Please use this identifier to cite or link to this item: http://hdl.handle.net/11455/90585
標題: Determination of drug residues in food and biological samples by using QuEChERS combined with liquid chromatography-tandem mass spectrometry
QuEChERS 前處理技術結合液相層析串聯質譜術 於食品及生物樣品中藥物殘留之分析
作者: 王培成
Pei-Cheng Wang
關鍵字: QuEChERS
LC-MS/MS
cyromazine
melamine
illicit drugs
QuEChERS
液相層析串聯質譜術
賽滅淨
三聚氰胺
濫用藥物
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摘要: The aim of this study is to investigate a quick, easy, cheap, effective, rugged and safe (QuEChERS) sample preparation method coupled with liquid chromatography tandem-mass spectrometry (LC-MS/MS) for trace analysis of drugs residues in food and biological samples. The first part of this study was to develop a rapid and sensitive method for the simultaneous detection of cyromazine and melamine in chicken eggs using the QuEChERS method coupled with LC-MS/MS. The optimal extraction solvent for the liquid-liquid extraction was 5 mL of acetonitrile with a 0.1M hydrochloric acid aqueous solution (99.5 : 0.5, v/v). The extract was cleaned with 0.5 g of anhydrous magnesium sulfate and 10 mg of graphitized carbon black. The detection limits were 1.6 ng g-1 for cyromazine and 8 ng g-1 for melamine, and the quantitation limits were 5.5 ng g-1 for cyromazine and 25 ng g-1 for melamine. The recoveries of cyromazine and melamine in the spiked egg samples were 83.2% and 104.6%, respectively, with an relative standard deviation (RSD) of less than 18.1%. The intra-day and inter-day precisions, represented by the RSD ranged from 1.5% to 8.8% and 6.8% to 14.3%, respectively. The proposed method was tested by analyzing chicken eggs from the markets and from the veterinary medicine laboratory. The concentrations of cyromazine and melamine detected in these samples were in the range of 20 to 94 ng g-1. The results demonstrated that the QuEChERS method combined with LC-MS/MS is a simple, rapid and inexpensive method for the analysis of cyromazine and melamine in eggs. The second part was to develope a fast screening and high-throughput method for the analysis of mulitclassed illicit drugs in human urine by using QuEChERS coupled with LC-HESI-MS/MS. The target illicit drugs are including stimulants, hallucinogens, opioids, benzodiazepines, dissociative anesthetics, and new synthetic cannabinoids. The optimal conditions of the QuEChERS extraction method consisted of 2 mL of acetonitrile with 0.5 g sodium acetate and 5 mg C18-modified silica in 1mL urine sample. The limits of detection and quantification ranged from 0.01 to 2.7ng mL-1 and from 0.03 to 9 ng mL-1, respectively. The recoveries of the illicit drugs ranged from 74% to 117%, with a relative standard deviation (RSD) less than 16%. The RSD of intra- and inter-day precisions ranged from 0.3% to 16% and 0.7% to 20%, respectively. The proposed method was tested by analysis of suspected urine samples from a drug-testing laboratory. The concentrations of the detected illicit drugs ranged from 7 to 14460 ng mL-1. The results demonstrated that the QuEChERS method combined with LC-MS/MS is a simple, rapid, and inexpensive technique for the detection and analysis of illicit drugs in human urine.
本 研 究 主 要 探 討 一 快 速 (Quick) 、 簡 單 (Easy) 、 便 宜 (Cheap) 、 有 效(Effective) 耐用 (Rugged) 及安全(Safe) 的QuEChERS 萃取技術並結合質譜術,、於不同複雜基質中微量分析物之偵測。因此研究分為兩部分,一為以 QuEChERS萃取法結合液相層析串聯質譜儀分析市售雞蛋中殘留農藥賽滅淨及其代謝物三聚氰胺;另一為以 QuEChERS 結合液相層析串聯質譜術於高通量快速篩檢尿液中一至四級濫用藥物之研究。 利用 QuEChERS 萃取技術結合液相層析串聯質譜儀分析雞蛋中微量賽滅淨及三聚氰胺實驗結果顯示,於 1 克均質雞蛋樣品下經加入 5 毫升含 0.05%鹽酸之 乙腈溶劑進行液液萃取,經離心後萃取液加入 10 毫克活性碳(GCB)進行分散式 固相萃取淨化。其實驗結果顯示檢量線之線性範圍可得10~1000 ng g-1,最低偵測極限為1.6~8 ng g-1 。於添加不同濃度25、100、500 ng g-1 賽滅淨及三聚氰胺之雞蛋樣品分析,其回收率介於83.2%~104.6%。其精密度介於1.5%~14.3%。此方法成功用於雞蛋樣品中賽滅淨及三聚氰胺之檢測,並應用於 2 個經動物實驗之雞蛋樣品及 8 個市售雞蛋真實樣品分析,於經動物實驗之雞蛋樣品測得賽滅淨66~20 ng g-1 及三聚氰胺 94 ng g-1。 利用QuEChERS萃取技術成功應用於雞蛋基質中微量分析物之萃取後,探討此方法應用於人體尿液樣品內高通量濫用藥物篩檢分析。以QuEChERS萃取技術結合液相層析串聯質譜儀分析人體尿液中32種濫用藥物之研究。其實驗結果顯示以1毫升人體尿液樣品經添加0.5克醋酸鈉,加入2毫升乙腈進行液相液相萃取,萃取液經5毫克C18吸附劑進行分散式固相萃取淨化。實驗結果顯示檢量線之線性範圍範圍介於0.5~500 ng mL-1之間,偵測極限為0.01~2.7 ng mL-1。於添加不同濃度10、50、200 ng mL-1濫用藥物尿液分析,其回收率介74%~117%,精密度之相對標準偏差介於0.3%~20%,表示以此技術能用以萃取人體尿液中多種濫用藥物。應用所探討技術於多位濫用藥物嫌疑者真實尿液分析,測得嗎啡(378~1269 ng mL-1)、可待因(517~1804 ng mL-1)、安非他命 (78~1796 ng mL-1)、甲基安非他命 (114~14460 ng mL-1)、MDA (1650 ng mL-1)、MDMA (6267 ng mL-1)、愷他命 (255 ng mL-1)、去愷他命 (1412 ng mL-1)、苯甲基愛哥寧 (102~115 ngmL-1)、古柯鹼 (15~87 ng mL-1)、佐沛眠 (7~60 ng mL-1)、美沙東(35~192 ng mL-1)、三唑他(57 ng mL-1)、JWH-250 (41~152 ng mL-1)、JWH-073 (61~288 ng mL-1)、JWH-018 (135~316 ng mL-1)等多重濫用藥物成分。顯示此方法可有效快速篩檢濫用藥物者尿液中多重殘留藥物之分析。
URI: http://hdl.handle.net/11455/90585
文章公開時間: 10000-01-01
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