臺灣博碩士論文加值系統

由於地球環境氣候巨變，人類開始注意到二氧化碳排放對地球的危害，因此，重要的是發展新技術，以改善這一問題。目前有許多的技術用於分離和捕集二氧化碳，這些技術被使用於化學工業和氣體工業。使用醇胺（也稱為alkanolamines）吸收二氧化碳是現今最常見的技術，但此吸收方法存在著許多問題，如大量的能源消耗，成本增加及腐蝕設備的問題。因此，我們必須找到一種新的二氧化碳吸收劑來取代過去的溶劑，過去十年中，一種新的溶劑，稱為室溫離子液體日益受到重視，經過不同研究發現其良好的吸收性質，已被用於取代傳統的有機溶劑。
因此，我們將針對這兩種吸收劑做進一步的研究，本研究分為兩部分，第一部將討論離子液體及其特性而第二部將針對醇胺吸收二氧化碳進行討論 。第一部分是離子液體吸收二氧化碳溶解度及熱物性質的量測及計算，第二部分著重於將現有文獻中醇胺吸收二氧化碳氣液平衡數據加入回歸模式的計算，因為離子液體吸收二氧化碳文獻上數據非常稀少，所以需要以實驗來得到數據，而醇胺吸收二氧化碳因為文獻上數據非常充足，所以我們只針對計算方面來研究。
在第一部分的熱物性質測量方面，我們對於九種離子液體密度和折射率進行測量和計算回歸，實驗中所使用的離子液體為1-butyl-3-methylimidazolium tetrafluoroborate，1-butyl-3-methylimidazolium hexafluorophosphate，1-butyl-3-methylimidazolium methylsulfate，1-butyl-3-methylimidazolium trifluoromethanesulfonate，1-ethyl-3-methylimidazolium dicyanamide，1-ethyl-3-methylimidazolium tetrafluoroborate，1-ethyl-3-methylimidazolium ethylsulfate，1-ethyl-3-methylimidazolium trifluoromethanesulfonate，和 1-ethyl-3-methylimidazolium 2-(2-methoxyethoxy) ethylsulfate。密度和折射率量測壓力為常壓，最高量測溫度為353.2 K，也將實驗數據和溫度做回歸得到滿意的結果，這兩種熱物性質也使用多種不同的計算模式來做回歸，如Lorentz-Lorenz，Dale-Gladstone，Eykman，Oster，Arago-Biot，Newton，和 modified Eykman方程式等。
溶解度研究的第一部分包括吸收二氧化碳在九種離子液體中的溶解度溫度範圍從303.2到343.2 K和壓力達6.8 MPa，氣體溶解度定義為離子液體吸收達飽和（平衡）時的溶解度，也必須考慮到浮力效應對溶解度測量的影響，準確的狀態方程和密度的相關性為二氧化碳和離子液體，分別用來確定影響的浮力的氣體溶解度。在計算方面二氧化碳在離子液體中溶解度，我們將它表示成溫度及壓力的函數，本溶解度數據也使用亨利定律方程來做進一步回歸並得到滿意的結果。
第二部分中的氣體溶解研究，用簡化之CleggPitzer方程來計算探討二氧化碳在醇胺水溶液系統的溶解度，該研究系統是CO2TEAPZ H2O和CO2AMPPZH2O系統。TEA全名為triethanolamine，PZ為piperazine，AMP為2-amino-2-methyl-1-propanol，我們也針對化學平衡及工作方程式加以討論，並利用回歸文獻值的數據來證明此回歸模式的可行性，由於時間的關係我們只呈現出一些三成份CO2–MDEA–H2O系統初步的計算結果。

There is a growing concern that anthropogenic carbon dioxide emissions are contributing to global climate change. Thus, it is critical to develop technologies to mitigate this problem. A wide range of technologies currently exists for separation and capture of carbon dioxide. Such techniques have been used in the chemical industry and in the production of technical gases for industrial and laboratory use. Absorption with amine-based absorbents (also known as alkanolamines) is the most common technology for carbon dioxide removal as of today. It is a process with considerable inherent problems such as intensive energy consumption, cost increases, and corrosion problems. In this regard, it is also necessary to find a new kind of sequestering agent for carbon dioxide absorption. In the last decade, a new kind of solvents, referred to as room-temperature ionic liquids has received increasing attention among different investigators by virtue of their ability to replace successfully the traditional organic solvents for carbon dioxide absorption.
