利用四塔十六步驟變壓吸附法分離 CO2 甲烷化產氣之模擬暨實驗設計研究

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姓名

陳書昀(Shu-Yun 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

利用四塔十六步驟變壓吸附法分離 CO2 甲烷化產氣之模擬暨實驗設計研究
(Separation of Gases from Methanation by Four-bed Sixteen-step Pressure Swing Adsorption Process with Design of Experiments)

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摘要(中)

隨著國際社會推動2050年淨零排放目標，再生能源的比例將會大幅增加，為了解決再生能源的間歇性問題並提高電力調度的彈性，電轉氣（Power to Gas, P2G)技術已成為國際間積極推動的儲能技術。此技術能將多餘的再生能源經由電解水來產生氫氣，這些氫氣能被儲存也能藉由甲烷化將氫氣和二氧化碳進行反應，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。因此本研究目的為設計出一四塔十六步驟程序分離出高純度、高回收率甲烷以供後續能源使用並同時回收二氧化碳達到溫室
氣體減量目標。
本研究使用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，依據文獻資料根據選擇率擇定沸石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%乙烷時之四塔十六步驟PSA
程序之分離最適化操作條件。
比較之前實驗室模擬三塔九步驟最佳化程序及本次四塔十六步驟PSA最佳化程序分離結果發現，甲烷的純度從95.91%上升至97.51%，甲烷回收率從97.93%上升至98.96%，二氧化碳的純度大約持平為90%，回收率則從90.47%大幅提升
至 94.41%，捕獲二氧化碳所花費的能耗則也從0.45 GJ/t-CO2下降至0.35 GJ/t-
CO2。

摘要(英)

With the global pursuit of net-zero emissions by 2050, the proportion of renewable energy is expected to significantly increase. To address the intermittency issues of renewable energy and enhance grid flexibility, Power to Gas (P2G) technology has emerged as a promising energy storage solution. This technology enables the conversion of surplus renewable energy into hydrogen through electrolysis, which can be stored and further utilized through methanation, a process that involves the reaction of hydrogen with carbon dioxide. To minimize hydrogen wastage, methanation reactions often employ excess carbon dioxide. The resulting products of the reaction are carbon dioxide, methane, and ethane. Therefore, the aim of this study is to design a four-bed sixteen-step pressure swing adsorption (PSA) process for the purification and separation of high-purity methane for subsequent energy utilization, while simultaneously recovering carbon dioxide to achieve greenhouse gas reduction targets.
In this study, a simulation program was used to perform high-purity gas purification and separation of CO2 methanation products using PSA. Based on literature data and selectivity considerations, zeolite 13X was chosen as the adsorbent. Subsequently, the study combined process simulation with design of experiment (DOE) to identify the optimal operating conditions for a four-bed sixteen-step PSA process with feed composition of 67.9% methane, 30% carbon dioxide, and 2.1% ethane.
Comparing the results of the previous laboratory simulation of the three-bed nine-step PSA optimized process with the four-bed sixteen-step PSA optimized process, it was found that the methane purity increased from 95.91% to 97.51%, and the methane recovery increased from 97.93% to 98.96%. The purity of carbon dioxide remained approximately the same at around 90%, while the recovery significantly improved from 90.47% to 94.41%. The energy consumption required for capturing carbon dioxide also decreased from 0.45 GJ/t-CO2 to 0.35 GJ/t-CO2.

關鍵字(中)

★ 變壓吸附法
★ 電轉氣
★ 二氧化碳捕獲

關鍵字(英)

★ pressure swing adsorption
★ power to gas
★ carbon dioxide capture

論文目次

摘要 i
ABSTRACT ii
誌謝 iv
目錄 v
圖目錄 viii
表目錄 xi
符號說明 xiii
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 8
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回顧 13
2-2-3-1 分離甲烷與二氧化碳之比較 13
2-2-3-2 分離乙烷之比較 14
第三章、假設及理論 16
3-1基本假設 16
3-2統制方程式 16
3-3 吸附平衡關係式 19
3-3-1 等溫吸附平衡關係式 19
3-3-2 質傳驅動力模式(Driving force model) 20
3-3-3 吸附熱關係式 20
3-4 參數推導 21
3-4-1 軸向分散係數(Axial dispersion coefficient) 21
3-4-2 熱傳係數 22
3-4-3 線性驅動力質傳係數(Mass transfer coefficient of linear 24
3-5邊界條件與流速 26
3-5-1 邊界條件與節點流速 26
3-5-2 閥公式 27
3-6 求解步驟 28
3-7 能耗計算公式 31
第四章、模擬程序所需參數與驗證 32
4-1製程描述 32
4-2模擬驗證所需參數 35
4-3模擬驗證結果 36
第五章、多塔之模擬程序所需參數與驗證 38
5-1 吸附劑吸附能力比較 38
5-1-1 吸附劑吸附數據蒐集 38
5-1-2 吸附劑之選擇率計算結果與比較 41
5-1-3 Zeolite 13X等溫平衡吸附曲線 43
5-1-4 氣體與吸附劑性質 45
5-1-5 吸附塔參數 46
5-2 三塔九步驟PSA製程 46
5-3 三塔九步驟PSA最佳化結果與分析 49
第六章、四塔十六步驟PSA程序描述 55
6-1 不同四塔十六步驟PSA程序 55
6-2 不同四塔十六步驟PSA程序之模擬結果與分析 58
第七章、以實驗設計求最佳化結果 63
7-1 因子選定 63
7-2 變異數分析(Analysis of Variance, ANOVA) 64
7-2-1 殘差分析圖(Analysis of residual plots) 76
7-2-2 回歸分析(Regression analysis) 79
7-3 各響應組合之最佳化結果 80
7-3-1 各響應之邊界值 80
7-3-1-1 塔頂輕產物甲烷純度極大值 80
7-3-1-2 塔頂輕產物甲烷回收率極大值 82
7-3-1-3 塔底重產物二氧化碳純度極大值 84
7-3-1-4 塔底重產物二氧化碳回收率極大值 85
7-3-1-5 捕獲每噸二氧化碳所需能耗極小值 86
7-3-2 各響應組合最佳化結果及參數 88
7-4 以模擬程序驗證最佳化響應與結果 96
7-4-1 以模擬程序驗證實驗設計之最佳化結果 96
7-4-2 三塔九步驟最佳化結果與四塔十六步驟最佳化結果比較 100
第八章、結論 102
參考文獻 103
附錄A、流速之估算方法 110
附錄B、ANOVA全因子設計之各響應值 113
附錄C、三塔九步驟設計準則 117

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指導教授

周正堂(Cheng-Tung Chou)

審核日期

2023-7-24

推文