臺灣博碩士論文加值系統

前言：二苯甲酮類(Benzophenones, BPs)物質包含二苯甲酮(Benzophenone, BP)及其衍生物，BPs具內分泌干擾性與生殖毒性，BP為人類可能致癌物，BPs用於固化塑膠包裝材料與油墨以及食品調味劑添加等，因此BPs經由包裝材料遷移至食品或者食品存在BPs，人體可能經飲食暴露BPs，米飯與麵條為我國主食且攝食量較高，因此本研究探討國人經攝食米飯與麵條類食品暴露BPs濃度及健康風險。
方法：依攝食資料庫攝食量分配米飯與麵條採集比例，樣品共80件，一般米飯28件、複合米飯22件、一般麵條14件與複合麵條16件，購買地點為超市並分析熟重；比較四種前處理方法，固液萃取、固相萃取、QuEChERS及FaPEx，搭配超高效液相層析串聯質譜儀(UHPLC-MS/MS)分析米飯與麵條食品中BP及10種BP衍生物(BP-1、BP-2、BP-3、BP-4、BP-8、2-OHBP、4-OHBP、4-MBP、PBZ與M2BB)，並進行方法確效；以變異數分析探討BPs濃度與脂肪含量、包裝材質、是否微波等因子相關性；以蒙地卡羅模擬法計算國人經飲食米飯與麵條食品每人每日BPs暴露劑量、致癌風險與危害商數代表非致癌風險。
結果：前處理方法比較如下，背景值：固液萃取<固相萃取< QuEChERS ≃ FaPEx，萃取率：固相萃取< FaPEx< QuEChERS ≃固液萃取，精密度：固液萃取≃固相萃取< QuEChERS < FaPEx，選擇具較低背景值、較佳萃取率與較低精密度之方法因此，以固液萃取作為前處理方法；偵測極限與定量極限分別為0.01-1及0.02-2 ng/g，檢量線線性皆大於 0.995，精密度 1-29 %，準確度 56–125 %，背景低於定量極限訊號40%，洗出時間± 2.5%內，離子比例± 20%內；80件樣本檢出率與濃度範圍，BP:89%，0.4-7.4 ng/g，2-OHBP:25%，0.4-6.6 ng/g，4-OHBP:1%，0.4-1.4 ng/g，4-MBP:14%，0.4-1.5 ng/g，其他7種BPs皆低於偵測極限；複合米飯與麵條食品脂肪含量與BP濃度具顯著(p = 0.006)且正相關；國人八個年齡層經飲食米飯與麵條類食品暴露BP每日暴露劑量中位數為0.7-8.1 ng/kg/day，致癌風險中位數為2E-09–6E-08，非致癌風險為2E-05–4E-04。
結論：完成米飯與麵條類食品中BPs分析方法建立與方法確效，並應用於樣品分析，0-6歲孩童攝食米飯與麵條類食品每人每日BP劑量為國人八個年齡層中最高，國人致癌風險皆低於1E-06，非致癌風險皆低於1，以上顯示國人經攝食米飯與麵條類食品暴露BP之風險可接受。

Introduction: Benzophenone and its derivatives (BPs) are endocrine disruptors and reproductive toxicants, among which, BP is classified as a human possible carcinogen. BPs are used for curing plastic packaging materials and inks as well as adding flavoring to food, so BPs may migrate from packaging materials to food or BPs may exist in food, and humans may be exposed to BPs through diet. Since rice and noodles are staple foods and their intake is relatively high, this study investigated the exposure to BPs and health risks of rice and noodles consumption Taiwan.
Methods: Based on the Nutrition and Health Surveys in Taiwan (NAHSIT), 80 cereal-based samples (28 general rice, 22 composite rice, 14 general noodles, and 16 composite noodles) were collected and purchased from supermarkets and analyzed for cooked weight. Four pretreatment methods, namely solid-liquid extraction(SLE), solid-phase extraction (SPE), QuEChERS and FaPEx were compared and analyzed using ultra-high performance liquid chromatography coupled with tandem mass spectrometry (UHPLC-MS/MS). Residues of BP and 10 BPs (BP-1, BP-2, BP-3, BP-4, BP-8, 2-OHBP, 4-OHBP, 4-MBP, PBZ and M2BB) were measured. Analysis of variance (ANOVA) was used to explore the correlation between BPs concentration and fat content, packaging material, and with and without microwave. The estimated daily intakes, carcinogenic risks, and non-carcinogenic risks (hazard quotient, HQ) were predicted for eight age groups by using Monte Carlo simulation.
Results: The pretreatment methods were compared as follows, background: SLE < SPE < QuEChERS ≃ FaPEx, extraction rates: SPE < FaPEx < QuEChERS SLE, precision: SLE ≃ SPE < QuEChERS < FaPEx. SLE was selected for the pretreatment method with low background and precision, and high extraction rate. The limits of detections (LODs) and limits of quantifications (LOQs) of BPs for rice and noodles were 0.01-1 and 0.02-2 ng/g, respectively. All analytes exhibited good linearity (r2 > 0.995); the mean precision and accuracy ranges were 1%-29% and 56%-125%, respectively. The background was less than 40% of the LOQs, washout time within ± 2.5%, ion ratio within ± 20%. Of the 11 analytes, 7 were detected below LODs. BP, 2-OHBP, 4-OHBP, and 4-MBP were detected in 89%, 25%, 1% and 14%, respectively, and the ranges were 0.4-7.4 ng/g, 0.4-6.6 ng/g, 0.4-1.4 ng/g and 0.4-1.5 ng/g. A significant correlation was found between fat content and BP level (p = 0.006), in complex rice and noodle foods,. The median of the daily intakes of BP for rice and noodles was 0.7-8.1 ng/kg/day, and the median cancer risk was 2E-09 to 6E-08, and the HQ was 2E-05 to 4E-04.
Conclusion: We developed and validated SLE method involving UHPLC-MS/MS to analyze BP and BPs in rice and noodles. Children (age 0-6 years) had the highest HI of BP among all age groups. The HQ of BP was less than 1 and cancer risk was less than 1E-06, indicating that BP intake through rice and noodles consumption is acceptable in Taiwanese people.

摘要 i
Abstract iii
目錄 v
圖目錄 vii
表目錄 viii
第一章 前言 1
1.1研究背景 1
1.2研究動機 2
1.3研究目的 3
1.4研究架構 4
第二章 文獻回顧 6
2.1 BPs物化性質、用途、毒理研究與管制 6
2.2 食品採樣 13
2.3 食品中BPs前處理與分析 15
2.4 不同因子與食品BPs濃度相關性 25
2.5 BPs風險評估 29
第三章 材料與方法 34
3.1材料 34
3.2採樣方法 38
3.3分析方法 42
3.4 BPs遷移溶出測試方法 51
3.5統計分析 52
3.6健康風險評估 53
第四章 結果與討論 57
4.1建立米飯與麵條BPs前處理方法 57
4.2米飯與麵條BPs方法品保與品管 62
4.3米飯與麵條中BPs濃度 71
4.4影響米飯與麵條食品中BP之因素 75
4.5健康風險評估 78
第五章 結論與建議 84
5.1結論 84
5.2建議 85
參考文獻 86
附錄一 樣品清單 95
附錄二 待測物訊號 100

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