To this end, these two classes of absorbents for carbon dioxide absorption were investigated in this work. This study was divided into two general parts. First part dealt with ionic liquids and the second part studied the alkanolamines. The first part is an experimental and computational work on physical property measurements and solubility studies of carbon dioxide in certain groups of room-temperature ionic liquids. On the other hand, the second part is a pure computational study about carbon dioxide solubility in aqueous alkanolamine solutions where available data in literature were used to fit in the developed model for vapor-liquid equilibrium of the investigated systems. Experimental measurements were applied to ionic liquids since data for this absorbent are very scarce and a pure computational approach was considered in the alkanolamines since there are a lot of available data for this class of absorbent.
In the physical property measurements of the first part, properties like density and refractive index of nine room-temperature ionic liquids were measured and the relationship between these properties were examined. The studied room-temperature ionic liquids were 1-butyl-3-methylimidazolium tetrafluoroborate, 1-butyl-3-methylimidazolium hexafluorophosphate, 1-butyl-3-methylimidazolium methylsulfate, 1-butyl-3-methylimidazolium trifluoromethanesulfonate, 1-ethyl-3-methylimidazolium dicyanamide, 1-ethyl-3-methylimidazolium tetrafluoroborate, 1-ethyl-3-methylimidazolium ethylsulfate, 1-ethyl-3-methylimidazolium trifluoromethanesulfonate, and 1-ethyl-3-methylimidazolium 2-(2-methoxyethoxy) ethylsulfate. The density and refractive index of the investigated room-temperature ionic liquids were measured at atmospheric pressure and temperature up to 353.2 K. The present measurements on density and refractive index were presented and successfully correlated as a function of temperature. The relationships between these two properties were likewise satisfactory modeled using various known equations namely: LorentzLorenz, DaleGladstone, Eykman, Oster, AragoBiot, Newton, and modified Eykman.
The solubility studies in the first part include the absorption of carbon dioxide in the nine room-temperature ionic liquids for temperatures ranging from 303.2 to 343.2 K and pressures up to 6.8 MPa. The gas solubilities were determined from absorption saturation (equilibrium) data at each temperature and pressure. The buoyancy effect was accounted for in the evaluation of the gas solubilities. An accurate equation of state and density correlation for carbon dioxide and ionic liquids, respectively, were employed to determine the effect of buoyancy on the gas solubilities. The gas solubilities in the studied room-temperature ionic liquids were presented as a function of temperature and pressure. The present solubility data were satisfactory correlated using an extended Henry’s law equation.
In the second part of this work, the simplified Clegg–Pitzer equations were used to represent the vapor-liquid equilibrium of quarternary aqueous alkanolamine systems. The studied quarternaries were CO2–TEA–PZ–H2O and CO2–AMP–PZ–H2O. TEA corresponds to triethanolamine, PZ to piperazine, and AMP to 2-amino-2-methyl-1-propanol. The chemical equilibria for the two systems were discussed and the working equations were carefully derived. Available data (experimental and determined parameters) from literatures were used to validate the developed model. Unfortunately, due to lack of time, only the preliminary results were shown here, i.e., the results of calculation validity using the ternary system CO2–MDEA–H2O, and the results are very promising.

Table of Contents
摘要 i
Abstract iii
Acknowledgement v
Table of Contents vi
List of Tables ix
List of Figures xi
Nomenclature xiv
Chapter 1: INTRODUCTION 1
1.1 Background 1
1.2 Objectives 1
1.3 Significance 2
1.4 Scope and Limitation 3
Chapter 2: REVIEW OF RELATED LITERATURE 5
2.1 Global Warming 5
2.2 Greenhouse Gases 6
2.3 CO2 Emission, Taiwan and the World 6
2.4 Feasible Process for CO2 Reduction: CO2 Capture Technologies 8
2.5 Post-Combustion CO2 Capture 9
2.6 CO2 Absorption 10
2.6.1 CO2 absorbents 11
2.6.2 CO2 solubility studies 12
2.6.2.1 CO2 solubility experimental measurements 12
2.6.2.2 CO2 solubility models 13
2.7 Physicochemical Properties: Density and Refractive Index 15
Chapter 3: EXPERIMENTAL SECTION 17
3.1 Chemicals 17
3.2 Density and Refractive Index Measurements 17
3.3 Carbon Dioxide Solubility Measurements 18
3.3.1 Buoyancy effect calculations 20
3.3.1.1 Buoyancy effect on empty pan 20
3.3.1.2 Buoyancy effect on ionic liquid 21
3.3.2 Density data correlations 21
Chapter 4: RESULTS AND DISCUSSION 34
4.1 Density Measurements Data 34
4.2 Refractive Index Data and Correlation 36
4.3 Density and Refractive Index Correlations 38
4.4 CO2 Solubility in RTILs: Measurements Data 39
4.4.1 Buoyancy correction effect 40
4.4.2 Validation of experimental method 40
4.5 CO2 Absorption in RTIL: Modeling using Extended Henry’s Law Equation 42
4.6 CO2 Absorption in Aqueous Alkanolamine Solution: Modeling using Simplified CleggPitzer Equations 107
4.6.1 Thermodynamic Framework 107
4.6.1.1 Chemical Equilibria 107
4.6.1.2 Standard States 109
4.6.1.3 Thermodynamic Expression 110
4.6.1.4 Interaction Parameters 118
4.6.1.5 Analysis of Compositions 118
4.6.1.6 Model Application 121
Chapter 5: CONCLUSIONS AND RECOMMENDATIONS 130
REFERENCES 133
APPENDIX A: Conceptual Framework of Solubility Measurements 144
APPENDIX B: Sample Data from ThermoCahn 145
APPENDIX C: List of Publications * 146
APPENDIX D: Curriculum Vitae 155
.

