臺灣博碩士論文加值系統

中文摘要
對於廢棄物排放量逐年遞增，加上原物料上漲及環保意識，其在處理及資源化方面，將朝向資源化潛力發展，如廚餘、下水道污泥與畜牧業之糞便等。有機廢棄物經厭氧處理，藉由微生物分解有機物轉化為電能及氫能，但以固體廢棄物之研究甚少，因此，將模擬都市固體廢棄物配製合成垃圾 (Synthetic MSW) 作為微生物燃料電池 (Microbial fuel cell, MFC) 與微生物電解電池 (Microbial electrolysis cell, MEC) 之基質，探討本實驗篩選產氫菌之最佳生長環境因子與產氫效率，並馴化微生物燃料電池之藻類，作為微生物電解電池之電力來源，評估整體功率與藻類產油量之相關性。
單槽式微生物電解電池工作體積4公升，進料量依固體物停留時間 (Solid retention time, SRT) 20天為200 mL d-1合成垃圾基質，出料之消化產物進行各項參數分析；結果顯示，在不同電壓 (0 V、0.3 V、0.6 V、0.9 V, Cathode PEM) 與不同電極 (0.6 V, Cathode PEM、MEA) 操作條件下，累積產氣量以0.9 V 之陰極PEM (0.9V Cathode PEM) 與0.6 V之MEA (0.6V MEA) 為最佳條件，分別是40,050 mL與57,800 mL，在pH 5.4 ~ 6.0、ORP -200 ~ -300 mV與EC 0.74 ~ 1.65 mS cm-1的環境因子，每克VS可獲得最大產氣量80 ~ 85 mL g-1VS；並以不同預處理方式篩選厭氧污泥，找尋適合合成垃圾基質之操作條件，且提高氫氣純度，其中以酸篩條件氫氣濃度可高達57.20 %，其次為未處理41.90 %，證實當pH 在4 ~ 5之間呈現酸化現象可有效抑制甲烷菌，且提高氫氣純度。
雙槽式微生物燃料電池工作體積各為1.5公升，陽極依固體物停留時間20天計算進料量為75 mL d-1，出料之消化產物比照微生物電解電池參數分析，陰極以藻類生成氧氣作為電子接受者，並分析藻類油脂含量，且將兩種反應槽串聯 (Algae MFC - MEC)，以微生物燃料電池電力供給微生物電解電池產氫 (MEA)；結果顯示，串聯後可提高電壓0.84 V、功率密度5.46mW m-2及油脂量430.5 mg g-1，但因電阻累加而降低電流密度為24.3 mA m-2；在Algae MFC - MEC產能效率方面，電子還原效率與氫氣還原效率最高可達到8.41 % 與6.15 %，而庫倫效率為28.68 %，略低於以電源供應器供給電力之反應槽，但與施加0.6 V, Cathode PEM相比，氫氣純度明顯差相10 %，每克VS可獲得最大產氫量為101.9 mL-H2 g-1VS。

Abstract
In this study, organic waste was used to investigate microbial electrolysis cell (MEC, 4 L) and microbial fuel cell (MFC, 1.5 L) for electricity, hydrogen and biofuel production.
This study was divided into three parts, the first part investigated the different voltage (0, 0.3, 0.6 and 0.9 V) for optimal biogas production. Biogas accumulation of 0, 0.3, 0.6 and 0.9 V was found to be 34,000, 35,050, 37,500 and 40,050 mL respectively. The coulombic efficiency was also found to be 6.23, 11.94, 16.30 and 37.74% respectively. It was found that 0.6 V was suitable for biogas production. MFC could produce 0.89 voltage (V) and algal oil (biofuel) 430.5 mg g-1. MEC could produce hydrogen of 101.9 mL-H2 g-1VS. Internal resistance of traditional plates (4,000 - 6,000 Ω) allocation was found to decrease to be 400 - 600 Ω in the MEA allocation. Biogas accumulation and coulombic efficiency of traditional plates and MEA allocation reached 21,100 and 57,800 mL and 15.48 and 28.68% respectively. The maximum power density and algae oil content were found to be 36.67 mA m-2 and 109.8 ~ 430.5 mg g-1 respectively. Biogas composition from MEC with MEA allocation was analyzed to be H2 8.44%, CH4 41.59% and CO2 49.97% at VS 3.64 - 4.69%. The maximum hydrogen production is 101.9 mL-H2 g-1. The electron reduction efficiency (Ee) and hydrogen reduction efficiency (EH) reached 8.41% and 6.15% respectively which was slightly lower than those in the literatures.

