对羟基苯甲酸酯在我国典型河口潮间带沉积物中的含量水平与分布特征
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摘要
为了解对羟基苯甲酸酯(Parabens)在我国典型河口潮间带沉积物中的含量水平与分布特征,应用HPLC-MS/MS对采自国内典型河口潮间带沉积物样品中6种Parabens污染物(MeP、Et P、PrP、Bu P、Bz P和Hep P)的含量进行测定.测定结果显示,沉积物中Parabens总含量(∑parabens; 6种Parabens单体含量总和)介于2.20—24.5 ng·g~(-1)之间,几何平均含量为8.11 ng·g~(-1),略高于美国(4.93 ng·g~(-1))、日本(5.78 ng·g~(-1))和韩国(6.46 ng·g~(-1))等地所报道的结果.在6种Parabens单体中,MeP为主要的单体(检出率:100%,贡献率:79.9%),其次是PrP (91%,17.7%);而Bu P和Hep P在所有测定的沉积物样品中均未检出.九龙江潮间带沉积物中∑parabens的含量水平最高,其几何平均含量为14.6 ng·g~(-1);而北戴河潮间带沉积物中∑parabens的含量水平最低,其几何平均含量为4.34 ng·g~(-1).主成分分析结果表明各潮间带沉积物样品中Parabens的来源非常相似.
In order to investigate the levels and distributions of parabens in the sediments from typical tidal estuarine zones in China,six paraben analogues,methyl-( Me P),ethyl-( EtP),propyl-( PrP),butyl-( BuP),benzyl-( BzP) and heptyl parabens( HepP) were determined by highperformance liquid chromatography-tandem mass spectrometry( HPLC-MS/MS). The results showed that the total concentration( sum of six parabens: ∑parabens) of parabens in the sediment samples ranged from 2.20 to 24. 5 ng·g~(-1),with a geometric mean value of 8.11 ng·g~(-1). That was slightly higher than those reported from the United States( 4.93 ng·g~(-1)),Japan( 5.78 ng·g~(-1)) and South Korea( 6. 46 ng·g~(-1)). MeP was the predominant compound among the six paraben analogues( detection rate: 100%,percent contribution: 79. 9%),followed by PrP( 91%,17. 7%).Nevertheless,BuP and HepP were not found in any sediment samples. The total concentration of parabens in the sediments from Jiulong Estuary was the highest( geometric mean ∑ parabens:14.6 ng·g~(-1)),while that from Beidai River Estuary was the lowest( 4. 34 ng·g~(-1)). Principal component analysis suggests the similar source of parabens in the sediment samples from tidal estuarine zones in China.
In order to investigate the levels and distributions of parabens in the sediments from typical tidal estuarine zones in China,six paraben analogues,methyl-( Me P),ethyl-( EtP),propyl-( PrP),butyl-( BuP),benzyl-( BzP) and heptyl parabens( HepP) were determined by highperformance liquid chromatography-tandem mass spectrometry( HPLC-MS/MS). The results showed that the total concentration( sum of six parabens: ∑parabens) of parabens in the sediment samples ranged from 2.20 to 24. 5 ng·g~(-1),with a geometric mean value of 8.11 ng·g~(-1). That was slightly higher than those reported from the United States( 4.93 ng·g~(-1)),Japan( 5.78 ng·g~(-1)) and South Korea( 6. 46 ng·g~(-1)). MeP was the predominant compound among the six paraben analogues( detection rate: 100%,percent contribution: 79. 9%),followed by PrP( 91%,17. 7%).Nevertheless,BuP and HepP were not found in any sediment samples. The total concentration of parabens in the sediments from Jiulong Estuary was the highest( geometric mean ∑ parabens:14.6 ng·g~(-1)),while that from Beidai River Estuary was the lowest( 4. 34 ng·g~(-1)). Principal component analysis suggests the similar source of parabens in the sediment samples from tidal estuarine zones in China.
引文
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[15] CARMONA E,ANDREU V,PICO Y. Occurrence of acidic pharmaceuticals and personal care products in Turia River Basin:from waste todrinking water[J]. Science of the Total Environment,2014,484:53-63.
[2] LIAO C Y,LEE S G,MOON H B,et al. Parabens in sediment and sewage sludge from the United States,Japan,and Korea:Spatialdistribution and temporal trends[J]. Environmental Science&Technology,2013,47:10895-10902.
[3] DARBRE P D,BYFORD J R,SHAW L E,et al. Oestrogenic activity of isobutylparaben in vitro and in vivo[J]. Journal of AppliedToxicology,2002,22(4):219-226.
[4] LEMINI C,JAIMEZ R,VILA M E,et al. In vivo and in vitro estrogen bioactivities of alkyl parabens[J]. Toxicology and IndustrialHealth,2003,19(2-6):69-79.
[5]王亮,毛茜慧,袁守军,等.气相色谱-质谱联用法同时测定污水中对羟基苯甲酸酯和甾体雌激素[J].环境化学,2016,35(1):49-56.WANG L,MAO Q H,YUAN S J,et al. Simultaneous determination of parabens and steroid estrogens in sewage water using gaschromatography-mass spectrometry[J]. Environmental Chemistry,2016,35(1):49-56(in Chinese).
[6] OISHI S. Effects of butyl paraben on the male reproductive system in mice[J]. Archives of Toxicology,2002,76(7):423-429.
[7] KANG K S,CHE J H,RYU D Y,et al. Decreased sperm number and motile activity on the F1 offspring maternally exposed to butyl p-hydroxybenzoic acid(butyl paraben)[J]. Journal of Veterinary Medical Science,2002,64(3):227-235.
[8] PENG X Z,XIONG S S,OU W H,et al. Persistence,temporal and spatial profiles of ultraviolet absorbents and phenolic personal careproducts in riverine and estuarine sediment of the Pearl River catchment,China[J]. Journal of Hazardous Materials,2017,323:139-146.
[9] KARTHIKRAJ R,VASU A K,BALAKRISHNA K,et al. Occurrence and fate of parabens and their metabolites in five sewage treatmentplants in India[J]. Science of the Total Environment,2017,593-594:592-598.
[10] LI W H,GAO L H,SHI Y L,et al. Spatial distribution,temporal variation and risks of parabens and their chlorinated derivatives in urbansurface water in Beijing,China[J].Science of the Total Environment,2016,539:262-270.
[11] LIAO C Y,CHEN L X,KANNAN K. Occurrence of parabens in foodstuffs from China and its implications for human dietary exposure[J].Environment International,2013,57:68-74.
[12] LIU W R,ZHAO J L,LIU Y R,et al. Biocides in the Yangtze River of China:Spatiotemporal distribution,mass load and risk assessment[J]. Environmental Pollution,2015,200:53-63.
[13] NUNEZ L,TADEO J L,GARCIA-VALCARCEL A I,et al. Determination of parabens in environmental solid samples by ultrasonic-assistedextraction and liquid chromatography with triple quadrupole mass spectrometry[J]. Journal of Chromatography A,2008,1214:178-182.
[14] NUNEZ L,TURIEL E,MARTIN-ESTEBAN A,et al. Molecularly imprinted polymer for the extraction of parabens from environmental solidsamples prior to their determination by high performance liquid chromatography-ultraviolet detection[J]. Talanta,2010,80:1782-1788.
[15] CARMONA E,ANDREU V,PICO Y. Occurrence of acidic pharmaceuticals and personal care products in Turia River Basin:from waste todrinking water[J]. Science of the Total Environment,2014,484:53-63.