臺灣博碩士論文加值系統

本研究論文包含兩個研究重點: (1)新型PProDOT衍生物對電極；(2)新型離子液體電解液。第一部分係用電化學聚合法備製導電高分子PProDOT衍生物poly(3,3-dibenzyl-3,4-dihydro-2H-thieno[3,4-b][1,4]dioxepine) (PProDOT-Bz2)、poly(3,3-dibutyl-3,4-dihydro-2H-thieno[3,4-b][1,4]dioxepine) (PProDOT-Bu2)與poly(3-(allyloxymethyl)-3-ethyl-3,4-dihydro-2H-thieno[3,4-b][1,4]dioxepine)(PProDOT-DB)。三種導電高分子PProDOT-Bz2、PProDOT-Bu2、PProDOT-DB摻雜少量白金作為染料敏化太陽能電池之對電極；藉以降低白金含量，製備低成本之染料敏化太陽能電池。由實驗結果可得知，添加導電高分子PProDOT-Bz2可使電荷轉移電阻(Charge Transfer Resistance, Rct)降低並提升電催化特性，進而提升光電轉換效率。最佳備製條件為0.05 C/cm2 PProDOT-Bz2與濺鍍30 s白金之複合對電極，其光電轉換效率可達3.50%；相當於濺鍍360 s白金對電極。另一方面，本研究亦合成兩種新型離子液體1-ethyl-1-(2-(2-(2-methoxyethoxy)ethoxy)ethyl)-piperidinium iodide (EMEEPII-1)與1-ethyl-1-(2-(2-methoxyethoxy)ethyl)-piperidinium iodide (EMEEPII-2)並作為染料敏化太陽能電池之電解液，並探討染料敏化太陽能電池於不同照度下，其光電特性之影響。由實驗結果可得知，當添加離子液體EMEEPII-1電解液之染料敏化太陽能電池，於30 mW/cm2之光照強度下其光電轉換效率可達4.50%。綜合上述結果，此論文備製之染料敏化太陽能電池新型PProDOT衍生物複合對電極及離子液體電解液，具備良好開發潛力備製低成本、簡易備製及可應用於不同光照強度之染料敏化太陽能電池。

The research of this thesis contains two research topics: (1) novel PProDOT derivative counter electrodes; (2) novel ionic liquid electrolytes. Three types of PProDOT-derivatives poly(3,3-dibenzyl-3,4-dihydro-2H-thieno [3,4-b][1,4]dioxepine) (PProDOT-Bz2), poly(3,3-dibutyl-3,4-dihydro-2H-thieno [3,4-b][1,4]dioxepine) (PProDOT-Bu2) and poly(3-(allyloxymethyl)-3-ethyl-3,4-dihydro-2H-thieno[3,4-b][1,4]dioxepine) (PProDOT-DB) were synthesized by electrochemical polymerization. PProDOT-Bz2, PProDOT-Bu2 and PProDOT-DB were doped with a small amount of platinum as the counter electrodes of dye-sensitized solar cells to decrease the platinum content and fabricate low cost dye-sensitized solar cells. According to the experimental results, the charge transfer resistances (Rct) of the counter electrodes comprising conductive polymer PProDOT-Bz2 and Pt with sputtering time of 30 s composite film were lower than that of Pt counter electrode with the sputtering time of 30 s, and further result in improving η. The best power conversion efficiency of the DSSC based on 0.05 C/cm2 PProDOT-Bz2/30 s Pt counter electrode is 3.50%, which is equivalent to that of Pt counter electrode with the sputtering time of 360 s. On the other hand, two novel ionic liquids 1-ethyl-1-(2-(2-methoxyethoxy) ethoxy)ethyl)-piperidinium iodide (EMEEPII-1) and 1-ethyl-1-(2-(2-methoxyethoxy)ethyl)piperidinium iodide (EMEEPII-2) was used as the electrolytes of dye-sensitized solar cells; the effect on the photovoltaics properties of dye-sensitized solar cells by the addition of ionic liquids EMEEPII-1 and EMEEPII-2 under different light intensities were systematically investigated. The power conversion efficiency of EMEEPII-1-based electrolyte is up to 4.50% under 30 mW/cm2 light intensity. Based on the above results, the novel PProDOT-derivatives counter electrodes and ionic liquid electrolytes have a great developed potential to prepare low cost, simple process DSSCs and can be applied to DSSCs under different light intensities.