中文摘要 I
Abstract III
致謝 V
第一章 前言 1
1.1 研究緣起 1
1.2 研究目的 3
第二章 文獻回顧 4
2.1 氫能 4
2.2 產氫技術 5
2.2.1 熱化學法 6
2.2.2 電化學法 6
2.2.3 生物法 7
2.4 厭氧發酵產氫原理 12
2.4.1 厭氧污泥預處理 13
2.5 厭氧發酵代謝途徑 14
2.6 微生物燃料電池原理 15
2.6.1 陽極反應 16
2.6.2 陰極反應 17
2.7 微生物燃料電池設計 18
2.7.1 雙槽微生物燃料電池 18
2.7.2 單槽微生物燃料電池 19
2.8 微生物燃料電池影響因子 20
2.8.1 微生物種類 20
2.8.2 基質種類 22
2.8.3 電極材料 23
2.8.4 質子交換膜 25
2.9 藻類 27
2.9.1 油脂生成 28
2.9.2 光合作用 29
2.9.3 藻類培養種類 30
2.10 微生物電解電池原理 31
2.11 微生物電解電池設計 32
2.12 微生物電解電池影響因子 35
2.12.1 微生物菌種 35
2.12.2 甲烷對產氫影響 36
2.12.3 內電阻 37
2.12.4 膜電極組 38
第三章 材料與方法 40
3.1 實驗設計與流程 40
3.2 實驗材料 41
3.2.1 實驗設備及軟體 41
3.2.2 植種污泥 42
3.2.3 藻類 44
3.2.4 合成垃圾基質 44
3.2.5 電極材料 45
3.2.6 質子交換膜 (Proton exchange membrane, PEM) 46
3.2.7 電極膜組製作 (Membrane electrode assembly, MEA) 46
3.3 藻類MFC設計 48
3.4 MEC設計 49
3.5 分析參數 51
3.5.1 產氣量 51
3.5.2 酸鹼值 (pH) 51
3.5.3 氧化還原電位 (Oxidation-reduction potential, ORP) 51
3.5.4 導電度 (Electrical conductivity, EC) 51
3.5.5 溶氧量 (Dissolved oxygen, DO) 51
3.5.6 吸光值 (Optical density, OD) 52
3.5.7 光照度 (Illuminance) 52
3.5.8 化學需氧量 (Chemical oxygen demand, COD) 52
3.5.9 鹼度揮發酸 (Alkalinity, Volatile acids) 53
3.5.10 總固體物 (Total solids, TS) 與揮發性固體物 (Volatile solids, VS) 53
3.5.11 懸浮固體 (Suspended solids, SS) 54
3.5.12 油脂含量分析 54
3.5.13 氣相層析儀 (GC/TCD) 55
3.6 電能計算與分析 57
3.6.1 電流與功率密度 57
3.6.2 庫倫效率 57
3.7 氫氣產能計算與分析 58
3.7.1 電子還原效率 58
3.7.2 氫氣轉換效率 59
第四章 結果與討論 60
4.1 微生物電解電池之參數分析 60
4.1.1 產氣量 60
4.1.2 酸鹼值 (pH) 63
4.1.3 氧化還原電位 (ORP) 65
4.1.4 導電度 (EC) 66
4.1.5 化學需氧量 (COD) 與揮發性固體物 (VS) 之相關性 67
4.1.6 揮發酸 (Volatile acids) 69
4.2 藻類微生物燃料電池與微生物電解電池串聯之參數分析 72
4.2.1 基本監測參數 72
4.2.2 電壓與電流密度之變化 75
4.2.3 藻類油脂含量分析 76
4.2.4 藻類生長濃度分析 77
4.2.5 庫倫效率 (CE) 78
4.2.6 電子還原效率 (Ee) 80
4.2.7 氫氣還原效率 (EH) 81
4.2.8 氣體成分分析 (GC/TCD) 82
4.2.9 不同預處理之厭氧消化污泥 84
第五章 結論與建議 86
5.1 結論 86
5.2 建議 89
參考文獻 91


表目錄
表2-1 產氫微生物 ............................................................................................... 8
表2-2 產氫技術優缺點 ....................................................................................... 9
表2-3 菌種熱處理產氫率 ................................................................................. 14
表2-4 陽極反應化學式 ..................................................................................... 17
表2-5 陰極半反應式 ......................................................................................... 17
表2-6 純種與混種產電菌之差異 .................................................................... 21
表2-7 產電菌之基質利用種類......................................................................... 22
表2-8 微生物燃料電池之不同基質產電差異 ................................................ 23
表2-9 不同電子接受者對微生物燃料電池之產電效率 ................................ 25
表2-10 雙槽MEC與單槽MEC之菌種比例 ................................................. 35
表3-1 實驗設備及軟體 ..................................................................................... 41
表3-2 實驗設備及軟體 (續) ............................................................................ 42
