深共熔溶劑L-精氨酸鹽酸鹽/甘油之二氧化碳溶解度量測

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江瑞恆(Jui-Heng Chiang) 查詢紙本館藏

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化學工程與材料工程學系

論文名稱

深共熔溶劑L-精氨酸鹽酸鹽/甘油之二氧化碳溶解度量測
(Measurement of Carbon Dioxide Solubility in Deep Eutectic Solvent L-Arginine Hydrochloride/Glycerol)

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至系統瀏覽論文 (2029-10-16以後開放)

摘要(中)

二氧化碳是一種對環境有害的溫室氣體，是全球變暖的主要因素。因此從工業源點去除二氧化碳至關重要。胺類溶劑為工業上廣泛應用於從煙氣中去除二氧化碳的吸收劑，然而這些溶劑存在著缺點，胺類溶劑具有腐蝕性、揮發性、生物降解性低以及溶劑再生的高耗能等特性。深共熔溶劑近年被視為二氧化碳捕捉中有前途的替代吸收劑。深共熔溶劑是由兩種或多種純化合物組成，包括氫鍵受體和氫鍵供體，其共熔點溫度低於理想液態混合物的溫度。這類溶劑具有可忽略的蒸氣壓、高熱穩定性、低成本、良好可再生性、低毒性、且具有調節性，可以透過調整陰陽離子的比例改變物化性質。此外，它們製備過程相對簡單。
L-精氨酸是一種無毒、生物可降解且環保的天然產品，部分文獻中報導到精氨酸對二氧化碳捕捉有顯著的效果；而甘油在石油工業中被視為廢物，其產量超過需求量，利用甘油是一種環保的甘油回收方式。本研究選擇L-精氨酸鹽酸鹽/甘油作為目標DES，對比文獻，觀察氫鍵受體的改變對吸收量以及基本物理性質的影響，調查L-精氨酸鹽酸鹽/甘油的物理性質，包括凝固點、密度、黏度等特性。同時，量測了在不同莫耳比、不同溫度、不同含水量L-精氨酸鹽酸和甘油對二氧化碳的吸收情況。根據量測結果，莫耳比1:9 (L-ArgHCl:Gly) 在70°C的環境下能得到最大的吸收量，其溶解度為0.754 mol_(CO_2 )/mol_DES。此外，也進行了DES的再生實驗。透過傅立葉變換紅外光譜、核磁共振(氫譜、碳譜)，研究了DES與二氧化碳的相互作用機制。

摘要(英)

Carbon dioxide (CO2) is a harmful greenhouse gas and a major contributor to global warming. Therefore, removing CO2 from industrial point sources is crucial. Amine solvents are widely used in industry for CO2 removal from flue gas; however, these solvents have significant drawbacks, including corrosiveness, volatility, low biodegradability, and high energy consumption for regeneration. In recent years, deep eutectic solvents (DES) have emerged as promising alternative absorbents for CO2 capture. DESs are composed of two or more purified compounds, including hydrogen-bond acceptors (HBA) and hydrogen-bond donors (HBD), with a eutectic point temperature lower than that of an ideal liquid mixture. These solvents exhibit negligible vapor pressure, high thermal stability, low cost, good regenerability, low toxicity, and tunable properties, which can be adjusted by varying the ratio of the ions. Additionally, they are relatively simple to prepare.
L-arginine is a natural, non-toxic, biodegradable, and environmentally friendly product, with several studies reporting its significant effectiveness in CO2 capture. Glycerol, often considered waste in the petroleum industry due to its surplus, presents an eco-friendly option for recovery. This study selected L-arginine hydrochloride/glycerol as the target deep eutectic solvent (DES) and, by comparing it with the literature, aimed to observe how changes in the hydrogen bond acceptor affect absorption capacity and basic physical properties. The physical properties of L-arginine hydrochloride/glycerol, including freezing point, density, and viscosity, were thoroughly examined. CO2 absorption was measured under varying molar ratios, temperatures, and water contents. The 1:9 DES at 70°C exhibited the highest solubility, reaching 0.754 mol_CO2/mol_DES. Additionally, regeneration experiments were performed on the DES. The interaction mechanism between DES and CO2 was explored using FTIR, 1H NMR, and 13C NMR.

關鍵字(中)

★ 深共熔溶劑
★ 二氧化碳捕捉
★ 二氧化碳溶解度
★ L-精氨酸鹽酸鹽
★ 甘油

關鍵字(英)

★ Deep Eutectic Solvent
★ Carbon Capture
★ Carbon Dioxide Solubility
★ L-Arginine Hydrochloride
★ Glycerol

論文目次

摘要 i
ABSTRACT ii
致謝 iii
目錄 iv
圖目錄 vi
表目錄 viii
第一章、序論 1
1-1 氣候變遷的原因與二氧化碳捕獲與封存的重要性 1
1-2 二氧化碳捕獲技術 3
1-3 工業上二氧化碳分離技術 8
1-3-1. 吸收(Absorption): 8
1-3-2. 薄膜(Membranes): 10
1-3-3. 吸附(Adsorption): 11
1-3-4. 低溫二氧化碳分離法(Cryogenic Method): 12
1-3-5. 化學鏈燃燒法(Chemical Looping Combustion Method): 12
1-3-6. 鈣循環 (Calcium Looping): 13
1-4 深共熔溶劑(Deep Eutectic Solvents, DES) 15
1-4-1 深共熔溶劑種類 16
1-4-2 目前深共熔溶劑實際應用範圍 17
1-4-3 深共熔溶劑合成方式 20
1-4-4 深共熔溶劑之特性 20
1-4-5 常見之二氧化碳捕獲實驗裝置 25
1-5 研究動機 30
第二章、實驗方法 32
2-1 實驗藥品 32
2-2 實驗裝置 35
2-3 實驗步驟 37
2-3-1. 深共熔溶劑的製備: 37
2-3-2. 量測DES之吸收量: 38
2-3-3. 二氧化碳吸收與脫除循環/DES再生: 38
2-3-4. 深共熔溶劑之物理分析、吸收機制 39
2-4實驗分析儀器 40
2-4-1. 庫倫式水分儀 40
2-4-2. 熱重分析儀 40
2-4-3. 差式掃描量熱分析儀 41
2-4-5. 落球式黏度計 41
2-4-6. 傅立葉紅外先光譜儀 42
2-4-7. 核磁共振光譜儀 42
第三章、結果與討論 44
3-1 物理性質分析 44
3-1-1. 相圖 46
3-1-2. 密度 48
3-1-3. 黏度 51
3-2 深共熔溶劑之吸收實驗數據 54
3-2-1. 不同莫耳比、不同溫度對吸收的影響 54
3-2-2. 不同氫鍵受體的影響 57
3-2-3. 不同含水量對吸收的影響 58
3-2-4. 高溫下深共熔溶劑的揮發性 59
3-2-5. 吸收脫除實驗-深共熔溶劑再生 60
3-3 深共熔溶劑吸收機制 61
3-3-1. 深共熔溶劑吸收二氧化碳前後之FTIR分析結果 61
3-3-2. 深共熔溶劑吸收二氧化碳前後之1H NMR分析結果 62
3-3-3. 深共熔溶劑吸收二氧化碳前後之13C NMR分析結果 63
第四章、結論與未來展望 64
4-1 結論 64
4-2 未來展望 65
附錄一 67
附錄二 69
附錄三 70
參考文獻 73
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指導教授

謝介銘(Chieh-Ming Hsieh)

審核日期

2024-10-16

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