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研究生： 楊淳善
Yang, Chun-Shan
論文名稱： 利用微型裝置篩選微生物燃料電池的發電條件
Using miniature device to screen the electric generation conditions of microbial fuel cell
指導教授： 吳意珣
Ng, I-Son
共同指導教授: 王翔郁
Wang, Hsiang-Yu
學位類別： 碩士
Master
系所名稱： 工學院 - 化學工程學系
Department of Chemical Engineering
論文出版年： 2016
畢業學年度： 104
語文別： 中文
論文頁數： 132
中文關鍵詞： 微生物燃料電池 、微型裝置 、空氣陰極 、篩選操作條件
外文關鍵詞： microbial fuel cell, micro-scale device, air-cathode, screening operational conditions
相關次數： 點閱：130  下載：6 
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    • 隨著能源缺乏及環境物染的問題日益受到重視，由於微生物燃料電池可以同時處理廢水與產電，因此成為替代性能源中發展的重要方向。一般在微生物燃料電池的條件篩選上需要大量的樣品、時間與成本，因此本研究利用無膜式微型層流微生物燃料電池(LF-μMFC)其開路電壓差來比較微生物在不同條件下的產電活性，並將結果與實驗室規模H型微生物燃料電池進行比對，驗證LF-μMFC可以應用於微生物與碳源之快速篩選。此外利用微型空氣陰極微生物燃料電池(AC-μMFC)來進行不同條件的連續式操作，亦發現其可以用來篩選微生物燃料電池的操作條件。利用微型裝置來快速篩選，可更有效率改善較大規模微生物燃料電池之操作條件與其產電效果。
    整個LF-μMFC的設計是為了盡量減少外界因素對於產電的影響，而純粹以開路電壓差來反映微生物的產電能力。本研究將此LF-μMFC應用在檢測不同碳源對於不同微生物產電的影響，所用的碳源包括：甘油、葡萄糖、蔗糖、醋酸鈉和乳酸。所用的微生物包括：Proteus hauseri ZMd44、Aeromonas hydrophila NIU01和Shewanella oneidensis MR-1。結果顯示，蔗糖較適合P. hauseri ZMd44產電；甘油較適合A. hydrophila NIU01產電；葡萄糖較適合S. oneidensis MR-1產電。為了驗證上述LF-μMFC之結果，接著利用H型微生物燃料電池進行不同微生物在不同碳源中的培養，P. hauseri ZMd44以蔗糖作為碳源之庫倫效率為最大約5.85 %。A. hydrophila NIU01以甘油作為碳源之庫倫效率為最大約3.38 %。S. oneidensis MR-1以葡萄糖作為碳源之庫倫效率為最大約0.63 %。將陽極電解液利用液相層析儀分析成分，可以發現代謝產物與產電趨勢及細胞濃度有關。不同微生物利用不同碳源產電會得到不同的代謝產物，P. hauseri ZMd44利用不同碳源產電的主要代謝產物皆為乙酸與丙酸；A. hydrophila NIU01利用甘油當碳源產電的主要代謝產物為1,3-丙二醇，利用其他碳源產電的主要代謝產物則是乙酸；S. oneidensis MR-1利用不同碳源產電的主要代謝產物皆為甲酸與乙酸。
    由於在先前的實驗中，P. hauseri ZMd44利用蔗糖作為碳源所得到的庫倫效率最高，因此研究後段探討增加蔗糖濃度對於產電會有什麼影響。先以LF-μMFC進行不同濃度蔗糖的產電測試，結果發現當蔗糖濃度提升至2.5倍時開路電壓差最高，但當蔗糖濃度提升至3倍以上時，開路電壓差反而降低。接著以H型微生物燃料電池來驗證其結果，P. hauseri ZMd44以2.5倍濃度蔗糖當碳源之庫倫效率約6.10 %；以3倍濃度蔗糖當碳源之庫倫效率約6.04 %。將陽極電解液利用液相層析儀分析成分，發現3倍濃度蔗糖組別的代謝產物中含有乙醇，可能為使產電輸出降低的原因。
    將H型微生物燃料電池與LF-μMFC所得的結果比較，發現LF-μMFC所測得的開路電壓差與H型微生物燃料電池的庫倫效率有高度的線性關係，證明此LF-μMFC可應用於篩選適合微生物燃料電池發電的碳源種類以及最佳碳源濃度，對於未來微生物燃料電池的條件篩選與最佳化有相當大的潛力。
    由於LF-μMFC雖然可應用在微生物以及碳源的快速篩選，但無法將足量的微生物培養在裝置中進行連續式培養或是操作條件的最適化，因此使用AC-μMFC進行不同操作條件的實驗。結果發現將微生物包覆在高分子電解質微粒中可以提升功率輸出，且減緩功率降低的速度；降低水力滯留時間會使輸出功率降低；提高碳源濃度則可以增加輸出功率，此結果證明AC-μMFC可應用在操作條件的篩選，對於未來微生物燃料電池的操作條件最佳化有相當大的潛力。

    This study using two miniature devices to screen the eleectric generation conditions of microbial fuel cell (MFC), one was the laminar flow micro-scale microbial fuel cell (LF-μMFC), and the other was the air-cathode micro-scale microbial fuel cell (AC-μMFC). Three kinds of microorganisms were utilized in this study: Proteus hauseri ZMd44, Aeromonas hydrophila NIU01, and Shewanella oneidensis MR-1. Five carbon sources (sucrose, glucose, glycerol, sodium acetate and lactic acid) were chosen as independent variable.
