利用真空變壓吸附法純化生質沼氣之模擬暨實驗設計研究

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林柏瑋(Po-Wei Lin) 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

利用真空變壓吸附法純化生質沼氣之模擬暨實驗設計研究
(Simulation of Biogas Upgrading by Pressure Swing Adsorption Process with Study of Design of Experiments)

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★ 改善三塔真空變壓吸附程序捕獲煙道氣中二氧化碳之實驗設計分析

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摘要(中)

生質沼氣平均成分為60~70%甲烷、30~40%二氧化碳、0~4000 ppm硫化氫及其他微量氣體等，然而甲烷與二氧化碳為溫室效應之主要氣體，其中，甲烷的全球暖化潛勢為二氧化碳之25倍，對於溫室效應的影響力不容小覷，而硫化氫易造成機器損壞及管線腐蝕。因此本研究目的為設計出可分離硫化氫、純化生質沼氣中甲烷至高純度供後續再生能源使用且同時回收二氧化碳將溫室氣體減量之生質沼氣分離程序，此程序可謂一舉數得。
本研究使用模擬程序以變壓吸附法(pressure swing adsorption, PSA)進行生質沼氣純化分離，依據文獻資料擇定以沸石13X做為吸附劑，比較三個廠牌生產之沸石13X於溫度298K下由等溫平衡吸附數據計算之平衡選擇性(equilibrium selectivity)後，選出最適合的吸附劑為COSMO沸石13X，隨後，本研究以模擬程序結合實驗設計(design of experiment, DOE)，找出以進料條件為台灣6,000頭豬隻每日產生之排泄物經厭氧發酵後所產生的氣體量與進料組成64.8%甲烷、34.8%二氧化碳及4,000 ppm硫化氫時之雙塔八步驟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甲烷輕產物純度達99.34%、回收率91.93%，塔底重產物二氧化碳純度為可達96.37%、回收率49.16%，純化每噸甲烷產物所需能耗為1.02 GJ，捕獲每噸二氧化碳所需能耗為1.35 GJ，甲烷每日產能可達841.7 kg。

摘要(英)

The average composition of biogas is 60~70% methane, 30~40% carbon dioxide, 0~4,000 ppm hydrogen sulfide, and other trace gases. However, methane and carbon dioxide are both greenhouse gases. Furthermore, the global warming potential of methane is 25 times more than that of carbon dioxide. Its influence on the greenhouse effect cannot be underestimated. Moreover, hydrogen sulfide is able to cause machine damage and pipeline corrosion easily. Therefore, the purpose of this study is to design a pressure swing adsorption separation process which can separate hydrogen sulfide, produce high-purity methane as the resources for renewable energy, and capture carbon dioxide to reduce greenhouse gas emission.
In this study, PSA simulation program was applied to separate biogas. The adsorbent is chosen based on literature, and the sorbent parameter calculated from experimental data of the adsorption equilibrium curve. The simulation process combined with the design of experiments is used to find out the optimal operating conditions for the separation of the three-component feed which contained CH4/CO2/H2S. To find the optimal operating conditions, the central composite design was conducted. Considering the biogas produced from the anaerobic fermentation of the excrement of 6,000 pigs per day, with the composition of 64.8% methane, 34.8% carbon dioxide, and 4,000 ppm hydrogen sulfide as the feed conditions. After analysis, the optimal operating conditions were obtained to produce a top product at 99.34% CH4 purity with 91.93 % recovery, and a bottom product at 96.37% CO2 purity with 49.16% recovery. The mechanical energy consumption was estimated to be 1.02 GJ/t-CH4 and 1.35 GJ/t-CO2. The methane production is 841.7 kg per day.

關鍵字(中)

★ 變壓吸附程序
★ 生質沼氣
★ 甲烷
★ 二氧化碳
★ 硫化氫

關鍵字(英)

★ Pressure swing adsorption
★ Biogas
★ Methane
★ Carbon dioxide
★ Hydrogen sulfide