表3-3 植種污泥馴化前後之特性 .................................................................... 43
表3-4 藻類培養條件 ......................................................................................... 44
表3-5 合成垃圾基質、台中垃圾及台灣垃圾元素分析 ................................ 45
表3-6 電極規格與性質 ..................................................................................... 45
表3-7 碳氈電極元素含量表............................................................................. 45
表3-8 氣相層析儀氣體分析條件 .................................................................... 56
表3-9 各項計算公式表 ..................................................................................... 57
表3-10 庫倫效率計算公式表........................................................................... 58
表3-11庫倫效率計算公式表 (續) ................................................................... 58
表3-12電子還原效率計算公式表 ................................................................... 59
表3-13氫氣轉換效率計算公式表 ................................................................... 59


圖目錄
圖1-1 再生能源綜論 ........................................................................................... 2
圖2-1 產氫技術圖 ............................................................................................... 5
圖2-2 厭氧消化反應流程 ................................................................................. 13
圖2-3 葡萄糖發酵代謝途徑............................................................................. 15
圖2-4 微生物燃料電池原理圖......................................................................... 16
圖2-5 各類雙槽式微生物燃料電池架構圖(A) H型微生物燃料電池；(B) 上流式微生物燃料電池；(C)、(D) 改良式雙槽微生物燃料電池 ............ 19
圖2-6 單槽式微生物燃料電池架構圖(A) 典型單槽式微生物燃料電池；(B) 圓柱式單槽微生物燃料電池；(C) 改良式單槽微生物燃料電池 ......... 20
圖2-7 質子交換膜分子結構示意圖 ................................................................ 26
圖2-8 氫離子在水中之三種型態 .................................................................... 27
圖2-9 擬球藻生長曲線與油脂量之時間趨勢圖 ............................................ 28
圖2-10 油脂生成途徑 ....................................................................................... 29
圖2-11 光合作用途徑 ....................................................................................... 30
圖2-12 MFC (左圖)與MEC (右圖)原理架構圖 .............................................. 31
圖2-13 微生物電解電池反應架構圖(A) 單槽管柱型MEC；(B) 單槽無膜型MEC；(C) H型雙槽式MEC；(D) 半自動管柱型MEC ....................... 33
圖2-14 單槽式MEC ......................................................................................... 34
圖2-15 MEA結構 .............................................................................................. 39
圖3-1 本研究實驗架構圖 ................................................................................. 40
圖3-2 本研究熱篩之內胞子............................................................................. 43
圖3-3 碳氈元素分析圖 ..................................................................................... 46
