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    题名: 以綠色分析化學技術檢測水樣中防曬乳成分的殘留―開發金屬有機骨架材料作為吸附劑之探討
    作者: 邱彥瑜;Qiu, Yan-Yu
    贡献者: 化學學系
    关键词: 綠色分析化學技術檢測;金屬有機骨架材料
    日期: 2022-06-27
    上传时间: 2022-07-13 18:11:51 (UTC+8)
    出版者: 國立中央大學
    摘要: 本研究開發一套具有快速、環境友善的萃取方式檢測二苯基甲酮類化合物 (Benzophenones, 簡稱BPs)在環境水樣中的殘留。由於BPs為紫外線過濾劑,可以減輕有害輻射對皮膚和頭髮的負面影響,因此被廣泛使用在個人護理產品中,它們可能經由游泳、沐浴等與水相關的休閒活動方式或通過污水排放進入環境。相關研究指出,二苯基甲酮類化合物是潛在的內分泌干擾物,在生物系統中不僅含有潛在的危害性,且藉由生物累積的方式,易對環境及人類造成負面影響。
    本研究萃取方法是以金屬有機骨架材料(ZIF-8)結合分散式微固相萃取法 (Zeolitic imidazolate frameworks 8-based dispersive micro solid phase extraction,簡稱ZIF-8-D-µ-SPE) 萃取環境水樣中共五種BPs衍生物,接著利用超高效液相層析串聯電灑游離 (+) −四極桿飛行時間質譜儀 (UHPLC−ESI(+)−QTOF−MS) 進行後續檢測。本方法中所利用的吸附劑為金屬有機骨架材料當中的ZIF-8,因其具有良好的化學與熱穩定性、低成本、高比表面積等,可以有效吸附目標待測物,合成ZIF-8材料的方式為機械力化學合成法,此合成法快速又可以減少溶劑使用量,使整體萃取方法達到綠色分析化學的宗旨。
    透過使用Box−Behnken Design (BBD) 中的變異數分析 (Analysis of variance, 簡稱ANOVA) 優化各項數值因子得到實驗的最佳條件後,利用ZIF-8-D-µ-SPE方式,檢測五種BPs衍生物的偵測極限 (LOD) 為 0.05−7 ng/mL;Intra −day 和Inter−day 的相對標準偏差 (RSD) 低於8 %;而萃取回收率則介在 71 %−112 % 之間,表示本方法呈現良好的精密度及穩定性。在真實環境水樣檢測中,檢測到BP-3和BP-8的微量殘留。
    ;Benzophenones (BPs) are a type of ultraviolet (UV) filters that can absorb UV radiation. They are used in a variety of personal care products to attenuate the negative effects of sunlight harmful radiation on skin and hair. Since benzophenone-type UV filters are widely used, they may enter the environment via wash-off from skin or via sewage discharges. Moreover, benzophenone-type UV filters are potential endocrine-disrupting chemical (EDC). They have attracted much public attention due to the negative effects in humans.
    In this study, we used a simple and environmental−friendly method for the rapid determination of five BPs derivatives in water samples. The target analytes were effectively extracted from water samples using a Zeolitic imidazolate frameworks 8-based dispersive micro solid phase extraction (ZIF-8-D-µ-SPE), and their determination were performed by ultrahigh−performance liquid chromatography and electrospray ionization (+) −quadrupole time−of−flight mass spectrometry (UHPLC−ESI(+)−QTOF−MS). ZIF-8 is known for excellent chemical stability, thermal stability, and high surface area. Its application in sample pretreatment is appropriate for green chemistry, environmental protection, and sustainable development.
    To overcome the challenges in different experimental conditions, the experimental parameters of ZIF-8-D-µ-SPE were screened and optimized by Box-Behnken Design (BBD). The developed method was validated after optimization. The method provided low limits of detection (LODs) ranging from 0.05 to 7 ng/mL; high precisions and reproducibility for both intra- and inter-day analysis (i.e., the relative standard deviations (RSDs) were all less than 8 %); and high accuracy (mean extraction recovery) ranging from 71 to 112 % at different spiked concentration levels. Successfully, the developed method was applied for the analysis of BPs in real water samples.
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