澳洲煤岩氣體吸附模式研究

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藍一平(Yi-Ping Lan) 查詢紙本館藏

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應用地質研究所

論文名稱

澳洲煤岩氣體吸附模式研究
(A Study of Adsorptive Functions of Gas in Australian Coals)

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摘要(中)

控制排放二氧化碳以減少大氣中二氧化碳含量是現今相當重要且極需解決的議題之一。在無法開採的煤層中注入二氧化碳是一種永久封存人為排放二氧化碳的有效方法，同時可以進行煤層氣的開採。CO2-ECBM技術可以改善全球暖化以及增加能源，是一種具發展性的新技術。在評估二氧化碳在煤層中的儲量以及甲烷的生產量時，除了現地所測得的數據外，等溫吸附模式的選擇亦是相當重要的因素。因此本研究之目的為藉由煤岩性質與吸附實驗來探討影響氣體吸附之因素與不同吸附模式之擬合效果。一般而言，煤層氣中主要氣體為甲烷，然而在澳洲某些區域之煤層氣中二氧化碳之含量卻高達90%。澳洲煤層氣的特性可能會對二氧化碳地質封存計畫有所影響。本研究利用澳洲雪梨盆地及包溫盆地之煙煤進行工業分析、元素分析、比表面積分析及CO2、CH4的吸附實驗，然後比較四種較常見的吸附模式：Langmuir、BET、D-R與D-A的計算結果，期望能找到最佳的擬合曲線。在這些吸附方程中，Langmuir為最基本且常用的理論方程。煤吸附甲烷氣體的計算結果顯示D-A方程有最佳的擬合效果，其次為Langmuir及D-R， BET則最差。BET方程在相對壓力大於0.8時吸附量會大幅增加導致相對誤差值變大。D-A方程與其他三種吸附方程最大的差異在於多了一個異質性參數，此參數與孔隙組成及分布有一定的相關性，可能使D-A方程能夠更貼切的描述煤吸附氣體的行為。

摘要(英)

Ever since the Kyoto Protocol, controlling carbon dioxide emission and reducing its content in atmosphere are very important environmental issues up to today. One of the effective methods for permanent sequestration of anthropogenic CO2 is to inject CO2 into deep, unminable coal seams and recover coal bed methane at the same time. CO2-ECBM technology had been proved to be very promising to meet the needs of both environment and energy. Besides other external environment factors, capacity of CO2 adsorption and CH4 desorption are the most influencing factors in the selection of sites for the geological storage of CO2. Therefore, the objective of this study is to understand the relationship between gas adsorption and CO2 sequestration, by various experiments for the characterization of Australian coals. Generally speaking, coal seam gas comprises mostly of CH4, CO2, C2H6, and N2. However, some of the Australian coals were reported with significant amount of CO2 up to 90%, which might strongly affect their capacity of CO2 capture and storage (CCS). High to medium volatile bituminous coals from Sydney Basin and Bowen Basin of Australia were selected in this study. Proximate analysis, Ultimate analysis, specific surface area analysis as well as CH4 adsorption experiments were performed. Parameters for difference adsorption functions (Langmuir, BET, D-R and D-A) were thus calculated to fit their adsorption isotherms and the best fitting curve can then be found. In conclude, D-A function exhibits the best fitting result other than Langmuir, D-R and BET functions.

關鍵字(中)

★ 煤
★ Langmuir
★ BET
★ D-R
★ D-A

關鍵字(英)

★ Coal
★ Langmuir
★ BET
★ D-R
★ D-A

論文目次

目錄
中文摘要 i
英文摘要 ii
誌謝 iii
目錄 iv
圖目錄 vii
表目錄 ix
符號說明 x
一、緒論 1
1-1 研究動機與目的 1
1-2　　研究區域概述 3
1-2-1　地質背景 3
1-2-2　煤層氣來源 7
1-3　　內文概述 8
二、文獻回顧 10
2-1　　CO2-ECBM之發展 10
2-2　　煤層氣體吸附原理 12
2-2-1　氣體流動機制 12
2-2-2　等溫吸附曲線 13
2-2-3　差異吸附 15
2-3　　影響氣體吸附之因素 17
2-3-1　煤級 (Coal Rank) 17
2-3-2　煤素質組成 19
2-3-3　深度 20
2-3-4　煤岩結構 21
2-4　　絕對吸附量與Gibbs吸附量 23
三、等溫吸附模型 24
3-1　　吸附理論 24
3-1-1　Langmuir Equation 24
3-1-2　Brunauer-Emmett-Teller Equation 25
3-1-3　Dubinin–Radushkevitch (D–R) Equation 27
3-1-4　Dubinin–Astakhov (D–A) Equation 28
3-2　　吸附理論比較 28
四、研究方法 30
4-1　　研究流程 30
4-2　　研究樣本 30
4-2煤岩特性與孔隙分析 31
4-2-1　工業分析 31
4-2-2　元素分析 33
4-2-3　比表面積分析 36
4-3　　吸附實驗 38
4-3-1　樣本製備及煤樣物性資料 38
4-3-2　吸附實驗 39
4-3-3　氣體吸附計算 40
五、結果與討論 41
5-1 煤岩性質與氣體吸附能力之關聯性 41
5-1-1　元素組成 41
5-1-2　灰分、水分、揮發分及固定碳 43
5-1-3　比表面積及孔隙組成 45
5-2 氣體吸附結果 47
5-2-1　吸附實驗數據 47
5-2-2　吸附擬合結果 49
5-2-3　相關係數R-square及平均相對誤差MRE 53
5-2-4 澳洲煤樣甲烷吸附特性 54
5-2-5 不同地區之煤樣吸附擬合結果 55
5-2-6 D-A方程之n值的影響 59
5-3 Gibbs吸附量與絕對吸附量之差異 60
六、結論 61
參考文獻 63
附錄 69
A. 本研究澳洲煤樣之真密度 69
B. 四種吸附模式對印度地區煤樣之擬合曲線 70
C. 四種吸附模式對捷克地區煤樣之擬合曲線 84
D. 四種吸附模式對紐西蘭地區煤樣之擬合曲線 86

參考文獻

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指導教授

蔡龍珆(Loung-Yie Tsai)

審核日期

2013-1-23

推文