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系統識別號 U0002-0407201218182600
中文論文名稱 四氧化三鈷修飾陰極以提升希瓦氏腐敗菌為基底之微生物燃料電池之發電效益研究
英文論文名稱 The Research of Enhancing the Electricity Production of Shewanella putrefaciens - based Microbial Fuel Cell by Modifying Cobalt Oxide on the Cathode
校院名稱 淡江大學
系所名稱(中) 化學學系碩士班
系所名稱(英) Department of Chemistry
學年度 100
學期 2
出版年 101
研究生中文姓名 陳作榮
研究生英文姓名 Tso-Jung Chen
學號 698160446
學位類別 碩士
語文別 英文
口試日期 2012-05-28
論文頁數 169頁
口試委員 指導教授-林孟山
委員-呂晃志
委員-劉茂煌
委員-林孟山
中文關鍵字 微生物燃料電池  四氧化三鈷  氧氣還原反應  希瓦氏腐敗菌 
英文關鍵字 Microbial fuel cell  Cobalt(II,III) oxide  Oxygen reduction reaction  Shewanella putrefaciens 
學科別分類 學科別自然科學化學
中文摘要 微生物燃料電池是一種新穎的潔淨能源產出方案來因應即將到來的能源危機,與傳統燃料電池主要的差異在於它毋須使用金屬催化劑修飾陽極,而是使用特定微生物來催化有機分子的氧化,進而將得到的電子傳遞給陽極。接著經由電池外部導線而傳遞給陰極槽的氧氣,並與來自陽極並通透過半透膜的氫離子結合產生水的終產物。然而氧氣的還原反應需要很高的過電壓,在動力學上不利於反應進行,因此需要催化劑。傳統上,白金被廣泛的使用,然而它確有價格過於高昂的缺點,會大幅增加電池的生產成本。因此,本研究以探尋較為廉價的氧氣還原反應催化劑與其反應機制為目標,發現使用金屬氧化物修飾陰極具有能催化氧氣還原並增加微生物燃料電池功率的能力,最終決定使用四氧化三鈷。
本研究中尚探討了四氧化三鈷催化氧氣還原的機制與特性,並進一步進行電池操作參數的最佳化,條件為: 使用Co3O4做為催化劑,修飾比例為70%,陽極槽培養液pH值為5,以葡萄糖做為受質,陰極槽使用磷酸緩衝溶液,pH值設定為5,兩極距離為一公分。研究發現50%的四氧化三鈷可達到5%的白金修飾電極之催化效果,在電池功率方面,與使用僅修飾純導電碳膠的陰極之微生物燃料電池相比,電池最大功率密度在最佳化條件下提升9.53倍。本研究也進行了交流阻抗與電池生命週期的分析。
英文摘要 Microbial fuel cell (MFC) is a novel and clean energy source solution to imminent energy crisis. In contrast to conventional fuel cell, microbial fuel cell, instead of using metal catalyst as anode material, takes advantage of microorganisms to catalyze oxidation organic matters. The released electrons were then transferred to oxygen in catholyte through the external conductive wire. Combining with protons permeates from anolyte, thus the final product was water (H2O). However, the reduction reaction’s nature of high overpotential hinders its spontaneity thermodynamically. As a result, utilizing catalyst for oxygen reduction reaction (ORR) is necessary and inevitable. Conventionally, platinum is served as most frequently used catalyst material, but its high cost may limit large scale production of fuel cell. Therefore, the goal of this study is to search for more cost-effective catalyst material and to evaluate the reaction mechanism for oxygen reduction reaction as replacement of platinum. It is found that metal oxides can be potential candidates for acting as catalyst for oxygen reduction reaction; in the meanwhile, enhance power output efficiency of MFC. In the end, Co3O4 is chosen as the final option.
The catalysis mechanism and performance of ORR for Co3O4 is evaluated. In addition, the optimization of operating parameters has been undergone. The optimized conditions are: adopting Co3O4 as cathode catalyst material, modification ratio 70wt.%, anolyte as medium of pH5, glucose used as substrate, pH5 phosphate buffer solution served as catholyte, electrode distance of 1cm. In this study, the effect of modifying 50wt.% of Co3O4 is comparable to 5wt.% of Co3O4. In comparison to the MFC with pure conductive carbon ink modified cathode, the power density is enhanced 9.53 times. The evaluation of electrochemical impedance spectroscopy and life time of MFC is also studied.