論文目次

摘要 i
Abstract ii
誌謝 iii
目錄 iv
圖目錄 ix
表目錄 xiii
第一章、緒論 1
第二章、簡介及文獻回顧 7
2-1 吸附之簡介 7
2-1-1 吸附基本原理 7
2-1-2 吸附劑及其選擇性 8
2-1-3 吸附程序 10
2-1-4 突破曲線 12
2-2 研究目的及文獻回顧 14
2-2-1 PSA程序之發展與改進 15
2-2-2 理論之回顧 19
2-2-3 用於生質沼氣分離之吸附劑之回顧 22
2-2-3-1 分離甲烷與二氧化碳之比較 22
2-2-3-2 分離硫化氫之比較 23
2-2-3-3 吸附劑相關文獻回顧之結論 27
2-2-4 分離生質沼氣之變壓吸附程序之回顧 28
2-2-4-1 平衡吸附分離程序 28
2-2-4-2 動力學吸附分離程序 30
2-2-4-3 平衡與動力學分離程混合使用與比較 31
2-2-4-4 生質沼氣分離程序文獻回顧之結論 32
第三章、假設與理論 33
3-1 基本假設 34
3-2 統制方程式 34
3-3 吸附平衡關係式 39
3-3-1 等溫吸附平衡關係式 39
3-3-2 質傳驅動力模式(Driving force model) 40
3-3-3 吸附熱關係式 40
3-4 參數推導 41
3-4-1 軸向分散係數(Axial dispersion coefficient) 41
3-4-2 熱傳係數 43
3-4-3 線性驅動力質傳係數(Mass transfer coefficient of linear driving force) 45
3-5 邊界條件與流速 49
3-5-1 邊界條件與節點流速 49
3-5-2 閥公式 50
3-6 求解步驟 51
3-7 能耗及產率計算公式 54
第四章、模擬程序所需參數與驗證 55
4-1 吸附平衡 56
4-1-1 氣體與吸附劑性質 56
4-1-2 實驗裝置 57
4-1-3 實驗裝置之操作流程 60
4-1-4 天平校正 61
4-1-5 空白實驗 62
4-1-6 吸附劑對於二氧化碳與甲烷選擇性之比較 63
4-1-7 COSMO沸石13X之等溫平衡吸附曲線 68
4-2 吸附動力學 72
4-2-1 實驗裝置、各部規格及特性 72
4-2-2 突破實驗操作步驟 75
4-2-3 脫附實驗操作步驟 75
4-2-4 實驗室規模吸附塔之突破曲線與脫附曲線模擬驗證 76
4-3 模擬程序與實驗結果之驗證 79
4-3-1 單塔三步驟PSA實驗與模擬驗證 79
4-3-2 雙塔六步驟PSA實驗與模擬驗證 83
4-3-3 比較氮氣/二氧化碳與甲烷/二氧化碳分離程序 87
第五章、雙塔八步驟之三成分生質沼氣分離程序 88
5-1 進料流量、狀態以及組成 88
5-2 雙塔八步驟程序及參數 89
5-3 模擬程序結果與分析 92
第六章、以實驗設計求各響應最佳化結果 94
6-1 因子選定 94
6-2 反應曲面法(Response surface methodology, RSM) 95
6-2-1 殘差分析圖(Analysis of residual plots) 98
6-2-2 迴歸分析 103
6-3 各響應組合之最佳化結果 105
6-3-1 各響應之邊界值 105
6-3-1-1 塔頂輕產物甲烷純度極大值 105
6-3-1-2 塔底重產物二氧化碳純度極大值 107
6-3-1-3 塔頂輕產物甲烷回收率極大值 109
6-3-1-4 塔底重產物二氧化碳回收率極大值 110
6-3-1-5 捕獲每噸二氧化碳所需能耗極小值 111
6-3-1-6 捕獲每噸甲烷所需能耗極小值 112
6-3-1-7 每單位能耗可捕獲甲烷及二化碳之極大值 113
6-3-1-8 甲烷產率極大值 114
6-3-1-9 各響應邊界極值整理 115
6-3-2 各響應組合最佳化結果及參數 116
6-3-2-1 甲烷及二氧化碳純度最大化 116
6-3-2-2 塔頂輕產物甲烷回收率最大化 118
6-3-2-3 甲烷產率最大化 120
6-3-2-4 每噸甲烷能耗最小化 121
6-3-2-5 甲烷產率最大化同時每噸甲烷能耗最小化 122
6-3-2-6 響應組合最佳化結果整理 123
6-4 以模擬程序驗證最佳化響應與結果 124
6-4-1 各響應組合最佳化之模擬程序驗證 124
6-4-2 甲烷產率最大化同時每噸甲烷能耗最小化程序 128
6-4-3 等高線圖(Contour plot) 132
第七章、結論 133
符號說明 135
參考文獻 140
附錄A、流速之估算方法 146
附錄B、等溫吸附實驗數據 150
附錄C、 CCD結合ANOVA之參數與各響應值 153
附錄D、 CCD結合ANOVA之各響應回歸參數 162
附錄E、其他補充資料 163

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指導教授

周正堂楊閎舜

審核日期

2020-8-19

推文