製備矽膠固著聚苯胺吸附劑及吸脫附試驗與氣化合成氣經富氧燃燒後之變壓吸附程序二氧化碳純化實驗

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、以作者查詢臺灣博碩士

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姓名

吳碧卿(Bi-Ching Wu) 查詢紙本館藏

畢業系所

化學工程與材料工程學系

論文名稱

製備矽膠固著聚苯胺吸附劑及吸脫附試驗與氣化合成氣經富氧燃燒後之變壓吸附程序二氧化碳純化實驗
(Experimental study of CO2 Adsorption / Desorption with Solid Polyaniline Sorbent and Concentrating High Purity CO2 from Syngas after Oxy-fuel Combustion by Pressure Swing Adsorption Process)

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摘要(中)

隨著科技發展溫室效應造成全球暖化日益嚴重，而其中減少溫室氣體排放已成為重要議題。
本研究分為兩部分，第一部分為台電綜合研究所之製備矽膠固著聚苯胺吸附劑及吸脫附試驗。探討矽膠固著聚苯胺之二氧化碳吸附劑合成的不同條件，並以造粒方法探討製備矽膠固著聚苯胺吸附劑的最佳條件。利用探討造粒前後合成溫度，合成時間，反應物濃度，矽膠固著聚苯胺之固態吸附劑能力等因素的影響，並藉由微量天秤Thermo Cahn D-200測量吸附量和吸附等溫線，並以一大氣壓下，以發電廠氣體比例15％二氧化碳及85％氮氣計算選擇率。再以台電綜合研究所之熱重分析儀測量觀察本研究矽膠固著聚苯胺吸附劑吸附力衰變測試，並對吸附劑性能的影響進行探討。
本研究第二部分為氣化合成氣經富氧燃燒後之變壓吸附程序二氧化碳純化實驗。選用UOP 13X 沸石作為吸附劑，進料氣體為95%二氧化碳與5%氮氣。將吸附劑填入吸附塔進行突破曲線與脫附曲線實驗，藉由改變不同流量、溫度等探討突破曲線與脫附曲線的影響，進而以單塔四步驟變壓吸附程序純化二氧化碳，並探討如溫度、進料壓力、抽真空壓力、步驟時間等變因對其回收率、濃度的影響，研究最適化的操作條件，以獲得高純度二氧化碳。

摘要(英)

With technology development, the greenhouse effect is becoming more and more serious. Reducing greenhouse gas emissions has become an important issue.
The first part of the study is the experimental study of CO2 adsorption / desorption with Solid Polyaniline Sorbent of Taiwan Power Company (Taipower). Changing the different conditions for the synthesis of solid polyaniline carbon dioxide sorbent and the preparation of pelletization procedures obtains the optimal condition for producing solid polyaniline sorbent. The effects of different factors such as synthesis temperature, synthesis time, compound concentration and the adsorption capacity of solid polyaniline carbon dioxide sorbent before and after pelletization were discussed. Adsorption amount and adsorption isotherm were obtained by used Micro-Balance Thermo Cahn D-200 and selectivity of carbon dioxide with respect to nitrogen is calculated based on 15% CO2 / 85% N2 feed at 1 atm. The degree of adsorption amount decay of sorbent is obtained by using TGA of Taipower Research Institute.
The second part of the study is the experimental study of concentrating high purity CO2 from syngas after oxy-fuel combustion by pressure swing adsorption process. UOP 13X zeolite was used as the adsorbent, and the feed gas was 95% CO2 / 5% N2.
Breakthrough curves and desorption curves were discussed by changing the pressure and temperature. Next the carbon dioxide was purified by single-bed four steps pressure swing adsorption procedure. Variables such as temperature, feed pressure, vacuum pressure and step time were discussed to find their effects on CO2 recovery and purity in order to study the optimal operating conditions for obtaining high purity carbon dioxide.

