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博碩士論文 etd-0610117-155839 詳細資訊
Title page for etd-0610117-155839
論文名稱
Title
熱脫附結合火焰誘導大氣壓力化學游離質譜法之開發及應用
Development and Applications of Thermal Desorption Combined with Flame-induced Atmospheric Pressure Chemical Ionization Mass Spectrometry
系所名稱
Department
畢業學年期
Year, semester
語文別
Language
學位類別
Degree
頁數
Number of pages
85
研究生
Author
指導教授
Advisor
召集委員
Convenor
口試委員
Advisory Committee
口試日期
Date of Exam
2017-07-11
繳交日期
Date of Submission
2017-07-11
關鍵字
Keywords
大氣質譜法、熱脫附、農藥殘留、火焰誘導大氣壓力化學游離法、刑事鑑定
flame atmospheric pressure chemical ionization, thermal desorption, ambient mass spectrometry, food safety, forensic science
統計
Statistics
本論文已被瀏覽 5672 次,被下載 25
The thesis/dissertation has been browsed 5672 times, has been downloaded 25 times.
中文摘要
質譜儀一直是分析化學領域上強而有力的儀器,因其具有高選擇性及高靈敏度,可用於鑑定分析物的組成。由於傳統分析上必須在真空的條件下操作,且因搭配層析系統必須經過繁複的前處理步驟。自2004年由G.R. Cooks研究團隊發表脫附電噴灑游離法(Desorption Electrospray Ionization, DESI) 將質譜分析帶進一個嶄新的領域後,一個新穎的概念隨之產生,稱為大氣質譜法(Ambient mass spectrometry)。目前已有有許多技術不斷的被開發出來,而大氣質譜法顧名思義即是在大氣壓下進行操作,其特點為樣品幾乎不需或只需少量的前處理、置換樣品方便及能夠進行快速、即時且高通量的分析。
第一部分的研究利用熱脫附(Thermal desorption)結合火焰誘導大氣壓力化學游離法(Flame-induced Atmospheric Pressure Chemical ionization, FAPCI)開發出一套新穎的技術,其原理是利用依熱脫附裝置將分析物進行熱脫附,並藉由熱氣流帶至火焰游離區域,使氣態中性分析物與火焰所產生之反應性離子進行分子離子反應(Ion-molecule Reaction),藉由質子轉移使分析物攜帶電荷。實驗流程是利用採樣探針進行採樣,再放入熱脫附系統中使分析物氣化再由後游離源使其游離,並進入質譜儀進行分析。最後再以高溫火焰對探針進行清潔的,清潔過後即可進行下一次的分析,整個分析流程30秒內即可完成。與過往熱脫附電噴灑游離法(Thermal Desorption Electrospray Ionization, TD-ESI)相比,有更好的游離效率且偵測極限來得更低,相對標準偏差為5%。
第二部分研究利用此技術應用於多個領域上,如:蔬果表面農藥殘留、環境中物件的塑化劑分析及刑事鑑定等等。對於大多樣品進行快速定性的分析外,此技術亦具有半定量的能力,對於農藥偵測極限可達10 ppb ,尿液中毒品檢測偵測極限亦可達20 ppb。而此技術因搭配採樣探針進行樣品採樣,故不限樣品的形狀大小、外觀、表面平整度及游離源介面等影響,跳脫出必須在實驗室下才能進行分析的限制。
Abstract
The mass spectrometer is well-known of beinga powerful instrument in the field of analytical chemistry because of its high selectivity and high sensitivity. It can be used to identify the composition of the analyte. The traditional analysis must manipulate under vacuum condition. Withgas chromatography or liquid chromatography system,the whole processusually requiresophisticate pre-treatment steps and consumed large amount of time. In 2004, the G.R. Cooks research team published desorption electrospray ionization (DESI) on science, which brings mass spectrometry into a new field called the ambient mass spectrometry(AMS). This technique allows real-time, direct, rapid and high-throughput analysis with less or no sample pretreatment.
  Flameatmospheric pressure chemical ionization(FAPCI)is a new APCI method that generates a variety ofprimaryions such as CHO+, H3O+, H3O+(H2O)nin a flame forreacting and ionizing analytes through ion-molecule reactions (IMRs). In this study, thermal desorption(TD)combined with flame-induced atmospheric pressure chemical ionization mass spectrometry(FAPCI/MS)is developed. The TD-FAPCI/MS consists of a heated oven, oxyacetylene flame, and mass analyzer. A stainless steel probe was used to scrape sample surfaces andit was subsequently inserted into a heated oven for thermalevaporation. A stream of heated nitrogen gas carried gaseous analytes from the oven to the IMRs ionization region with charged species generated from the flame.
  TD-FAPCI/MS was used for direct detectionof plasticizer and trace explosives in objects. The analysis of pesticides on fruits and vegetables was also demonstrated without visible sample damage.As the extraction and separation processes were unnecessary, each sample analysis was completed in 15 s. To characterize drugs and metabolites in bio-fluids, sample solutions were extracted by organic solvents for10 seconds, followed by TD-FAPCI/MS analysis.The detection limits for illegal drugs in urine such asamphetamine、ketamine、norketamine、benzoylecgoninewere found to be at low ppb levels.In conclusion, TD-FAPCI/MS is a sensitive, reproducible, quantitative, and rapid technique that can be used for large-scale screeningand high throughputanalysis of food safety and forensic science.
目次 Table of Contents
論文審定書 i
公開授權書 ii
誌謝 iii
摘要 v
Abstract vii
圖目錄 x
表目錄 xiv
第一章、緒論 1
一、前言 1
二、真空游離法(Vacuum Ionization) 2
三、大氣壓力游離法(Atmospheric Pressure Ionization, API) 4
四、大氣質譜法(Ambient Mass Spectrometry, AMS) 8
五、大氣熱脫附游離質譜法(Ambient Thermal Desorption Ionization Mass Spectrometry) 16
六、論文目標 19
第二章熱脫附結合火焰誘導大氣壓力化學游離源之開發 20
一、儀器裝置 20
二、實驗藥品與試劑 27
三、藥品配置 32
四、結果與討論 32
第三章、熱脫附火焰誘導大氣壓力化學游離質譜法在各領域之應用 48
一、對於蔬果表面農藥殘留進行快速篩檢 48
二、對於環境中物件之塑化劑分析 52
三、刑事鑑定 54
第四章、結論 63
五、參考文獻 64
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