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研究生:蔡文瑜
研究生(外文):Wen-Yu Tsai
論文名稱:天然氣之分子間碳氫同位素及同分異構物之研究:生油岩封閉系統熱裂解實驗
論文名稱(外文):Compound-specific carbon, hydrogen isotopes and isomers analyses of gases generated from source rocks by closed system pyrolysis
指導教授:黃武良黃武良引用關係
指導教授(外文):Wuu-Liang Huang
學位類別:碩士
校院名稱:國立臺灣大學
系所名稱:地質科學研究所
學門:自然科學學門
學類:地球科學學類
論文種類:學術論文
論文出版年:2010
畢業學年度:98
語文別:英文
論文頁數:188
中文關鍵詞:天然氣成熟度同位素丁烷戊烷異構物熱裂解
外文關鍵詞:natural gasmaturitycompound-specific isotopeC4C5 isomerpyrolysis
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  天然氣之同位素及同分異構物為成熟度、來源、產氣過程影響因子之重要指標。本研究利用生油岩封閉系統熱裂解方法,一為瞬時水合熱裂解,進行天然氣之分子間碳氫同位素及同分異構物之研究。另以圍壓熱裂解(金管實驗)進一步探討不同沉積環境所產出之天然氣的丁烷、戊烷同分異構物及成熟度參數之關係。
為了辨認在不同成熟度範圍所生成之氣體同位素組成及化學組份,本研究以台灣北部東坑層之低成熟度煤頁岩,利用瞬時水合熱裂解之人工加熱方法,進行在油窗及氣窗範圍內十個成熟度(0.65 % Ro ~2.25 % Ro) 的實驗。隨後使用氣相層析同位素比質譜儀(GC-IR-MS)分析天然氣之分子間碳氫同位素組成及氣相層析儀(GC)分析其氣體組分。
  實驗結果顯示甲烷、乙烷、丙烷之分子間碳同位素值隨著成熟度之增加有倒轉的趨勢,並隨著成熟度之增加可將其劃分為三群。此外,將δ13Cn vs. 1/n (n為氣體分子之碳數)作圖,亦可發現隨著成熟度之不同可畫分為三群,且其分子間同位素比值呈現出一致性的δ13C3 < δ13C2 > δ13C1。進一步觀察可發現此種成群現象亦呈現於iC4/nC4 vs. iC5/nC5圖中,這暗示著此類型之油母質至少有三種結構複雜之組成。此種同位素倒轉的情形也存在前人研究中,但被解釋為不同來源的油氣混合的現象。然而由我們的研究結果顯示,這種同位素倒轉的現象,亦可由單一來源的生油岩在不同成熟度階段產氣所造成。此外,甲烷之氫同位素值,則隨著成熟度之增加,而有著上升的趨勢。
  在天然氣的組份方面,C1/(C1+C2+C3)、iC4/nC4、iC5/nC5比值大致在油窗內隨著成熟度的增加而遞減,而在氣窗範圍則呈現遞增之現象。比較iC4/nC4和iC5/nC5之關係,可發現熱生成之天然氣其丁烷、戊烷同分異構物比值(iC4/nC4) (iC5/nC5),大約落在1:1的對角線上。本研究另以封閉系統圍壓熱裂解(金管實驗)模擬自然界之產氣情形,目的在於了解產氣過程之天然氣成分變異,並探討有機物的沉積環境對於丁烷及戊烷同分異構物比值之影響,進一步研究氣體組份之成熟度指標的影響程度。實驗生油岩有湖相、海相、陸相之油母質,在溫度320℃、壓力13 MPa下進行,使得樣品達到油窗初期至末期之成熟度(% Ro = 0.79, 0.95, 1.10, 1.34)。
  結果顯示,參數C1/(C1+C2+C3)、iC4/nC4、iC5/nC5皆隨著成熟度增加而遞減,但根據不同類型之沉積環境其比值有所不同。由海相生油岩所產出之天然氣,顯示出最低的C1/(C1+C2+C3)、iC4/nC4、iC5/nC5比值,並隨著成熟度的增加而緩慢遞減,然而由陸相生油岩所產出之氣體,擁有較高之比值,並隨著增加之成熟度快速下降,湖相生油岩之熱生成天然氣,在低成熟度時,呈現變異較大之初始比值,而後隨著成熟度之增加表現出與陸相生油岩類似之趨勢。由實驗結果亦可發現,不同種類生油岩之產氣在油窗內呈現iC4/ nC4 < 0.6及iC5/ nC5< 0.7。進一步探討丁烷及戊烷同分異構物比值可發現,無論何種沉積環境,熱生成之天然氣其丁烷、戊烷同分異構物比值(iC4/nC4) (iC5/nC5),亦落在約1:1的對角線上。配合野外氣田資料,可以發現大部分野外採集之氣體的同分異構物組成顯示出較高之戊烷同分異構物比值(iC5/ nC5),此種現象可能肇因於混合作用、生物降解作用、擴散移棲作用。因此,本研究為天然氣之研究建立一個新指標,可能做為判別天然氣是否為原生或曾經由其他作用之產物。


誌謝 i
摘要 iii
Abstract v
Table of Contents vii
List of Figures ix
List of Tables xiii
Chapter 1 Introduction 1
1.1 Rationales and objectives 1
1.2 Review of previous studies 2
Chapter 2 Samples and Experiments 15
2.1 Samples 18
2.1.1 Hydrous pyrolysis experiment 18
2.1.2 Confined pressure (gold-tube) pyrolysis experiments 19
2.2 Experimental apparatus 21
2.2.1 Pressure vessel 21
2.2.2 Gas chromatography (GC) 21
2.2.2.1 Inlets 23
2.2.2.2 Columns 24
2.2.2.3 Detectors 24
2.3 Experimental procedures 26
2.3.1 Hydrous pyrolysis experiment 26
2.3.2 Confined pressure (gold-tube) pyrolysis experiments 28
2.4 Analysis of source rocks and gases 31
2.4.1 Hydrous pyrolysis 31
2.4.2 Confined pressure pyrolysis 36
Chapter 3 Results 39
3.1 General remark 39
3.1.1 Hydrous pyrolysis experiment 39
3.1.2 Confined pressure pyrolysis experiment 41
3.2 Results of hydrous pyrolysis experiment 41
3.2.1 Carbon and hydrogen isotope ratios from hydrous pyrolysis 41
3.2.2 Molecular composition of gas from hydrous pyrolysis 54
3.2.3 Isotope ratios versus chemical ratios 60
3.3 Results of Confined pressure pyrolysis experiment 62
3.3.1 Molecular composition of gas from confined pressure pyrolysis 62
Chapter 4 Discussions 72
4.1 Hydrous Pyrolysis 72
4.1.1 Carbon isotope ratios 72
4.1.2 Hydrogen isotope ratios 78
4.1.3 Molecular composition of gas 80
4.2 Confined pressure pyrolysis experiment 82
Chapter 5 Conclusions 90
References 92
Appendix I 107
Appendix II 109
Appendix III 133

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