圖3-4 MEA製作示意圖 .................................................................................... 47
圖3-5 MEA (左圖) 與陰極PEM (右圖)成品 .................................................. 47
圖3-6 藻類微生物燃料電池示意圖 ................................................................ 49
圖3-7 微生物電解電池示意圖......................................................................... 50
圖3-8 藻類微生物燃料電池與微生物電解電池串聯示意圖 ........................ 50
圖4-1 不同電壓施予微生物電解電池之產氣趨勢圖 .................................... 61
圖4-2 不同電極配置於微生物電解電池之產氣趨勢圖 ................................ 62
圖4-3 陰極PEM與MEA之內電阻合鬚圖 ................................................... 63
圖4-4 不同電壓施予微生物電解電池之pH趨勢圖 ..................................... 64
圖4-5 不同電極配置於微生物電解電池之pH趨勢圖 ................................. 64
圖4-6 不同(A圖)電壓與(B圖)電極配置於微生物電解電池之ORP趨勢圖 ..................................................................................................................... 65
圖4-7 不同(A圖)電壓與(B圖)電極配置於微生物電解電池之EC趨勢圖 66
圖4-8 不同電壓施予微生物電解電池之COD去除效率 (A圖) 與VS (B圖) 趨勢圖 ......................................................................................................... 67
圖4-9 不同電極配置於微生物電解電池之COD去除效率 (A圖) 與VS (B圖) 趨勢圖 .................................................................................................. 68
圖4-10 不同電壓施予微生物電解電池之揮發酸趨勢圖 .............................. 69
圖4-11 不同電壓施予微生物電解電池之揮發酸與產氣量關係圖 .............. 70
圖4-12 不同電極配置於微生物電解電池之揮發酸趨勢圖 .......................... 70
圖4-13 不同電極配置於微生物電解電池之揮發酸與產氣量關係圖 .......... 71
圖4-14 藻類微生物燃料電池串聯微生物電解電池之pH、ORP、EC趨勢圖 ..................................................................................................................... 73
圖4-15 藻類微生物燃料電池串聯微生物電解電池之pH、ORP、EC盒鬚圖 ..................................................................................................................... 74
圖4-16 藻類微生物燃料電池串聯微生物電解電池之電壓與電流密度變化 ..................................................................................................................... 75
圖4-17 藻類微生物燃料電池與微生物電解電池串聯前後之內電阻合鬚圖 ..................................................................................................................... 76
圖4-18 藻類微生物燃料電池串聯微生物電解電池之功率密度與油脂量變化 ................................................................................................................. 77
圖4-19 藻類乾重對應OD值之檢量線 ........................................................... 77
圖4-20 不同電壓及電極配置於微生物電解電池之庫倫效率 ...................... 78
圖4-21 藻類MFC串聯MEC (MEA) 與陰極PEM (0.6V) 之產氣合鬚圖 . 79
圖4-22 不同電壓及電極配置於微生物電解電池之電子還原效率 .............. 80
圖4-23 不同電壓及電極配置於微生物電解電池之氫氣還原效率 .............. 81
圖4-24 氣體成分分析圖A) 以陰極PEM測之氣體成分百分比；B)藻類MFC串連MEC (MEA) 測之氣體成分百分比 ................................................ 82
圖4-25 微生物電解電池每克VS產生之氫氣量 ........................................... 83
圖4-26 厭氧污泥以不同預處理之pH趨勢圖 ............................................... 85
圖4-27 厭氧污泥以不同預處理之氣體成分百分比 ...................................... 85

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