關鍵字(中)

★ 變壓吸附程序
★ 突破曲線
★ 脫附曲線
★ 二氧化碳
★ 選擇率
★ 等溫吸附平衡曲線

關鍵字(英)

★ pressure swing adsorption process
★ adsorption curve
★ desorption curve
★ CO2
★ selectivity
★ isotherm

論文目次

摘要 i
abstract ii
誌謝 iv
目錄 v
圖目錄 ix
表目錄 xix
第一章、緒論 1
第二章、簡介與文獻回顧 6
2-1 吸附之簡介 6
2-1-1 吸附基本原理 6
2-1-2 吸附劑及其選擇率參數 9
2-1-3 PSA 程序之發展與改進 11
2-1-4 突破曲線 16
2-1-5 高純度變壓吸附文獻回顧 18
2-2 矽膠固著聚苯胺吸附劑之製備相關文獻回顧 20
2-2-1 胺基化處理 21
2-2-2 苯胺聚合物反應 26
2-2-3 吸附劑造粒 32
2-2-4 等溫平衡吸附曲線 35
2-3 吸附劑比較 37
第三章、矽膠固著聚苯胺吸附劑實驗設備及方法 38
3-1 矽膠固著聚苯胺吸附劑之製備 38
3-1-1 實驗藥品 39
3-1-2 矽膠固著聚苯胺吸附劑製備流程 40
3-1-3 矽膠固著聚苯胺吸附劑造粒流程 46
3-1-4 矽膠固著聚苯胺吸附劑代號說明 48
3-2 等溫平衡吸附曲線實驗 50
3-2-1 實驗裝置 50
3-2-2 實驗裝置之操作流程 54
3-2-3 天平校正 55
3-2-4 空白實驗 55
3-3 矽膠固著聚苯胺吸附劑吸附力衰變測試實驗 56
第四章、製備矽膠固著聚苯胺吸附劑及吸脫附試驗結果與討論 57
4-1 浮力校正結果 57
4-2 矽膠固著聚苯胺吸附劑吸附量及性質探討 65
4-2-1 溫度對吸附劑造粒前後吸附量影響 66
4-2-2 矽膠固著聚苯胺吸附劑之粉體(100~200 mesh)吸附量 68
4-2-3 矽膠固著聚苯胺吸附劑之顆粒吸附量及其選擇率 75
4-2-4 矽膠固著聚苯胺吸附劑之針筒造粒及非針筒造粒比較 90
4-3 吸附力衰變測試 92
第五章、氣化合成氣經富氧燃燒後之變壓吸附程序實驗設備及方法 96
5-1 變壓吸附程序吸附劑選擇 96
5-2 突破曲線實驗與脫附曲線實驗 98
5-2-1 實驗裝置、各部規格及特性 98
5-2-2 實驗步驟 102
5-3 變壓吸附實驗 103
5-3-1 變壓吸附實驗裝置、各部規格及特性 106
5-3-2 實驗步驟 109
第六章、氣化合成氣經富氧燃燒後之變壓吸附程序實驗結果與討論 112
6-1 吸附劑選擇計算與討論 112
6-2 突破曲線實驗與脫附曲線實驗結果與討論 118
6-2-1 流速對突破曲線的影響 120
6-2-2 進料組成對突破曲線的影響 122
6-2-3 塔內溫度對突破曲線的影響 124
6-2-4 流速對脫附曲線的影響 126
6-2-5 進料組成對脫附曲線的影響 128
6-2-6 塔內溫度對脫附曲線的影響 130
6-3 變壓吸附實驗結果與討論 132
6-3-1 同向減壓時間對單塔四步驟變壓吸附程序之影響 134
6-3-2 進料壓力對單塔四步驟變壓吸附程序之影響 137
6-3-3 高壓吸附時間對單塔四步驟變壓吸附程序之影響 141
6-3-4 逆向減壓壓力對單塔四步驟變壓吸附程序之影響 145
6-3-5 逆向減壓時間對單塔四步驟變壓吸附程序之影響 149
6-3-6 塔內溫度對單塔四步驟變壓吸附程序之影響 154
第七章、結論 158
7-1 製備矽膠固著聚苯胺吸附劑及吸脫附試驗 158
7-2氣化合成氣經富氧燃燒後之變壓吸附程序二氧化碳純化實驗 159
參考文獻 161
附錄A等溫平衡校正曲線詳細數據 166
附錄B 粉體等溫平衡吸附曲線詳細數據 177
附錄C顆粒等溫平衡吸附曲線詳細數據 197
附錄D 變壓吸附程序詳細數據 220

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指導教授

周正堂(Cheng-tung Chou)

審核日期

2017-8-22

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