List of Tables
Table
No. Title Page No.
2.1 Worldwide ranking on CO2 discharged 16
2.2 Worldwide ranking on average personal CO2 discharged 16
3.1 Ionic liquids investigated in this work 25
3.2 Cation and anion volumes of the investigated ionic liquids 26
3.3 Calculation of densities for the investigated [Bmim]-based RTILs using Eq. (3.6) 27
3.4 Calculation of densities for the investigated [Emim]-based RTILs using Eq. (3.6) 28
3.5 Determined parameters of Eq. (3.5) for the studied ionic liquids 29
3.6 Calculation of densities for the investigated ionic liquids using Eq. (3.5) 30
4.1 Density  and refractive index n of the investigated [Bmim]-based ionic liquids at various temperatures 46
4.2 Density  and refractive index n of the investigated [Emim]-based ionic liquids at various temperatures 47
4.3 Calculation of refractive indices for the studied ionic liquids using Eq. (4.1) 48
4.4 Determined parameters of Eq. (4.1) for the studied ionic liquids 48
4.5 Parameters k and i of different empirical equations from Eq. (4.2) 49
4.6 Solubility of carbon dioxide a (on molality scale) in [Bmim][BF4] 50
4.7 Solubility of carbon dioxide a (on molality scale) in [Bmim][PF6] 50
4.8 Solubility of carbon dioxide a (on molality scale) in [Bmim][MeSO4] 51
4.9 Solubility of carbon dioxide a (on molality scale) in [Bmim][CF3SO3] 51
4.10 Solubility of carbon dioxide a (on molality scale) in [Emim][C2N3] 52
4.11 Solubility of carbon dioxide a (on molality scale) in [Emim][BF4] 52
4.12 Solubility of carbon dioxide a (on molality scale) in [Emim][EtSO4] 53
4.13 Solubility of carbon dioxide a (on molality scale) in [Emim][CF3SO3] 53
4.14 Solubility of carbon dioxide a (on molality scale) in [Emim][MDEGSO4] 54
4.15 Henry’s constant of CO2 in the studied [Bmim]-based RTILs at zero pressure 55
4.16 Henry’s constant of CO2 in the studied [Emim]-based RTILs at zero pressure 56
4.17 Determined parameters li of Eq. (4.9) for the studied RTILs 57
4.18 Determined parameters of and for the Henry’s law equation 57
4.19 Temperature dependence of the equilibrium constants for the studied reactions and Henry’s constant for CO2 124
4.20 Temperature dependence of the density for pure solvents 124
4.21 Temperature dependence of the dielectric constant for pure solvents 125
4.22 Fitted values of solventsolvent interaction parameters Ann’ 125
4.23 Fitted values of ionion interaction parameters BMX 126
4.24 Fitted values of ionsolvent interaction parameters Wsolvent, MX 126
4.25 CO2 solubility into 23.63 wt % MDEA aqueous solutions 126
4.26 Interaction parameters for MDEA–H2O–CO2 system 127


List of Figures
Figure
No. Title Page No.
