臺灣博碩士論文加值系統

本研究主要利用濕壁柱探討CO2與PZ水溶液、混合醇胺TEA + PZ水溶液的反應動力學，濃度範圍為PZ (0.23M; 0.46M; 0.69M; 0.92M) + H2O及 TEA (0.5 kmol‧m-3) + PZ (0.1-0.5 kmol‧m-3) + H2O及TEA (1.0 kmol‧m-3) + PZ (0.1-0.5 kmol‧m-3) + H2O。溫度範圍30、35及40aC, 操作壓力為常壓下。對於CO2，本研究以pseudo-first-order的模式來描述CO2與醇胺之反應動力行為，而對於PZ、TEA則皆使用一級反應的反應動力學模式來探討。相關的物理數據如黏度、密度、亨利常數以及擴散係數也ㄧ併量測。CO2亨利常數以及擴散係數是採用N2O類比法來推算。
由於PZ與CO2的反應速率常數在文獻上的結果差異甚大，因此在本研究中對於PZ水溶液與二氧化碳的反應動力學數據再加以量測，以期求得正確的反應速率常數。而在三級醇胺TEA中加入PZ來吸收CO2的反應動力學數據在文獻上尚未有探討則是我們以TEA + PZ + H2O這個系統來研究的另一主題。
由實驗結果可發現，本研究的實驗範圍符合擬一級反應之條件的假設，而且以一級反應可以用來合理解釋CO2與PZ、TEA的反應。CO2 與 PZ + H2O的反應速率常數經實驗結果和文獻上Bishnol and Rochell (2000)的結果相近，代表本實驗得到結果是正確的。另外由實驗結果我們可以得知，在TEA醇胺水溶液中，加入少量的PZ，確實能使系統的反應吸收速率大大提升。
本研究結果所得到的數據可以用來作為設計酸性氣體吸收設備的計算基礎。

The reaction kinetics of the absorption of CO2 into aqueous solutions of piperazine (PZ) and into mixed aqueous solutions of PZ and triethanolamine (TEA) and were investigated by a wetted wall column at 30 to 40 aC. For CO2 + PZ + H2O, the systems studied are aqueous 0.23, 0.46, 0.69, and 0.92 (kmol‧m-3 PZ) solutions; for CO2 + PZ + TEA + H2O, the systems considered are PZ (0.1, 0.2, 0.3, 0.4, and 0.5 kmol‧m-3) + TEA (0.5 and 1.0 kmol‧m-3) + H2O. The physical properties such as density, viscosity of the solutions and the solubility and diffusivity of nitrous oxide (N2O) in the aqueous alkanolamine solutions were also measured. The N2O analogy was applied to estimate the solubilities and diffusivities of CO2 in aqueous amine systems. Based on the pseudo-first-order for the CO2 absorption, the overall pseudo first-order reaction rate constants were determined from the kinetic measurements. For CO2 absorption into aqueous PZ solutions, the obtained second-order reaction rate constants for the reaction of CO2 with PZ are in a good agreement with the results of Bishnoi and Rochelle (2000). For CO2 absorption into mixed aqueous solutions of PZ and TEA, it was found that the addition of small amounts of PZ to aqueous TEA solutions has significantly effect on the enhancement of the CO2 absorption rate. A second-order reaction rate equation is applied to model the reaction of CO2 with PZ and the reaction of CO2 with TEA. The model is satisfactory to represent the CO2 absorption into mixed aqueous solutions of PZ and TEA. The result of this study can be used as a data base for calculating the gas absorption rate in the <a href="http://www.ntsearch.com/search.php?q=design&v=56">design</a> of the gas absorption apparatus using TEA + CO2 +H2O as absorbents.