論文目次 Contents
Chapter 1 Preface 7
1.1 Research motives 7
1.2 Development History of Microbial Fuel Cell 9
1.2.1 Designs of Anode Configuration 11
1.2.2 Microorganisms used in MFCs 15
1.2.3 Various Sources of Substrates for Microorganisms in Anode Chamber 22
1.2.4 Designs of Cathode Configuration 26
1.2.5 MFCs for waste and pollution reduction 37
1.2.6 MFCs for Hydrogen Production 48
1.3 Principle of Microbial Fuel Cells 51
1.4 Performance Characterization of Microbial Fuel Cells 53
1.5 Configurations of MFC 54
1.6 Electrochemical Impedance Spectroscopy 57
1.7 Brief Introduction of Cobalt (II, III) Oxide (Co3O4) 59
1.8 Research goals 60
Chapter 2 Experimental Section 62
2.1 Configuration of Microbial Fuel Cell and its Assembly 62
2.2 Instruments 65
2.2.1 Electrochemical Analysis 65
2.2.2 Power Output Analysis 66
2.2.3 Microorganism Incubation 67
2.2.4 Others 67
2.3 Chemicals 68
2.3.1 Chemicals Preparation 69
2.4 Electrodes Preparation for Electrochemical Analyzer 70
2.4.1 Pretreatment of Electrodes 70
2.4.2 The Preparation of Co3O4 – modified Electrode 71
2.5 Experimental Methods 71
2.5.1 The Evaluation of Oxygen Reduction Mechanism 71
2.5.2 The optimization of the MFC Power Output Performance 72
2.5.3 Electrochemical Impedance Spectroscopy 77
2.5.4 Life Time of the MFC 77
2.6 Characterization of Co3O4 78
Chapter 3 Results and Discussion 79
3.1 Design of a Cathode Suitable for the Development of MFC 79
3.2 The Effect of Catholyte pH 91
3.3 The Effect of Catholyte Buffer Solution Type on the Catalysis Behavior of Co3O4 94
3.4 The Evaluation of Catalysis Mechanism 96
3.5 The Anolyte pH Determination 109
3.6 Substrate for Bio-assisted Organic Compound Oxidation Study 114
3.7 The Effect of Electrode distance on the Performance of MFC 116
3.8 The Modification Ratio of Co3O4 on the Cathode 118
3.9 The Effect of Catholyte pH 121
3.10 Compromised pH in Both Chamber 124
3.11 Electrochemical Impedance Spectroscopy of Optimized MFC 126
3.12 Life Time Study 129
3.13 The Optimized Operating Parameters of MFC 130
3.14 Characterization of Co3O4 131
3.15 General Current-Potential Curves at the RDE 133
Chapter 4 Conclusion 136
Appendix 137
Reference 151


Graph Contents
Figure (1) Schematic diagram of the MFC Principle……………………….…..……55
Figure (2) Schematic diagram of the single-chambered MFC……………….………57
Figure (3) Schematic diagram of the Dual-chambered MFC………………….……..58
Figure (4) Schematic diagram of the Tubular Up-flow MFC………………………..58
Figure (5) Schematic of Co3O4 Structure…………………………………….………61
Figure (6) Schematic of Microbial Fuel Cell Assembly…………………….……….68
Figure (7) I-V Curve of the Co3O4 – modified GCE…………………………..……..84
Figure (8) I-V Curve of the CuO – modified GCE……………………………….….84
Figure (9) I-V Curve of the Fe2O3 – modified GCE…………………...........……….85
Figure (10) I-V Curve of the Fe3O4 – modified GCE……………………………..…85
Figure (11) I-V Curve of the NiO2 – modified GCE………………………..……..…86
Figure (12) I-V Curve of the CaTiO3 – modified GCE…………………………....…86
Figure (13) I-V Curve of the LiMn2O4 – modified GCE……………………….……87
Figure (14) I-V Curve of the WO2 – modified GCE…………………………………87
Figure (15) I-V Curve of the Pb3O4 – modified GCE………………………….…….88
Figure (16) Stable I-V Curve of the Fe3O4 – modified GCE………………….…..…89
Figure (17) Stable I-V Curve of the LiMn2O4 – modified GCE…………….……….89
Figure (18) Steady-state currents at 0V - Fe3O4 – modified GCE……………..…….90
Figure (19) LSV - Effect of catholyte pH……………………………..….………….94
Figure (20) Power density – voltage polarization curve - Effect of catholyte pH…...95
Figure (21) LSV - Effect of catholyte buffer kind……………………………………97
Figure (22) Steady-state reduction current vs. each potential - Pure conductive carbon
ink – modified GCE………………………………………………………………….99
Figure (23) Steady-state reduction current vs. each potential - 10 wt.% Co3O4 -
modified GCE………………………………………………………….…………...100
Figure (24) Steady-state reduction current vs. each potential - 30 wt.% Co3O4 -
modified GCE……………………………………………………………….……...100
Figure (25) Steady-state reduction current vs. each potential - 50 wt.% Co3O4 -
modified GCE……………………………………………………………….……...101
Figure (26) Steady-state reduction current vs. each potential - 70 wt.% Co3O4 -
modified GCE……………………………………………………………….……...101
Figure (27) Steady-state reduction current vs. each potential - 50 wt.% platinum
coated carbon powder - modified GCE….……………………………….….……...102
Figure (28) I-t amperometric plot (0.4V) - 50 wt.% Co3O4 – modified
