食品中二恶英类化合物生物可及性研究及其在膳食暴露评估中的应用

发布时间：2018-06-12 06:32

本文选题：生物可及性 + 二恶英　；参考：《中国疾病预防控制中心》2015年博士论文

【摘要】：本文参考荷兰RIVM体外消化模型,模拟食物中二恶英类污染物在胃肠内的释放,经分析消化液中PCB和PCDD/F的浓度并与食物中原浓度比较,获得了不同食物中的PCB和PCDD/F在不同烹饪方式下的生物可及性参数,为开展更准确的膳食暴露评估工作提供了可具体操作的基础数据。结合近年污染物监测结果,得到经校正生物可及性的膳食暴露结果,并与2000年和2007年总膳食暴露结果做了对比。本文包括以下五部分内容：1,对国内外围绕POPs生物可及性研究开展的体内、体外实验及其研究进展做了综述。2,建立了加速溶剂萃取-多维固相柱净化-程序升温进样-高分辨磁质谱分析的技术,解决了少量低残留样本中持久性有机污染物分析面临的技术难题。该技术在2 μL-40μL的进样范围内线性良好,血液分析的样品量需求可由10 mL左右降低至1-2 mL,极大地提高了方法的灵敏度。为未来采用动物实验对体外消化实验结果进行验证时,可能需要的小样品量血液检测、以及PCB和PBDE代谢产物分析,提供了有力技术支撑。3,探讨了影响体外胃肠模型的因素,建立了适合食品中PCB类POPs生物可及性研究的RIVM模型。重点考察了烹饪过程对生物可及性的影响,获得了水煮和油炒两种烹饪方式下大米、青菜、牛肉、鸡蛋、鱼肉等食物中PCDD/F和PCB的生物可及性数据：水煮大米PCDD/F的生物可及性介于5-10%,经过油炒烹饪提高到15-20%；PCB的生物性由10-15%提高到30-80%。奶粉中PCDD/F的生物可及性在25.73%到30.50%之间,PCB的生物可及性在28.46%到95.56%之间。水煮青菜PCDD/F的生物可及性介于0.3-3.4%,经过油炒提高到12.4-19.0%；PCB的生物性由2.0-7.7%提高到20.9-50.0%。水煮鸡蛋PCDD/F的生物可及性介于7.3-12.4%,经过油炒提高到11.0-23.5%；PCB的生物可及性由20.4-43.4%提高到39.4-85.0%。水煮牛肉PCDD/F的生物可及性介于5.9-12.1%,经过油炒提高到22.4-31.4%；PCB的生物性由41.4-59.0%提高到69.4-85.0%。水煮淡水鱼PCDD/F的生物可及性介于6.1-13.0%，经过油炒生物可及性提高到19.9-36.6%；PCB的生物可及性由18.2-60.6%提高到59.4-103%。4,对我国2009年全国海产品,2012年乳制品,2013年和2014年乳制品、猪肉、牛肉和淡水鱼中二恶英类化合物监测结果做了总结。利用这些数据,结合膳食消费数据和生物可及性参数,计算得到浙江省居民二恶英类污染物经校正的膳食暴露量,结果介于13.0 pg TEQ/人日(煮)至41.8 pg TEQ/人日(炒)之间(均值27.4 pg TEQ/人日),与全国总膳食调查得到的全国平均水平比较接近(2000年:29.3 pg TEQ/人日；2007年：32.2 pg TEQ/人日)。表明本研究获得的生物可及性参数用于暴露评估,与总膳食研究获得的结果具有可比性,有望成为总膳食研究的有力验证和有益补充。5,初步探讨了PCB代谢产物OH-PCB的分析技术。确立了以三甲基硅烷化重氮甲烷作为衍生试剂生成MeO-PCB的优化衍生条件,确定了适合高分辨质谱-同位素稀释法测定MeO-PCB和MeO-PBDE各单体的精确质量数,得到了十余种MeO-PCB标准品在60 m DB-5MS色谱柱上的出峰顺序,为下一步组织样品中这些代谢物分析奠定了基础。
[Abstract]:In this paper, we refer to the model of Holland RIVM in vitro digestion model to simulate the release of dioxin pollutants in the gastrointestinal tract. By analyzing the concentration of PCB and PCDD/F in the digestive juice and comparing with the central food concentration, the biological accessibility parameters of PCB and PCDD/F in different foods are obtained in different cooking methods, in order to carry out a more accurate dietary exposure assessment. The work provides specific operational basic data. Combined with the results of recent pollutants monitoring, the results of dietary exposure to calibrated bioavailability are obtained and compared with the results of total dietary exposure in 2000 and 2007. This article includes the following five parts: 1, in vivo and in vitro experiments on POPs bioavailability at home and abroad The technology of accelerated solvent extraction - Multidimensional solid phase column purification - temperature programmed sampling - high resolution magnetic mass spectrometry was established, and a technical problem for the analysis of persistent organic pollutants in a small number of low residual samples was solved. The technology was linear in the sampling range of 2 mu L-40 L and the quantity of blood analysis samples. The demand can be reduced from about 10 mL to 1-2 mL, which greatly improves the sensitivity of the method. For the future use of animal experiments to verify the experimental results