臺灣博碩士論文加值系統

本研究論文主要針對無”白金”對電極進行系統性的開發，與設計新型不含”透明導電氧化基材”，應用於低成本、高效率之染料敏化太陽能電池。本研究論文主要可分為兩大部分：(1)無白金對電極(第三章和第四章)；(2)無白金和無透明導電氧化基材對電極(第五章和第六章)。
無白金對電極之開發主要目的為降低染敏電池之製造成本，透過簡單、非真空、低成本的製程製備多種電催化觸媒材料，用以完全取代昂貴的白金材料。因此，本研究論文首先以碘系統電解質為標準，進行三大類的無白金複合對電極之開發。(一)過渡金屬化合物型：包含第三章中的二硒化鈷/三氧硒化鈷之奈米方體、奈米棒狀、奈米顆粒；第四章中的二硒化鈷/三氧硒化鈷之複合奈米海膽狀結構。(二) 過渡金屬/導電高分子型：包含硒化鉬奈米片/PEDOT:PSS複合薄膜於第五章，可提供高表面積、快速電解質滲透、良好的附著力、快速碘離子還原反應。(三) 碳材型：純碳氣凝膠於第六章被討論，該材料被前驅物間苯二酚(R)/甲醛(F)和間苯二酚(R)/碳酸鈉(C)的摩耳比控制比表面積。無白金和無透明導電氧化基材對電極中，鈦板與碳氣凝膠用來取代透明導電氧化基材，因為它們的低成本、容易製備與易量產化，(一)鈦板與硒化鉬奈米片/PEDOT:PSS複合薄膜搭配應用於染敏中具有8.51 ± 0.05%的效率，高於白金於鈦板上的效率8.21 ± 0.02%。(二)碳氣凝膠取代整個傳統對電極 (白金/透明導電氧化層/玻璃基材)，該染敏電池與CA-C CE搭配下，有著效率9.08 ± 0.01%，高於其他碳氣凝膠。總而言之，本研究論文開發三種無白金複合奈米薄膜：二硒化鈷/三氧硒化鈷、硒化鉬奈米片/PEDOT:PSS、碳氣凝膠，為可取代白金之替代材料，因為他們皆具有良好的催化碘還原能力、低成本、簡易製程、易於大面積製備等特性。

This dissertation aimed to systematically study Pt-free and TCO-free counter electrodes (CEs) with low-costs and highly cell efficiencies (η’s). This dissertation is divided into two parts: (1) Pt-free CEs (Chapter 3 and Chapter 4) and (2) Pt-free and TCO-free CEs (Chapter 5 and Chapter 6).
In the case of Pt-free CEs, we aim to reduce the costs of the DSSCs using various electro-catalysts for completely replacing the expensive Pt via the simple, non-vacuum, and low-cost fabrication processes. Accordingly, three types of Pt-free composite films were studied using a standard iodide electrolyte. (I) Transition metallic compound-type CEs, i.e. CoSe2/CoSeO3 with nanocube (NC), nanorod (NR), and nanoparticle (NP) structures in Chapter 3, the composite films of CoSe2/CoSeO3 with hierarchical urchin-like structure in Chapter 4, were indivitually investigated. In the composite film, the different nanostructures were separately used to provide attractive electro-catalytic abilities and large active areas for I3- reduction. (II) Transition metallic and conducting polymer type CEs, i.e. MoSe2 NS/PEDOT:PSS in Chapter 5, were investigated to provide large surface area, fast eletrolyte penetration, well adhesion, and rapid reaction rate for I3- reduction. (III) Carbonaceous-type CEs, i.e. pristine monolithic carbon aerogel (CA-O, CA-Q, CA-F, CA-C, and CA-G) in Chapter 6, were investigated by controlled resorcinol (R)/formaldehyde (F) and resorcinol (R)/sodium carbonate (C) molar ratios. In the case of Pt-free and TCO-free CEs. In the case of Pt-free and TCO-free CEs, the classic TCO substrate is replaced by Ti foil and carbon aerogel for low-cost, simple preparation process, and large-scale production. (I) Ti foil substrate collocate with MoSe2 NS/PEDOT:PSS, which presents a higher η of 8.51 ± 0.05%, as compared to a lower η of 8.21 ± 0.02% using the Pt-coated Ti foil CE. (II) Carbon aerogel replace traditional CEs based on the Pt/FTO/glass in DSSCs. The DSSCs using the as-prepared CA-C CE gave the best η of 9.08 ± 0.01%, among all the CA CEs. In brief, this dissertation explores three Pt-free composite films of CoSe2/CoSeO3, MoSe2 NS/PEDOT:PSS, and CA are a promising substitutions of Pt due to their outstanding properties, i.e., good electro-catalytic ability for I3– reduction, low-cost, simple preparation process, and easy for large-scale production.

