臺灣博碩士論文加值系統

本研究主要以黑磷烯(Phosphorene)摻入二氧化鈦(Titanium dioxide, TiO2)膠體中，並通過刮刀法沉積於氟摻雜氧化錫(Fluorine-doped tin oxide, FTO)導電玻璃作為染料敏化太陽能電池之光電極。其原因為黑磷烯擁有高電子遷移率與高光吸收率之特性，可以增強二氧化鈦薄膜電子傳輸與增加逆向復合阻抗，藉此可進一步達到提升電流密度之目的。本研究藉由掃描電子顯微鏡分析黑磷烯之表面結構；以紫外光-可見光吸收光譜儀量測薄膜之光吸收率；以電化學阻抗分析儀量測染料敏化太陽能電池之內部阻抗。相較於純二氧化鈦光電極之染料敏化太陽能電池，其光伏轉換效率為3.50%，添加適量黑磷烯於二氧化鈦光電極之染料敏化太陽能電池，最佳光伏轉換效率達4.35%，光伏轉換效率增加24%。
此外，本研究以射頻濺鍍系統沉積銀修飾鉑對電極以提升染料與電解液之間的氧化還原反應，其原因為銀具有高導電率，根據晶格應變效應使薄膜造成拉伸應變，使薄膜提升吸附能力。本研究以銀之不同厚度探討其銀鉑對電極之導電率及催化效率。藉由掃描電子顯微鏡分析鉑與銀之表面結構；以四點探針量測系統量測鉑銀對電極之片電阻；以電化學阻抗分析儀量測染料敏化太陽能電池之內部阻抗。相較於純鉑對電極，鉑銀對電極可以提供更高的導電率和更佳的催化活性。染料敏化太陽能電池之光伏轉換效率從鉑對電極之3.82%提升至鉑銀對電極之4.46%，光伏轉換效率增加16%。最後，將黑磷烯修飾二氧化鈦光電極與銀修飾鉑對電極之最佳複合薄膜染料敏化太陽能電池於低照度下進行探討，於1.75 mW/cm2照度下之光伏轉換效率為7.21%，相較於100 mW/cm2照度下之4.76%，光伏轉換效率增加52%。

In this study, phosphorene was mixed with titanium dioxide (TiO2) colloid and deposited on fluorine-doped tin oxide (FTO) conductive substrate by doctor blade method as the photoelectrode of dye-sensitized solar cell (DSSC). The reason is because phosphorene has high electron mobility and high absorption, which could enhance the electron transfer ability and increase the recombination resistance, thus improve the current density. The surface morphology of phosphorene film was characterized by field-emission scanning electronic microscopy (FE-SEM). The optical absorption of phosphorene-TiO2 composited film was measured by UV–visible spectrometer. The interface resistance of DSSC was measured by electrochemical impedance spectroscopy. Compared with the photovoltaic conversion efficiency of 3.50% based on pure TiO2 photoelectrode, it is found that the optimal photovoltaic conversion efficiency of 4.35% is achieved when the phosphorene is introduced to TiO2 photoelectrode, and the efficiency increases by 24%.
More than that, silver (Ag) was deposited by radio frequency sputtering to modify the conventional platinum (Pt) counter electrode to enhance the redox reaction between electrolyte and dye molecule. The reason is because Ag has the highest electrical conductivity in metal, and the lattice strain effect will increase the surface absorption ability of film. The silver modified Pt counter electrode with different Ag thicknesses was investigated for electrical conductivity and catalytic activity. The surface morphology of Pt/Ag counter electrode was characterized by FE-SEM. The sheet resistance of Pt/Ag counter electrode was measured by 4-point probing system. The interface resistance of DSSC was measured by electrochemical impedance spectroscopy. Compared with the pure Pt counter electrode, the silver modified Pt counter electrode can provide a higher electrical conductivity and a superior catalytic activity. Moreover, the photovoltaic conversion efficiency of DSSC can be enhanced from 3.82% with the Pt counter electrode to 4.46% with the Pt/Ag counter electrode, and the efficiency increases by 16%. Finally, the DSSC of optimal composited films with phosphorene-TiO2 photoelectrode and Pt/Ag counter electrode was investigated under low illumination. The photovoltaic conversion efficiency of the DSSC can be enhanced from 4.76% under illumination of 100 mW/cm2 to 7.21% under illumination of 1.75 mW/cm2 and the efficiency increases by 52%.