目錄
摘要……………………………………………………………………Ⅰ
Abstract………………………………………………………………..Ⅱ
誌謝……………………………………………………………………Ⅲ
目錄……………………………………………………………………Ⅳ
表目錄…………………………………………………………………Ⅶ
圖目錄…………………………………………………………………Ⅹ
第一章 緒論…………………………………………………………..1
1-1 前言…………………………………………………………….1
1-2 醇胺的使用…………………………………………………….2
1-3 TEA與PZ的熱物性質………………………………………..3
1-3.1 TEA………………………………………………………...3
1-3.2 PZ…………………………………………………………..3
1-4 PZ混合醇胺水溶液文獻探討…………………………………4
1-5 研究動機……………………………………………………….7
第二章 原理與理論…………………………………………………13
2-1 反應動力學模式……………………………………………...13
2-1.1 CO2與水的反應……………………………..……………13
2-1.2 CO2與醇胺的反應…………………..……………………13
2-1.3 CO2與PZ的反應………………………………………...15
2-1.4 CO2與TEA + PZ + H2O的反應…………………………15
2-2 N2O類比理論…………………………………………………16
2-3 氣體吸收模式的探討………………………………………...18
2-3.1 物理吸收的模式………………………………………....18
2-3.2 化學吸收模式……………………………………………20
2-3.3 無因次群定義的由來……………………………………28
2-3.4 擬一級反應條件的推導…………………………………32
2-4 混合醇胺水溶液吸收模式探討……………………………...34
2-4.4 Jhaveri (1969)的吸收模式...……………………………...34
2-4.2 Rangwala et al. (1992)的吸收模式……………………….36
2-5 本實驗所採用的吸收模式…………………………………...38
2-5.1 CO2 + PZ + H2O....…………………………………..……38
2-5.2 CO2 + TEA + PZ + H2O…………………………………..39
2-6 相關物理數據回歸模式……………………………………...39
2-6.1 密度的計算回歸模式……………………………………40
2-6.2 黏度的計算回歸模式……………………………………41
2-6.3 亨利常數的回歸計算模式………………………………42
2-6.4 擴散係數的計算回歸模式……………………………....44
第三章 實驗………………………………………………………....46
3-1 實驗藥品……………………………………………………...46
3-2 密度的量測…………………………………………………...46
3-3 黏度的量測…………………………………………………...47
3-4 亨利常數的量測……………………………………………...47
3-5 擴散係數的量測……………………………………………...49
3-6 二氧化碳吸收的量測………………………………………...51
第四章 結果討論……………………………………………………56
4-1 CO2 + PZ + H2O…………………………………………….....56
4-1.1 密度和黏度的量測結果....……………………………....56
4-1.2 亨利常數的量測結果……………………………………56
4-1.3 擴散係數的量測結果……………………………………57
4-1.4 CO2 + PZ + H2O化學吸收的量測結果…….…………....58
4-2 CO2 + TEA + PZ + H2O………………….................................80
4-2.1 密度和黏度的量測結果....……………………………....80
4-2.2 亨利常數的量測結果……………………………………80
4-2.3 擴散係數的量測結果……………………………………81
4-2.4 CO2 + TEA + PZ + H2O化學吸收的量測結果……..…....82
第五章 結論………………………………………………………...115
符號說明…………………………………………………………….116
參考文獻…………………………………………………………….119
自 述…………………………………………………………….127
表目錄

Table 1-1. Commonly used alkanolamines. 9
Table 1-2. Literature review on the reaction of CO2 with aqueous blended amine solutions.. 10
Table 1-3. Literature data on the reaction of CO2 with aqueous TEA solutions. 11
Table 1-4. Literature review on the reaction of CO2 with aqueous PZ solutions. 12
Table 4-1. Densities and viscosities of PZ + H2O solutions. 62
Table 4-2. Parameters of density equation……………….……………...63
Table 4-3. parametersof viscosity equation 64
Table 4-4. Estimated solubility of CO2 in PZ + H2O using N2O analogy
68
Table 4-5. Parameters of the Henry's constant equation. 69
Table 4-6. Estimated diffusivity of CO2 in PZ + H2O using N2O analogy 72
Table 4-7. Parameters of the diffusivity equation 73
Table 4-8. Kinetics data obtained for CO2 in PZ + H2O solutions. 75
Table 4-9. Kinetic data for the absorption of CO2 in PZ + H2O solutions
76
Table 4-10. Diffusivity of amines in solutions used to calculate instantaneous enhancement factor for CO2 in PZ + H2O solutions 77
Table 4-11. Densities and viscosities of TEA (0.5 M) + PZ + H2O solutions.... 85
Table 4-12. Densities and viscosities of TEA (1.0 M) + PZ + H2O
solutions. 86
Table 4-13. Parameters for the densities and viscosities of pure fluids
... 87
Table 4-14. Parameters of the density equation 88
Table 4-15. Parameters of the viscosity equation 89
Table 4-16. Estimated solubility of CO2 in TEA (0.5 M) + PZ + H2O using N2O analogy 94
Table 4-17. Estimated solubility of CO2 in TEA (1.0 M) + PZ + H2O using N2O analogy. 95
Table 4-18. Parameters of the Henry’s constant equation 96
Table 4-19. Estimated diffusivity of CO2 in TEA (0.5 M) + PZ + H2O using the N2O analogy.. 99
Table 4-20. Estimated diffusivity of CO2 in TEA (1.0 M) + PZ + H2O using the N2O analogy.. 100
Table 4-21. Parameters of the diffusivity equation 101
Table 4-22. Kinetics data of CO2 in aqueous TEA (0.5 M) + PZ solutions. 104
Table 4-23. Kinetics data of CO2 in aqueous TEA (1.0 M) + PZ solutions 105
Table 4-24. Kinetics data for the absorption of CO2 in aqueous
TEA (0.5 M) + PZ solutions 106
Table 4-25. Kinetics data for the absorption of CO2 in aqueous
TEA (1.0 M) + PZ solutions 107
Table 4-26. Diffusivity of amines in solutions used to calculate instantaneous enhancement factor for CO2 in aqueous
TEA (0.5 M) + PZ solutions 108
Table 4-27. Diffusivity of amines in solutions used to calculate instantaneous enhancement factor for CO2 in aqueous
TEA (1.0 M) + PZ solutions 109
Table 4-28. Compare results in aqueous TEA (0.5 M) + PZ solution for Eq. 4-10 110
Table 4-29. Compare results in aqueous TEA (1.0 M) + PZ solution for Eq. 4-10 111
圖目錄