Table of Contents
中文摘要 I
Abstract II
Table of Contents III
List of Tables VI
List of Figures VIII
Nonmenclatures XIII
Chapter 1 Introduction 1
1-1 Background of DSSCs 1
1-2 Mechanism of DSSCs 3
1-3 Sun light and photovoltaic performance of solar cells 5
1-4 Counter electrodes in DSSCs 7
1-4-1 Transition metallic compound-type 9
1-4-2 Conducting polymer-type 13
1-4-3 Carbonaceous-type 16
1-5 Motivation 20
Chapter 2 Experimental 25
2-1 Materials 25
2-2 Fabrication of photoanodes 26
2-3 Fabrication of counter electrodes 28
2-4 Preparation of electrolytes and DSSC assembly 30
2-5 Analytical techniques 31
2-5-1 Morphology, optical, and electrical properties 31
2-5-2 Photovoltaic performance 31
2-5-3 Electrochemical properties 32
Chapter 3 Microemulsion-controlled synthesis of CoSe2/CoSeO3 composite crystals for electrocatalysis in dye-sensitized solar cells 36
3-1 Abstract 36
3-2 Introduction 36
3-3 Results and discussions 39
3-3-1 Phase behavior 39
3-3-2 FE-SEM analyses 40
3-3-3 X-ray diffraction patterns and X-ray photoelectron spectra 42
3-3-4 Photovoltaic performance 43
3-3-5 Cyclic voltammetry 47
3-3-6 Tafel polarization curves and electrochemical impedance spectra 49
3-3-7 Dim light 51
3-4 Summary 52
Chapter 4 One step synthesized hierarchical urchin-like structure CoSe2/CoSeO3 electro-catalysts for dye-sensitized solar cells: up to 19% at dim light illumination 54
4-1 Abstract 54
4-2 Introduction 54
4-3 Results and discussions 58
4-3-1 FE-SEM analyses 58
4-3-2 X-ray diffraction patterns and X-ray photoelectron spectra 59
4-3-3 Photovoltaic performance 60
4-3-4 Cyclic voltammetry 63
4-3-5 Electrochemical impedance spectra and Tafel polarization curves 65
4-3-6 Dim light 67
4-4 Summary 69
Chapter 5 MoSe2 nanosheet/poly(3,4-ethylenedioxythiophene): poly(styrenesulfonate) composite film as a Pt-free counter electrode for dye-sensitized solar cells 70
5-1 Abstract 70
5-2 Introduction 71
5-3 Results and discussions 72
5-3-1 FE-SEM and EDX analyses 72
5-3-2 Photovoltaic performance and IPCE spectra of DSSCs 76
5-3-3 Cyclic voltammetry 79
5-3-4 Rotating disk electrode analysis 81
5-3-5 Tafel polarization curves and electrochemical impedance spectra 83
5-3-6 Flexible counter electrode 85
5-4 Summary 88
Chapter 6 A Pt-free pristine monolithic carbon aerogel counter electrode for dye-sensitized solar cells: up to 20% at dim light illumination 90
6-1 Abstract 90
6-2 Introduction 90
6-3 Results and discussions 92
6-3-1 FE-SEM analysis 92
6-3-2 Brunauer-Emmett-Teller analysis 94
6-3-3 Photovoltaic performance 95
6-3-4 Cyclic voltammetry 99
6-3-5 Electrochemical impedance spectroscopy and Tafel polarization curves 100
6-3-6 Dim light 101
6-4 Summary 103
Chapter 7 Conclusions and suggestions 104
7-1 Conclusions 104
7-2 Suggestions 105
References 106
Appendix Curriculum vitae 127

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