    When three microorganisms were investigated in the LF-μMFC, sucrose resulted in the highest ΔOCV for P. hauseri ZMd44, glycerol resulted in the highest ΔOCV for A. hydrophila NIU01 and glucose resulted in the highest ΔOCV for S. oneidensis MR-1. Next, lab-scale H-type MFCs were applied to confirm the results of LF-μMFC. Comparing the ΔOCV from LF-μMFC with the coulombic efficiency from H-type MFC, the results were highly correlateed. This shows that LF-μMFC can predict the efficiency of electricity generation in larger scale setup and has great potential in screening optimal conditions for MFCs.
    In order to find the optimal condition of electricity generation, several conditions were tested in AC-μMFC. When the microorganisms were encapsulated in polyelectrolyte microparticle, the output power is higher than directly form biofilm on the surface of the anode. When reducing hydraulic retention time, the output power was decreased. When raising concentration of carbon sources, the output power was increased. This shows that AC-μMFC has great potential in screening optimal conditions for MFCs.

    摘要 I Extended Abstract III 誌謝 VIII 目錄 IX 表目錄 XV 圖目錄 XVI 第一章 緒論 1 1-1 研究動機與目的 1 1-2 研究架構 2 第二章 文獻探討 3 2-1 微生物燃料電池的發展與歷史 3 2-2 微生物燃料電池的運作原理與介紹 3 2-3 微型化微生物燃料電池 11 第三章 實驗與材料 15 3-1 實驗材料 15 3-1-1 溶液配製 15 3-1-1-1 標準酸鹼溶液配製 15 3-1-1-2 陰極電解液 15 3-1-1-3 陽極電解液 16 3-1-1-3-1 產電用微生物 16 3-1-1-3-2 LB 培養液 16 3-1-1-3-3 微生物培養液 17 3-1-1-3-4 微生物培養液替換碳源 18 3-1-2 標準參考電極製備 20 3-1-3 微型層流微生物燃料電池(LF-μMFC)製備 22 3-1-3-1 黃光微影製程 22 3-1-3-1-1 鍍金微電極製作 22 3-1-3-1-2 矽晶圓模板 25 3-1-3-2 高分子翻模 26 3-1-3-3 微型微生物燃料電池組裝 27 3-1-4 H型微生物燃料電池製備 29 3-1-4-1 H型微生物燃料電池組裝 29 3-1-4-2 H型微生物燃料電池分析 30 3-1-5 微型空氣陰極微生物燃料電池(AC-μMFC)製備 32 3-1-5-1 電極製備 32 3-1-5-1-1 鍍金電極製備 32 3-1-5-1-2 碳布電極製備 33 3-1-5-2 高分子電解質微粒製備 33 3-1-5-2-1 矽晶圓模板 33 3-1-5-2-2 高分子翻模 34 3-1-5-2-3 微流道裝置製備 35 3-1-5-2-4 高分子電解質微粒製備 36 3-1-5-3 微型電池槽製備 38 3-1-5-4 微型空氣陰極微生物燃料電池(AC-μMFC)組裝 38 3-2 實驗儀器 41 3-2-1 溶液配製 41 3-2-2 標準參考電極製備 41 3-2-3 微型層流微生物燃料電池(LF-μMFC) 42 3-2-3-1 微型層流微生物燃料電池(LF-μMFC)製備與組裝 42 3-2-3-2 微型微生物燃料電池分析 44 3-2-4 H型微生物燃料電池 45 3-2-4-1 H型微生物燃料電池組裝 45 3-2-4-2 