RRDE….………………………………...…………………………………..……...104
Figure (29) I-t amperometric plot (0.3V) - 50 wt.% Co3O4 – modified
RRDE….………………………………...…………………………………..……...104
Figure (30) I-t amperometric plot (0.2V) - 50 wt.% Co3O4 – modified
RRDE….………………………………...…………………………………..…..….105
Figure (31) I-t amperometric plot (0.1V) - 50 wt.% Co3O4 – modified
RRDE….………………………………...…………………………………..…..….105
Figure (32) I-t amperometric plot (0V) - 50 wt.% Co3O4 – modified
RRDE….………………………………...…………………………….…………....106
Figure (33) I-t amperometric plot (-0.1V) - 50 wt.% Co3O4 – modified
RRDE….………………………………...…………………………….……………106
Figure (34) I-t amperometric plot (-0.2V) - 50 wt.% Co3O4 – modified
RRDE….………………………………...…………………………….……….…...107
Figure (35) I-t amperometric plot (-0.3V) - 50 wt.% Co3O4 – modified
RRDE….………………………………...………………………………….……....107
Figure (36) I-t amperometric plot (-0.4V) - 50 wt.% Co3O4 – modified
RRDE….………………………………...………………………………….……....108
Figure (37) I-t amperometric plot (-0.5V) - 50 wt.% Co3O4 – modified
RRDE….………………………………...…………………………………….…....108
Figure (38) I-t amperometric plot (-0.6V) - 50 wt.% Co3O4 – modified
RRDE….………………………………...……………………………………….....109
Figure (39) Signals of oxygen vs. applied potential plot - 50 wt.% Co3O4 – modified
RRDE….……….……………...……………………………………………....…....109
Figure (40) Calibration plot of H2O2 - 50 wt.% Co3O4 – modified
RRDE….……….……………...………………………………...………….……....110
Figure (41) Proposed ORR mechanism on Cobalt (II, III) oxide modified
electrode…………………………………………………………………………….110
Figure (42) LSV - Effect of culture medium pH on the performance of
anodes….……….…………………...…………………………...…………….…....113
Figure (43) LSV - Effect of culture medium pH on the performance of
anodes….……….…………………...…………………………...………….……....114
Figure (44) Power density – voltage polarization curve - Effect of culture medium
pH….……….…….………...…………………………...………………...…...…....114
Figure (45) LSV - Effect of various subsrates on the performance of the
anode….……….…………………...…………..………………...………….……....117
Figure (46) Power density – voltage polarization curve - Effect of electrode distance
on the performance of the microbial fuel cell…………………………………...….119
Figure (47) LSV - Effect of modification ratio…………………………….……….121
Figure (48) Power density – voltage polarization curve - Effect of modification
ratio….……….…….………...…………………...……………...………….……....122
Figure (49) Modification ratio vs. maximum power density……………………….122
Figure (50) LSV - Effect of catholyte pH…………………………………………..124
Figure (51) Power density – voltage polarization curve - Effect of catholyte
pH…………………………………………………………………………………...125
Figure (52) Plot of pH vs.time…………………………………………..………….127
Figure (53) Power density – voltage polarization curve - Effect of both chambers with
the same pH……………………………………..………………………….…….…128
Figure (54) EIS data of MFC performed as Nyquist plot………………….………..130
Figure (55) Equivalent circuit for two-chambered MFC…………………….……..130
Figure (56) The life time of MFC…………………………………….…………….131
Figure (57) The XRD spectrum of Co3O4…………………………………………..133
Figure (58) FE-SEM images of Co3O4……………………………………………...133
Figure (59) Variation of 1/i with ω-1/2 at 0V………………………………………...136
Figure (60) Variation of i with ω at 0V……………………………………………...136

Table Contents
Table (1) Electrochemical parameters used in MFCs study………………………….56
Table (2) The open circuit potential of each metal oxide – modified
GCE………………………………………………………..………….……………...90
Table (3) The performances evaluation of various metal oxides as cathodic
modifier………………………………………………………………………….…...92
Table (4) The open circuit potential of 50 wt.% Co3O4 – modified GCE in each kind
of buffer solution……………………………………………………………….…….94
Table (5) The open circuit potential of anodes incubated with various pH
medium…………………………………………………………………….…...…...112
Table (6) The open circuit potential of MFC with various electrode
distances.....................................................................................................................116
Table (7) The open circuit potential of GCE coated with various modifier………...120
Table (8) The open circuit potential of cathode modified with 50 wt.%
Co3O4……………………………………………………………………………......122
Table (9) Various parts of internal resistances of MFC……………………….…….127
Table (10) Optimized operating parameters
table………………………………………………………………………………....129
Table (11) Rate constants corresponding to each applied potential………………...137
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