Figure 2-1. Enhancement factor for second order reaction plotted against Hatta number. (Drew et al., 1981) 23
Figure 2-2 Concentration profile for very slow reaction………………..24
Figure 2-3 Concentration profile for moderate reaction………………...25
Figure 2-4 Concentration profile for Moderate reaction in liquid film and fast reaction in bulk………………………………………….25
Figure 2-5 Concentration profile for Fast reacton occur in liquid film…26
Figure 2-6. Enhancement factor for second order reaction for Hatta number greater than 3 (Ha > 3). (van Krevelen and Hoftijzer, 1948) 27
Figure 2-7 Concentratuon profile for Instantaneous reaction…………...29
Figure 2-8 Concentration profile for gas reaction with liquid…………..31
Figure 2-9 Concentration profile for gas fast and completed reacted with liquid in liquid film…..…………………………………..….32
Figure 2-10 Concentration profile for one gas and two reactants : both fast pseudo-first-order reaction……………………………...35
Figure 3-1. Gay-Lussac pycnometer 52
Figure 3-2. Cannon-Fenske routine viscometer. 53
Figure 3-3. Schematic drawing of physical gas absorption apparatus. 54
Figure 3-4. Schematic drawing of wetted-wall column apparatus 55
Figure 4-1. Density of aqueous PZ solutions. 65
Figure 4-2. Viscosity of aqueous PZ solutions 66
Figure 4-3. Solubility of N2O in <a href="http://www.ntsearch.com/search.php?q=water&v=56">water</a> as a function of temperature 67
Figure 4-4. Solubility of N2O in aqueous PZ solutions.. 70
Figure 4-5. Diffusivity of N2O in <a href="http://www.ntsearch.com/search.php?q=water&v=56">water</a> as a function of temperature …71
Figure 4-6. Diffusivity of N2O in aqueous PZ solution 74
Figure 4-7. Pseudo-first-order apparent reaction rate constant for the reaction of CO2 with PZ + H2O solutions -…..……………………………………….…………………78
Figure 4-8. Arrhenius plot of k2,PZ as function of temperature……….…79
Figure 4-9. Density of aqueous TEA (0.5 M) + PZ solutions
90
Figure 4-10. Density of aqueous TEA (1.0 M) + PZ solutions
………..………………………………………………………91
Figure 4-11. Viscosity of aqueous TEA (0.5 M) + PZ solutions
………….….…………………………………………….……92
Figure 4-12. Viscosity of aqueous TEA(1.0 M) + PZ solutions
…………..................................................................................93
Figure 4-13. Solubility of N2O in aqueous TEA (0.5 M) + PZ solutions 97
Figure 4-14. Solubility of N2O in aqueous TEA (1.0 M) + PZ solutions 98
Figure 4-15. Diffusivity of N2O in aqueous TEA (0.5 M) + PZ solution 102
Figure 4-16. Diffusivity of N2O in aqueous TEA (1.0 M) + PZ solution 103
Figure 4-17. Pseudo-first-order apparent reaction rate for the reaction of CO2 with TEA (0.5M) + PZ + H2O solution . 112
Figure 4-18. Pseudo-first-order apparent reaction rate for the reaction of CO2 with TEA (1.0 M) + PZ + H2O solution.. 113
Figure 4-19. Arrhenius plot of k2,TEA as function of temperature.. 114

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