H型微生物燃料電池分析 45 3-2-5 微型空氣陰極微生物燃料電池(AC-μMFC) 46 3-2-5-1 微型空氣陰極微生物燃料電池(AC-μMFC)製備與組裝 46 3-2-5-2 微型空氣陰極微生物燃料電池(AC-μMFC)分析 47 3-3 實驗方法 48 3-3-1 溶液配製 48 3-3-1-1 標準酸鹼溶液配製 48 3-3-1-2 陰極電解液 48 3-3-1-3 陽極電解液 48 3-3-1-3-1 LB 培養液 48 3-3-1-3-2 微生物培養液 49 3-3-1-3-3 添加碳源量計算 49 3-3-2 標準參考電極製備 50 3-3-3 微型層流微生物燃料電池(LF-μMFC)製備 51 3-3-3-1 黃光微影製程 51 3-3-3-1-1 鍍金微電極製作 51 3-3-3-1-2 矽晶圓模板 53 3-3-3-2 高分子翻模 55 3-3-3-3 微型層流微生物燃料電池(LF-μMFC)組裝 55 3-3-3-4 電解液前處理 56 3-3-3-4-1 陽極電解液 56 3-3-3-4-2 陰極電解液 56 3-3-3-5 微型層流微生物燃料電池(LF-μMFC)架設與儀器設置 56 3-3-3-6 實驗觀察 57 3-3-4 H型微生物燃料電池製備 59 3-3-4-1 實驗前陽極電解液處理 59 3-3-4-2 H型微生物燃料電池組裝 59 3-3-4-3 H型微生物燃料電池分析 61 3-3-4-3-1 產電表現 61 3-3-4-3-2 功率曲線測量 61 3-3-4-3-3 細胞濃度測量 61 3-3-4-3-4 陽極電解液成分分析 61 3-3-5 微型空氣陰極微生物燃料電池(AC-μMFC)製備 63 3-3-5-1 電極製備 63 3-3-5-1-1 鍍金電極製備 63 3-3-5-1-2 碳布電極製備 63 3-3-5-2 陽極電解液前處理 64 3-3-5-3 高分子電解質微粒製備 65 3-3-5-3-1 矽晶圓模板 65 3-3-5-3-2 高分子翻模 65 3-3-5-3-3 微流道裝置組裝與改質 65 3-3-5-3-4 高分子電解質微粒生產 65 3-3-5-4 微型電池槽製備 68 3-3-5-5 微型空氣陰極微生物燃料電池(AC-μMFC)組裝 69 3-3-5-6 微型空氣陰極微生物燃料電池(AC-μMFC)架設與儀器設置 70 3-3-5-7 微型空氣陰極微生物燃料電池(AC-μMFC)分析 70 3-3-5-7-1 產電表現 70 3-3-5-7-2 細胞濃度測量 70 3-3-5-7-3 陽極電解液成分分析 71 第四章 結果與討論 72 4-1 碳源對於微生物於微型層流微生物燃料電池(LF-μMFC)產電的影響 72 4-1-1 Proteus hauseri ZMd44 72 4-1-2 Aeromonas hydrophila NIU01 73 4-1-3 Shewanella oneidensis MR-1 74 4-2 碳源對於微生物於H型微生物燃料電池產電的影響 75 4-2-1 Proteus hauseri ZMd44 75 4-2-1-1 產電表現 75 4-2-1-2 陽極電解液成分分析 79 4-2-2 Aeromonas hydrophila NIU01 84 4-2-2-1 產電表現 84 4-2-2-2 陽極電解液成分分析 87 4-2-3 Shewanella oneidensis MR-1 92 4-2-3-1 產電表現 92 4-2-3-2 陽極電解液成分分析 95 4-3 給予微生物不同碳源於微型層流微生物燃料電池(LF-μMFC)與H型微生物燃料電池產電結果比較 100 4-3-1 Proteus hauseri ZMd44 100 4-3-2 Aeromonas hydrophila NIU01 102 4-3-3 Shewanella oneidensis MR-1 104 4-4 不同蔗糖濃度對於微生物Proteus hauseri ZMd44產電的影響 107 4-4-1 微型層流微生物燃料電池(LF-μMFC) 107 4-4-2 H型微生物燃料電池 109 4-4-2-1 產電表現 109 4-4-2-2 陽極電解液成分分析 111 4-4-3 於微型層流微生物燃料電池(LF-μMFC)與H型微生物燃料電池 產電比較 113 4-5 不同因素對於微型空氣陰極微生物燃料電池(AC-μMFC)產電影響 115 4-5-1 微生物有無被包覆於高分子電解質微粒中對於產電的影響 115 4-5-2 不同水力滯留時間 118 4-5-3 不同碳源濃度 120 4-5-3-1 產電表現 120 4-5-3-2 出口成分分析 124 第五章 結論 125 5-1 結論 125 5-2 未來展望 126 參考文獻 127

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