3.1 Cations and anions structure of the investigated room-temperature ionic liquids 31
3.2 Experimental set-up for CO2 solubility measurements using a thermogravimetric microbalance 32
3.3 Calibration curves of the empty sample pan from this work. 33
4.1 Comparison of density data for [Bmim][BF4] 58
4.2 Comparison of density data for [Bmim][PF6] 59
4.3 Comparison of density data for [Bmim][MeSO4] 60
4.4 Comparison of density data for [Bmim][CF3SO3] 61
4.5 Comparison of density data for [Emim][BF4] 62
4.6 Comparison of density data for [Emim][EtSO4] 63
4.7 Comparison of density data for [Emim][CF3SO3] 64
4.8 Comparison of refractive index data for [Bmim][BF4] 65
4.9 Comparison of refractive index data for [Bmim][PF6] 66
4.10 Comparison of refractive index data for [Bmim][MeSO4] 67
4.11 Comparison of refractive index data for [Emim][EtSO4] 68
4.12 Comparison of density calculations for the investigated [Bmim]-based ionic liquids 69
4.13 Comparison of density calculations for the investigated [Emim]-based ionic liquids 70
4.14 Solubility of CO2 in the studied RTILs at 303.2 K 71
4.15 Buoyancy effect (changes in CO2 solubility) as a function of pressure for [Bmim][BF4] at different temperatures 72
4.16 Buoyancy effect (changes in CO2 solubility) as a function of pressure for [Bmim][PF6] at different temperatures 73
4.17 Buoyancy effect (changes in CO2 solubility) as a function of pressure for [Bmim][MeSO4] at different temperatures 74
4.18 Buoyancy effect (changes in CO2 solubility) as a function of pressure for [Bmim][CF3SO3] at different temperatures 75
4.19 Buoyancy effect (changes in CO2 solubility) as a function of pressure for [Emim][C2N3] at different temperatures 76
4.20 Buoyancy effect (changes in CO2 solubility) as a function of pressure for [Emim][BF4] at different temperatures 77
4.21 Buoyancy effect (changes in CO2 solubility) as a function of pressure for [Emim][EtSO4] at different temperatures 78
4.22 Buoyancy effect (changes in CO2 solubility) as a function of pressure for [Emim][CF3SO3] at different temperatures 78
4.23 Buoyancy effect (changes in CO2 solubility) as a function of pressure for [Emim][MDEGSO4] at different temperatures 80
4.24 Comparison of CO2 solubility in [Bmim][BF4] at low and moderate pressure 81
4.25 Comparison of CO2 solubility in [Bmim][BF4] at high pressure 82
4.26 Comparison of CO2 solubility in [Bmim][PF6] 83
4.27 Comparison of CO2 solubility in [Bmim][MeSO4] 84
4.28 Comparison of CO2 solubility in [Bmim][CF3SO3] 85
4.29 Comparison of CO2 solubility in [Emim][EtSO4] 86
4.30 Pressure dependence of for [Bmim][BF4] at different temperatures 87
4.31 Pressure dependence of for [Bmim][PF6] at different temperatures 88
4.32 Pressure dependence of for [Bmim][MeSO4] at different temperatures 89
4.33 Pressure dependence of for [Bmim][CF3SO3] at different temperatures 90
4.34 Pressure dependence of for [Emim][C2N3] at different temperatures 91
4.35 Pressure dependence of for [Emim][BF4] at different temperatures 92
4.36 Pressure dependence of for [Emim][EtSO4] at different temperatures 93
4.37 Pressure dependence of for [Emim][CF3SO3] at different temperatures 94
4.38 Pressure dependence of for [Emim][MDEGSO4] at different temperatures 95
4.39 Determined Henry’s constant of CO2 in the studied [Bmim]-based RTILs (at zero pressure) as a function of temperature 96
4.40 Determined Henry’s constant of CO2 in the studied [Emim]-based RTILs (at zero pressure) as a function of temperature 97
4.41 Equilibrium solubility of CO2 in [Bmim][BF4] at different temperatures 98
4.42 Equilibrium solubility of CO2 in [Bmim][PF6] at different temperatures 99
4.43 Equilibrium solubility of CO2 in [Bmim][MeSO4] at different temperatures 100
4.44 Equilibrium solubility of CO2 in [Bmim][CF3SO3] at different temperatures 101
4.45 Equilibrium solubility of CO2 in [Emim][C2N3] at different temperatures 102
4.46 Equilibrium solubility of CO2 in [Emim][BF4] at different temperatures 103
4.47 Equilibrium solubility of CO2 in [Emim][EtSO4] at different temperatures 104
4.48 Equilibrium solubility of CO2 in [Emim][CF3SO3] at different temperatures 105
4.49 Equilibrium solubility of CO2 in [Emim][MDEGSO4] at different temperatures 106
4.50 CO2 Solubility in 23.63 wt % MDEA aqueous solutions at 297.7 K 128
4.51 Liquid-phase concentration of a CO2-loaded 23.63 wt % MDEA aqueous solution at 297.7 K. 129

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