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研究生:蔡伊珊
研究生(外文):Tsai,I-Shan
論文名稱:揮發作用對油品化學指紋與特徵因子比值影響之探討
論文名稱(外文):Evaporation effect on the chemical fingerprints and diagnostic ratios of oil
指導教授:高振山高振山引用關係吳素慧吳素慧引用關係
指導教授(外文):Kao Chen-ShanWu Suh-Huey
口試委員:沈俊卿郭政隆
口試委員(外文):Jun-Chin ShenCheng-Lung Kuo
口試日期:2012-06-25
學位類別:碩士
校院名稱:國立聯合大學
系所名稱:環境與安全衛生工程學系碩士班
學門:工程學門
學類:環境工程學類
論文種類:學術論文
論文出版年:2012
畢業學年度:100
語文別:中文
論文頁數:144
中文關鍵詞:風化揮發漏油生物指標特徵因子
外文關鍵詞:evaporationoil spillboimarkerdiagnostic ratio
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原油與柴油都有其獨特的生物指標(Biomarker)與化學指紋圖譜,這些特性是否會因不同程度之風化作用所影響頗值得研究。由於油品風化作用機制十分複雜且牽涉很多過程,本研究主要針對油品初期風化作用中的揮發因子進行探討。研究中先將原油與柴油樣品放入風化實驗器皿中,進行長時間自然揮發的風化實驗,實驗為期半年,並將不同風化程度之樣品加以採樣後,以GC-MS進行化學圖譜分析。分析如原油中的飽和烴(SAT)、芳香烴(ARO)等化學指紋,期能從中探究原油與柴油受長期揮發作用影響下之化學指紋圖譜變化趨勢並嘗試以統計方法找出適用的生物指標和特徵因子比值,亦即不易受風化作用影響之特徵因子與比值。此於漏油污染鑑識上就顯得十分重要。
揮發作用研究結果顯示,原油之正烷烴(n-Paraffins)經24小時揮發後C8 、C9已大量揮發,經8週後已影響至C16,而揮發實驗經16週後其碳數較低者(C8~C15)已明顯受到影響,C15以前之正烷烴含量幾乎已揮發殆盡;且於16週至24週期間正烷烴分佈僅有微小變異。顯示揮發作用對於正烷烴之影響已接近終了。實驗亦發現雙環類倍半萜烷(Bicyclic Sequiterpanes)經24週揮發作用後,其化學指紋圖譜亦明顯受到影響。研究之另一重點為運用t檢驗法與重覆性限法找出適用於鑑識上的特徵因子比值與生物指標如: 雙環類倍半萜烷、類萜烷(Terpanes)、類固烷(Sterants)、多環芳香烴(PAHs)等化合物。本研究發現經24週揮發作用後,雙環類倍半萜烷特徵因子比值已明顯受到揮發作用影響而不適用,然而類萜烷與類固烷化合物之特徵因子比值則不受影響。本研究結果將可提供漏油污染鑑識時之重要參考。

Crude oil and diesel have unique biomarkers and chemical fingerprint chromatograms and aren’t easily altered unless undergone severe weathering processes. To study effects of weathering processes, particularly evaporation process, oils samples were prepared and underwent natural evaporation process for six months. Oil samples with subsequent evaporation time intervals were taken and analyzed by GC-MS. Tendency of weathering effects and chemical fingerprints of alkanes, aromatic hydrocarbon compounds, etc., were investigated to find out the appropriate biomarkers and diagnostic ratios that were not easily changed via evaporation. Such biomarkers and diagnostic ratios are important for oil spill identification purpose.
For n-paraffins of crude oils, results showed that after 24 hours, significant amount of n-C8 and n-C9, had been evaporated. After 8 weeks n-C16 had been affected greatly and after 16 weeks n-C8 ~ n-C15 had been evaporated almost completely. It was also shown that within 16-24 weeks interval the n-paraffins showed only tiny changed. Furthermore, the degrees of evaporation effect of diagnostic ratios in forensic and biomarker such as bicyclic sequiterpanes, terpanes, sterants, polycyclic aromatic hydrocarbons, etc., can be tested and evaluated by repeatability limit and student’s t-test. Results showed that chemical fingerprints and ratios of bicyclic sequiterpanes had been significantly changed after 24 weeks evaporation. However, diagnostic ratios of terpanes were not affected and so were sterants. The difference can be used as a reference for oil spill pollution forensic.

致謝 II
摘要 III
Abstract I
目錄 III
圖目錄 IV
表目錄 I
第一章 前言 1
1-1背景 1
1-2目的 4
第二章 文獻回顧 5
2-1污染鑑識流程 5
2-2風化作用 6
2-3生物指標 9
2-4特徵因子比值統計分析方法 23
第三章 材料與方法 25
3-1 藥品與材料 25
3-2實驗流程 26
3-3 GC/MS條件設定上機分析 27
3-3-1GC/MS儀器設定 27
3-3-2上機條件 27
3-4模擬風化(揮發因子) 30
3-5油品指紋、生物指標描述 32
第四章 結果與討論 42
4-1揮發作用對原油化學指紋變化之影響 42
4-1-1原油TIC(正烷烴) 42
4-1-2原油生物指標 63
4-2揮發作用對原油特徵因子比值變化之探討 90
4-3揮發作用對重質柴油化學指紋變化之影響 110
4-4揮發作用對重質柴油特徵因子比值變化之探討 119
第五章 結論與建議 124
5-1結論 124
5-2建議 126
參考文獻 127


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