利用變壓吸附法分離CO2甲烷化產氣之模擬暨實驗設計研究

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陳韻庭(Yun-Ting Chen) 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

利用變壓吸附法分離CO2甲烷化產氣之模擬暨實驗設計研究

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摘要(中)

鑒於全球暖化日益嚴重，及再生能源發電中棄風棄光現象造成能源大量浪費的問題，因此電轉氣(Power to Gas, P2G)為目前歐盟所積極推動的儲能技術。此技術以電解水來產生氫氣，藉利用水電解產生的氫氣和二氧化碳進行甲烷化反應，為了使氫氣不被浪費，甲烷化反應中常會以二氧化碳過量的方式來進行，經反應後，產物組成為二氧化碳、甲烷及乙烷。
本研究模擬探討以變壓吸附法(pressure swing adsorption, PSA)進行CO2甲烷化反應後之氣體高純度純化分離，依據文獻資料擇定以沸石13X做為吸附劑。隨後，本研究以程序模擬結合實驗設計(design of experiment, DOE)，找出以進料條件為67.9%甲烷、30%二氧化碳及2.1%乙烷時之三塔九步驟PSA程序之分離最適化操作條件，經分析後，最佳化程序可使塔頂輕產物甲烷純度95.91%、回收率97.93%，塔底重產物二氧化碳純度90.27%、回收率90.47%。

摘要(英)

In view of serious global warming problem and the massive energy waste in renewable energy, power-to-gas (P2G) is currently an energy storage technology actively promoted by the European Union. The P2G technology uses green energy or off-peak residual electricity with a low-energy amphoteric membrane to electrolyze water to produce hydrogen and oxygen. In addition, the captured and desorbed high-purity carbon dioxide is hydrogenated with hydrogen into high-purity methane through a catalyst. Moreover, the methanation reaction often reacts with excess carbon dioxide. After the reaction, the gas composition is carbon dioxide, methane, ethane and a small amount of hydrogen.
In this research, the pressure swing adsorption (PSA) process was applied to purify carbon dioxide and methane from the product gases from CO2 methanation. By simulation study, the adsorbent is chosen based on literature, and the sorbent parameters were calculated from experimental data of the adsorption equilibrium curve. We used 13X zeolite as adsorbent due to its high CO2/CH4 selectivity. The PSA process simulation combined with the design of experiments (DOE) is used to find out the optimal operating conditions for the separation of the three-component feed which contained 67.9% CH4, 2.1% C2H6 and 30% CO2. After analysis, the optimal operating conditions of a three-bed nine-step PSA process were obtained to produce a top product at 95.91% methane purity with 97.93 % recovery, and a bottom product at 90.27% carbon dioxide purity with 90.47 % recovery.

關鍵字(中)

★ 變壓吸附
★ 二氧化碳
★ 甲烷

關鍵字(英)

★ Pressure swing adsorption
★ Carbon dioxide
★ Methane

論文目次

摘要 i
Abstract ii
誌謝 iii
圖目錄 vii
表目錄 ix
第一章、緒論 1
第二章、簡介及文獻回顧 3
2-1 吸附之簡介 3
2-1-1 吸附之基本原理 3
2-1-2 吸附劑之選擇性 4
2-1-3 吸附程序 6
2-1-4 突破曲線 7
2-2 研究目的及文獻回顧 9
2-2-1 PSA程序之發展與改進 9
2-2-2 理論之回顧 12
2-2-3 用於甲烷化反應後氣體分離之吸附劑之回顧 14
第三章、假設及理論 17
3-1 基本假設 17
3-2 統制方程式 18
3-3 吸附平衡關係式 21
3-3-1 等溫吸附平衡關係式 21
3-3-2 質傳驅動力模式(Driving force model) 21
3-3-3 吸附熱關係式 21
3-4 參數推導 22
3-4-1 軸向分散係數(Axial dispersion coefficient) 22
3-4-2 熱傳係數 24
3-4-3 線性驅動力質傳係數(Mass transfer coefficient of linear driving force) 26
3-5 邊界條件與流速 29
3-5-1 邊界條件與節點流速 29
3-5-2 閥公式 29
3-6 求解步驟 30
3-8 產率計算 32
第四章、模擬程序所需參數與驗證 33
4-1 雙塔六步驟製程描述 33
4-2 模擬驗證所需參數 34
4-3 模擬驗證結果 36
第五章、雙塔八步驟之甲烷化氣體分離程序 37
5-1 吸附劑吸附能力比較 37
5-1-1 吸附劑吸附數據蒐集 37
5-1-2 吸附劑之選擇率計算結果與比較 40
5-2 雙塔八步驟PSA製程描述 42
5-3 模擬所需參數 44
5-3-1 氣體與吸附劑性質 44
5-3-2 等溫平衡吸附取線 45
5-4 雙塔八步驟PSA模擬結果與分析 47
第六章、三塔九步驟之甲烷化氣體分離程序 49
6-1 製程描述 49
6-2 模擬結果與分析 51
第七章、以實驗設計求最佳化結果 56
7-1 因子選定 56
7-2 變異數分析(Analysis of Variance, ANOVA) 59
7-2-1 殘差分析圖(Analysis of residual plots) 68
7-2-2 回歸分析(Regression analysis) 71
7-3 各響應組合之最佳化結果 73
7-3-1 以甲烷及二氧化碳高純度為目標 73
7-3-2 以提升二氧化碳回收率為目標 79
7-4 以模擬程序驗證實驗設計之最佳化結果 82
第八章、結論 85
符號說明 86
參考文獻 90
附錄A、流速之估算方法 97
附錄B、ANOVA全因子設計之各響應值 100

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指導教授

周正堂(Cheng-Tung Chou)

審核日期

2022-9-8

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