本文選題：生物可及性 + 二惡英��； 參考：《中國(guó)疾病預(yù)防控制中心》2015年博士論文

【摘要】：本文參考荷蘭RIVM體外消化模型,模擬食物中二惡英類污染物在胃腸內(nèi)的釋放,經(jīng)分析消化液中PCB和PCDD/F的濃度并與食物中原濃度比較,獲得了不同食物中的PCB和PCDD/F在不同烹飪方式下的生物可及性參數(shù),為開展更準(zhǔn)確的膳食暴露評(píng)估工作提供了可具體操作的基礎(chǔ)數(shù)據(jù)。結(jié)合近年污染物監(jiān)測(cè)結(jié)果,得到經(jīng)校正生物可及性的膳食暴露結(jié)果,并與2000年和2007年總膳食暴露結(jié)果做了對(duì)比。本文包括以下五部分內(nèi)容：1,對(duì)國(guó)內(nèi)外圍繞POPs生物可及性研究開展的體內(nèi)、體外實(shí)驗(yàn)及其研究進(jìn)展做了綜述。2,建立了加速溶劑萃取-多維固相柱凈化-程序升溫進(jìn)樣-高分辨磁質(zhì)譜分析的技術(shù),解決了少量低殘留樣本中持久性有機(jī)污染物分析面臨的技術(shù)難題。該技術(shù)在2 μL-40μL的進(jìn)樣范圍內(nèi)線性良好,血液分析的樣品量需求可由10 mL左右降低至1-2 mL,極大地提高了方法的靈敏度。為未來采用動(dòng)物實(shí)驗(yàn)對(duì)體外消化實(shí)驗(yàn)結(jié)果進(jìn)行驗(yàn)證時(shí),可能需要的小樣品量血液檢測(cè)、以及PCB和PBDE代謝產(chǎn)物分析,提供了有力技術(shù)支撐。3,探討了影響體外胃腸模型的因素,建立了適合食品中PCB類POPs生物可及性研究的RIVM模型。重點(diǎn)考察了烹飪過程對(duì)生物可及性的影響,獲得了水煮和油炒兩種烹飪方式下大米、青菜、牛肉、雞蛋、魚肉等食物中PCDD/F和PCB的生物可及性數(shù)據(jù)：水煮大米PCDD/F的生物可及性介于5-10%,經(jīng)過油炒烹飪提高到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%之間,PCB的生物可及性在28.46%到95.56%之間。水煮青菜PCDD/F的生物可及性介于0.3-3.4%,經(jīng)過油炒提高到12.4-19.0%；PCB的生物性由2.0-7.7%提高到20.9-50.0%。水煮雞蛋PCDD/F的生物可及性介于7.3-12.4%,經(jīng)過油炒提高到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%,經(jīng)過油炒提高到22.4-31.4%；PCB的生物性由41.4-59.0%提高到69.4-85.0%。水煮淡水魚PCDD/F的生物可及性介于6.1-13.0%，經(jīng)過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,對(duì)我國(guó)2009年全國(guó)海產(chǎn)品,2012年乳制品,2013年和2014年乳制品、豬肉、牛肉和淡水魚中二惡英類化合物監(jiān)測(cè)結(jié)果做了總結(jié)。利用這些數(shù)據(jù),結(jié)合膳食消費(fèi)數(shù)據(jù)和生物可及性參數(shù),計(jì)算得到浙江省居民二惡英類污染物經(jīng)校正的膳食暴露量,結(jié)果介于13.0 pg TEQ/人日(煮)至41.8 pg TEQ/人日(炒)之間(均值27.4 pg TEQ/人日),與全國(guó)總膳食調(diào)查得到的全國(guó)平均水平比較接近(2000年:29.3 pg TEQ/人日；2007年：32.2 pg TEQ/人日)。表明本研究獲得的生物可及性參數(shù)用于暴露評(píng)估,與總膳食研究獲得的結(jié)果具有可比性,有望成為總膳食研究的有力驗(yàn)證和有益補(bǔ)充。5,初步探討了PCB代謝產(chǎn)物OH-PCB的分析技術(shù)。確立了以三甲基硅烷化重氮甲烷作為衍生試劑生成MeO-PCB的優(yōu)化衍生條件,確定了適合高分辨質(zhì)譜-同位素稀釋法測(cè)定MeO-PCB和MeO-PBDE各單體的精確質(zhì)量數(shù),得到了十余種MeO-PCB標(biāo)準(zhǔn)品在60 m DB-5MS色譜柱上的出峰順序,為下一步組織樣品中這些代謝物分析奠定了基礎(chǔ)。
[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.
【學(xué)位授予單位】：中國(guó)疾病預(yù)防控制中心
【學(xué)位級(jí)別】：博士
【學(xué)位授予年份】：2015
【分類號(hào)】：R114

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