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题名: 我国典型沿海区域有机锡污染及砂海螂丁基锡标准参考物质的研究
作者: 张可刚
学位类别: 博士
答辩日期: 2012
授予单位: 中国科学院研究生院
授予地点: 北京
导师: 魏复盛 ; 江桂斌
关键词: 有机锡 ; Organotin ; 沉积物 ; Sediment ; 渔港 ; Fishing ports ; 珠江口 ; Pearl River Estuary ; 标准参考物质 ; Certified reference material
其他题名: Organotin Pollution in Selected Coastal Areas of China and Assessment of a New Mya arenaria Reference Material for Butyltin Compounds
中文摘要:       随着有机锡化合物在船体防污涂料添加剂、聚氯乙烯塑料添加剂、工业催化剂等工业产品中的广泛应用,大量的丁基锡化合物进入到海洋环境中,造成了严重的海洋污染,对海洋水生生物产生了巨大的威胁。及时准确的弄清有机锡的污染状况对海洋环境保护与管理具有重要的意义。复杂环境介质样品的分析需要经过繁琐的前处理,往往造成对测量结果的偏差,而标准参考物质的研制则为测量结果的准确性提供了保证。 本文研究了我国典型沿海渔港和珠江口表层沉积物中有机锡的污染状况。在渔港表层沉积物中,丁基锡是有机锡主要的存在形态,一丁基锡(MBT)的浓度明显高于二丁基锡(DBT)和三丁基锡(TBT)。不同渔港表层沉积物中有机锡浓度差别很大,其中位于南海的各渔港(深圳蛇口港、珠海香洲港、澳门湾仔港、茂名水东港、三亚港渔业区)丁基锡的浓度要高于位于东海(舟山沈家门港、宁波北仑港、厦门西港)和黄海(青岛沙子口港)的渔港中丁基锡的浓度。除位于东海的各渔港外,其他渔港一苯基锡(MPhT)污染较为普遍。MBT除来自于TBT的降解外,可能有直接的排放源。珠江口表层沉积物中的有机锡同样以丁基锡为主,其分布同沉积物在珠江口的沉积规律有关。TBT分布于主要的航道上,为近源沉积,船舶防污涂料是其主要的来源。MBT和DBT主要分布于东部沿岸地区,该区沉积物既有近源沉积,又有来自河流的远源沉积。虽然研究区域各渔港和珠江口表层沉积物中有机锡的检出率较高,但浓度水平较低,与文献中报道的相关环境和生态毒理标准相比,其环境和生态毒理风险较低。 环渤海地区软体动物中丁基锡连续监测结果表明,丁基锡化合物在软体动物中普遍存在,浓度范围为<1.1 至 765.0 ng Sn g-1 (干重)。各城市软体动物中丁基锡污染水平不一,其中威海、烟台、天津、北戴河、葫芦岛污染水平明显高于其他各个城市,尤以威海、北戴河污染最为严重;蓬莱、寿光、营口、大连污染水平较轻,且各年度污染水平相当。不同种类的软体动物具有明显不同的丁基锡富集能力,牡蛎、砂海螂中丁基锡浓度明显高于其他物种。TBT在采样年份具有一定的降低趋势。 对实验室研制的砂海螂丁基锡标准参考物质的特性值进行了检验。结果表明,DBT和TBT能够满足均匀性和一年内稳定性的要求,而MBT均匀性检验和稳定性t检验的结果不甚理想,其不稳定的原因有待于进一步分析。结合三种定值方式,对所研制的标准物质进行了定值,并通过溯源性分析确定了其不确定度。该标准参考物质的成功研制将为我国软体动物中丁基锡成分的分析提供质量保证,在我国近海有机锡污染的监测工作中发挥重要的作用。
英文摘要:
      Marine environment has been seriously polluted by organotin compounds (OTCs) due to their wide application in catalysts, antifouling paints and stabilizers. The high toxicity of organotin compounds has been of great concern for their severe impacts on non-target marine organisms. Ascertaining the status of pollution timely and accurately would be helpful to the protection and management of marine environment. The tanglesome pretreatment procedures needed for many complicated environmental samples may be lead to the error of the research results. However, the preparation of reference materials will give a support of assuring the accuracy of the results. A research has been carried out for the pollution of organotin compounds in surface sediments from selected Chinese coastal fishing ports and Pearl River Estuary. The results showed that butyltin compounds (BTs) were the main species in the sediments from selected fishing ports. The concentrations of monobutytin (MBT) compounds were higher than those of dibutyltin (DBT) and tributyltin (TBT) compounds. The concentrations of OTCs in the sediments varied widely among different sampling locations with much higher butyltin levels at fishing ports close to the South China Sea. MPhT was prevalent in most fishing ports except for those in coast of the East China Sea. BTs were also the main species in the sediments from Pearl River Estuary. The concentrations of BTs have a good relationship with the accumulation of sediments. TBT was mainly found on the navigation channels. Antifouling paints are the main source. MBT and DBT were predominant species in the east coastal area. It was assumed that the MBT and DBT were come from antifouling paints and terrestrial runoff. Although OTCs were detected in the selected areas with high detected frequency, the relatively lower concentrations showed low environmental and ecotoxicological risks. BTs including MBT, DBT and TBT, were determined in mollusks collected from the Chinese Bohai coastal cities in 2007, 2009-2011. BTs compounds were widely existed in the collected samples, with the ranges from <1.1 to 765.0 ng Sn g-1 dry weight. The concentrations of BTs in mollusks varied widely among different locations. The concentrations of BTs in mollusks from Weihai, Tianjin, Yantai, Beidaihe and Huludao were much higher than those from Shouguang, Penglai, Yingkou and Dalian. Bioaccumulation of BTs varied strongly among different organisms. The concentrations of BTs in oysters and Mya arenaria were obviously higher than those in other species. A tendency of decomposition for TBT was observed. The new biological reference material, Mya arenaria, for analysis of BTs prepared by our lab was assessed. DBT and TBT showed good homogeneity and stability in one year at 300 mg levels of intakes. However, the homogeneity in a -test and the stability in a t-test for MBT were unsatisfactory. The reason of instability for MBT would be further analyzed. The certified values of BTs were obtained by the combination of three various certified methods. And the uncertainties of the certified values were calculated through traceability analysis. This new material will be of great support to ensure the quality control of butyltin determination in mollusk, as carried out in environmental monitoring programmes.
内容类型: 学位论文
URI标识: http://ir.rcees.ac.cn/handle/311016/35163
Appears in Collections:环境化学与生态毒理学国家重点实验室_学位论文

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Recommended Citation:
张可刚. 我国典型沿海区域有机锡污染及砂海螂丁基锡标准参考物质的研究[D]. 北京. 中国科学院研究生院. 2012.
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