摘要 i
ABSTRACT ii
誌謝 iv
Table of contents v
List of Tables viii
List of Figures ix
Chapter 1 Background and Motivation 1
1.1 Background 1
1.1.1 Advances in Energy Technologies 1
1.1.2 Types of Solar Cell 1
1.1.3 Dye-sensitized Solar Cell 4
Chapter 2 Literature Survey 7
2.1 Structure of Dye-sensitized Solar Cell 7
2.1.1 Transparent Conductive Oxide 8
2.1.2 Compact Layer 9
2.1.3 Photoelectrode 9
2.1.4 Dye 13
2.1.5 Electrolyte 15
2.1.6 Counter Electrode 15
2.2 Principle of Dye-sensitized Solar Cell 17
2.3 Photovoltaic Properties of Dye sensitized Solar Cell 19
2.3.1 Short-circuit Current Density (JSC) 19
2.3.2 Open-circuit Voltage (VOC) 19
2.3.3 Fill Factor (F. F.) 19
2.3.4 Photovoltaic Conversion Efficiency (η) 21
2.4 Efficiency Improvement of Dye-sensitized Solar Cell 22
2.4.1 Improvement of Photoelectrode 22
2.4.2 Improvement of Counter Electrode 24
Chapter 3 Experimental 26
3.1 Materials 26
3.2 Fabrication Procedure of Dye-sensitized Solar Cell 28
3.2.1 Preparation of Transparent Conductive Oxide Substrate 28
3.2.2 Fabrication of Compact Layer 28
3.2.3 Fabrication of Phosphorene-TiO2 Photoelectrode 28
3.2.4 Fabrication of Platinum/Silver Counter Electrode 30
3.2.5 Fabrication of N3 Dye 30
3.2.6 Fabrication of Electrolyte 30
3.2.7 Fabrication of Dye-sensitized Solar Cell 31
3.3 Measurement Systems 33
3.3.1 Field-Emission Scanning Electron Microscope (FE-SEM) 33
3.3.2 Atomic Force Microscope (AFM) 35
3.3.3 Radio Frequency Sputtering System 37
3.3.4 Solar Simulator Measurement System 39
3.3.5 4-Point Probing System 41
3.3.6 Alpha-Step (α-Step) Surface Profilometer 43
3.3.7 Electrochemical Impedance Spectroscopy (EIS) 45
3.3.8 Cyclic Voltammetry (CV) 47
3.3.9 Ultraviolet-Visible Spectroscopy (UV-vis) 49
Chapter 4 Results and Discussion 51
4.1 Analysis of Photoelectrodes 51
4.1.1 Raman Characteristics of Phosphorene 51
4.1.2 Characterization of Phosphorene-TiO2 Composited Film and TiO2 Film 53
4.1.3 Optical Properties of Phosphorene-TiO2 Composited Films 57
4.1.4 Dye Adsorption of Phosphorene-TiO2 Composited Films 61
4.1.5 Electrochemical Impedance Characteristics of Phosphorene-TiO2 Composited Films 63
4.1.6 Photovoltaic Characteristics of Dye-Sensitized Solar Cell with Phosphorene-TiO2 Composited Films 65
4.2 Analysis of Counter Electrodes 67
4.2.1 Characterization of Platinum Film and Silver Film 67
4.2.2 The AFM Measurement of Counter Electrodes 69
4.2.3 Effects of Platinum/Silver Film Thicknesses on Sheet Resistance of Counter Electrodes 73
4.2.4 Catalytic Properties of Platinum/Silver Counter Electrodes 75
4.2.5 Electrochemical Impedance Characteristics of Different Platinum/Silver Counter Electrodes 78
4.2.6 Photovoltaic Characteristics of Different Platinum/Silver Counter Electrodes for Different Silver Sputtering Time 80
4.2.7 Comparison between the 200-nm-thick Pt CE and the Pt/Ag (2min) CE 82
4.3 Fabrication of Dye-sensitized Solar Cell under Low Illumination 84
4.3.1 Effect of Photovoltaic Characteristics under Different Illumination 84
Chapter 5 Conclusion 86
Chapter 6 Future Works 88
References 89
Appendices口試委員之問題與建議 99

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