Contents
摘要 i
ABSTRACT ⅱ
誌謝 iv
Contents vi
List of Tables x
List of Figures xii

Chapter 1 Introduction 1
1.1 Background 1
1.2 Overview of this thesis 2

Chapter 2 Theory and literature review 5
2.1 Introduction of Dye-Sensitized Solar Cell 5
2.2 Working Mechanism of Solar Cell 6
2.3 Composition of Dye-Sensitized Solar Cell 7
2.3.1 Substrate 7
2.3.2 Photoanode 8
2.3.3 Dye 8
2.3.4 Counter Electrode 9
2.3.5 Electrolyte 12
2.4 Overview of Ionic Liquids 13
2.4.1 Introduction of Ionic Liquid 13
2.4.2 Viscosity of Ionic Liquids 13
2.4.3 Density of Ionic Liquids 14
2.4.4 Conductivity of Ionic Liquids 14
2.4.5 Application of Ionic Liquids 14
2.5 Principles of Electrochemical Polymerization 15
2.6 Motivation 15

Chapter 3 Experimental 17
3.1 Flowchart of Fabrication Processes 17
3.2 Materials 18
3.2.1 Synthesis of PProDOT-derivatives 20
3.2.2 Synthesis of Ionic Liquid EMEEPII-1 and EMEEPII-226
3.3 Experimental and Measurement Instruments 30
3.3.1 Nuclear Magnetic Resonance Spectroscopy (NMR) 31
3.3.2 Radio Frequency Sputtering System 32
3.3.3 Furnace 33
3.3.4 Electrochemical Impedance Spectroscopy (EIS) 34
3.3.5 Electrochemical Analyzer 35
3.3.6 Field emission Scanning Electron Microscopy (FE-SEM) 36
3.3.7 Solar Simulator Measurement System 38
3.4 Experimental Procedures 39
3.4.1 Substrate Cleaning 39
3.4.2 Counter Electrode 39
3.4.3 Preparation of Electrolytes 41
3.4.4 Preparation of TiO2 Film 42
3.4.5 Preparation of Dye Solution 42
3.4.6 Assembly of the Dye-Sensitized Solar Cells 42

Chapter 4 Results and Discussion 44
4.1 Characteristics and Analyses of Conjugated Polymer
Counter Electrodes 44
4.1.1 Electrochemical Polymerizations of Conjugated Polymer
Counter Electrodes 44
4.1.2 Surface Morphologies of Conjugated Polymer Counter
Electrodes 46
4.1.3 Photovoltaic Characteristics of Conjugated Polymer
Counter Electrodes 54
4.2 Characteristics and Analyses of Conjugated Polymer/Pt
Composite Films 58
4.2.1 Surface Morphologies of DSSCs with Different
Conjugated Polymer/Pt Composite Films 58
4.2.2 Photovoltaic Characteristics of DSSCs with Different
Conjugated Polymer/Pt Composite Films 65
4.2.3 Electrochemical Impedance Spectroscopy of DSSCs with
Different Conjugated Polymer/Pt Composite Film 69
4.2.4 Cyclic Voltammetry of DSSCs with Different Conjugated
Polymer/Pt Composite Films 75
4.3 Characteristics and Analyses of Different Ionic
liquids-based Electrolytes 78
4.3.1 Basic properties of Different Ionic liquid 78
4.3.2 Photovoltaic Characteristics of DSSCs with Different
Ionic liquids-based electrolytes 86
4.3.3 Electrochemical Impedance Spectroscopy of DSSCs with
Different Ionic liquids-based electrolytes 90
4.4 Photocurrent-Voltage Characteristics of DSSCs with Conjugated Polymer CEs and Ionic liquids-based electrolytes under Different Light Intensities 93

Chapter 5 Conclusions 98

Chapter 6 Future Prospects 99

References 100

 

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