of digestion in vitro, it may be necessary to detect the sample quantity of blood, as well as the analysis of the metabolites of PCB and PBDE, and provide a strong technical support.3, and discuss the factors affecting the external gastrointestinal model. A RIVM model suitable for the study of PCB POPs bioavailability in food was established. The effect of cooking process on biological accessibility was emphatically investigated. The bioavailability of PCDD/F and PCB in rice, vegetables, beef, eggs and fish in two cooking methods of cooking and oil stir frying were obtained. The bioavailability of PCDD/F in boiled rice was between 5-10%, The bioavailability of PCB is increased from 10-15% to 15-20%, and the biological accessibility of PCDD/F from 10-15% to 30-80%. milk powder is between 25.73% and 30.50%, and the bioavailability of PCB is between 28.46% and 95.56%. The bioavailability of boiled cabbage PCDD/F is between 0.3-3.4%, oil and 12.4-19.0%; PCB's biological nature is increased by 2.0-7.7%. The bioavailability of PCDD/F boiled eggs to 20.9-50.0%. is between 7.3-12.4% and 11.0-23.5%, and the bioavailability of PCB's bioavailability from 20.4-43.4% to 39.4-85.0%. boiled beef PCDD/F is between 5.9-12.1%, after oil stir fry to 22.4-31.4%, PCB biomass is increased from 41.4-59.0% to boiling water. The bioavailability of water fish PCDD/F is between 6.1-13.0%, and the accessibility of fried organisms to 19.9-36.6%; the bioavailability of PCB is increased from 18.2-60.6% to 59.4-103%.4. The monitoring results of dioxin compounds in dairy products, dairy products in 2012, 2013 and 2014, dairy products, pork, beef and freshwater fish in China are summarized. Using these data, combined with dietary consumption data and biological accessibility parameters, the corrected dietary exposure of dioxin like pollutants in Zhejiang province was calculated. The results were between 13 PG TEQ/ days (boiled) to 41.8 PG TEQ/ days (27.4 PG TEQ/ people day) and compared with the national average level of total national dietary survey. Near (2000: 29.3 PG TEQ/ day; 2007: 32.2 PG TEQ/ day). It shows that the biological accessibility parameters obtained in this study are used for exposure assessment, and are comparable to the results obtained from the total dietary study. It is expected to be a powerful validation and beneficial supplement to the total dietary study and a preliminary discussion of the analytical techniques of the PCB metabolite OH-PCB. With three methyl silanate diazonium methane as a derivative reagent, the optimum derivation conditions of MeO-PCB were obtained. The accurate mass number of MeO-PCB and MeO-PBDE monomers was determined by high resolution mass spectrometry isotope dilution method. The peak order of more than ten MeO-PCB standard products on the 60 m DB-5MS column was obtained, which was the next step in the tissue samples. The analysis of metabolites lays the foundation.
【学位授予单位】：中国疾病预防控制中心
【学位级别】：博士
【学位授予年份】：2015
【分类号】：R114

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