相色谱-高分辨飞行时间质谱(GCxGC-HRToFMS)和磁扇形GC-HRMS的综合分析方法,对2012年和2018年采集自日本广岛湾的贻贝和沉积物样品中的有机卤素化合物(OHCs)进行了非靶/靶筛选。通过GCXGC-HRToFMS的非靶分析显示,在贻贝中检测到约60种OHC,包括分子式为C9 H6 Br 3ClO、C9 H5 Br 4ClO和C9 H4 Br 5ClO的未知混合卤代化合物(UHC-Br 3 -5Cl)。有趣的是,贻贝样本中的UHC-Br 3 -5Cl浓度(通过GC-HRMS进行了半定量)在所有调查地点均与持久性有机污染物的浓度相当或高于持久性有机污染物的浓度,并且其地理分布模式与其他OHC不同。这些结果表明,UHC-Br 3 -5Cl在广岛湾沿岸沃茨中普遍存在,并有特定的来源。对贻贝(纳克/克液重)和沉积物(纳克/克总有机碳)的配对样本组估算的UHC-Br 3 -5Cl的生物群-沉积物累积因子比具有相似K(o)w值的持久性有机污染物的生物群-沉积物累积因子高1个数量级,表明其具有较高的生物累积潜力。
Recent screening surveys have shown the presence of unknown halogenated compounds in the marine environment at comparable levels to persistent organic pollutants (POPs). However, their exposure levels and profiles in marine organisms and bioaccumulative potentials remain unclear. The present study performed nontarget/target screening of organohalogen compounds (OHCs) in mussel and sediment samples collected from Hiroshima Bay, Japan, in 2012 and 2018 by using integrated analyses of two-dimensional gas chromatography-high resolution time-of-flight mass spectrometry (GCxGC-HRToFMS) and magnetic sector GC-HRMS. Nontarget analysis by GCXGC- HRToFMS revealed the detection of approximately 60 OHCs including unknown mixed halogenated compounds (UHC-Br3-5Cl) with molecular formulae of C9H6Br3ClO, C9H5Br4ClO, and C9H4Br5ClO in the mussel. Interestingly, UHC-Br3-5Cl concentrations in the mussel samples, which were semi-quantified by GC- HRMS, were comparable to or higher than those of POPs at all the locations surveyed, and their geographical distribution patterns differed from those of other OHCs. These results suggest that UHC-Br3-5Cl are ubiquitous in coastal waters of Hiroshima Bay and derived from a specific source(s). The biota-sediment accumulation factors (BSAFs) of UHC-Br3-5Cl, estimated for a paired sample set of mussel (ng/g lw) and sediment (ng/g TOC), were 1 order of magnitude higher than those for POPs with similar log K(o)wvalues, indicating their high bioaccumulative potential.