本研究旨在從分子工程的面向開發高效率之染料敏化太陽能電池(DSSC)。目前已設計了許多染料，並結合不同的氧化還原介質應用於DSSC中。除了新穎的染料外，DSSC組成中的氧化還原介質、對電極之電化學特性及其對元件性能的影響皆被深入地研究，使其逐漸發展成熟。
染料敏化太陽能電池以弱光(像是螢光及LED等光源)下具有較好的光捕獲能力而聞名，然而DSSC在弱光與太陽光之性質差異非常大，因此大多數高效率之DSSC都是針對弱光條件下去設計的。在此，我們針對新穎的全色釕金屬染料進行研究，其帶有三級丁基取代的6-quinolin-8-yl-2,2’-bipyridine與外圍的輔助基團C3F7，不僅提升了可見光與近紅外光區域之光捕獲能力效率，還能有效抑制介面再結合。在太陽光模擬器與T5螢光下，TF36染料結合I-/I3-氧化還原介質的最佳效率分別為10.37%和31.82%。值得注意的是，此效率不需要共敏化及修改製作元件之流程即可達到。
在接下來的章節中，介紹了一種供體-π-受體結構的有機染料。此染料以1,2-di(anthracene-9-yl)ethyne基團作為延伸的 π-bridge，並且在第二個蒽基的4,5-位結合了雙羧基，第二個蒽基以及兩個錨定基團的引進能讓吸收光譜紅移以及改善元件的穩定性。
第四章針對新型“雙柵欄”結構的鋅-卟啉染料之開創性工作去做討論，該結構帶有四個在鄰位被長烷氧基取代的 β-苯基卟啉環。相較於其“單柵欄”內消旋替代之對應物，新提出的“雙柵欄”卟啉染料與Co3+/ Co2+氧化還原介質一起使用在抑制染料聚集與介面再結合有更好的表現。
第五章介紹了一系列根據Cu2+/ Cu+氧化還原介質所設計的蒽基-bridge染料。在蒽基 2,6-位取代的長鏈烷基抑制了染料聚集與電子再結合，得到 1.12 V 的高光電壓。此外，該染料在照度6000勒克斯之T5螢光下表現出37%的創紀錄效率。
第六章深入探討了TBP與[Cu(dmp)2] 2+/+的配位機制及其與元件穩定性的關係。通過光度滴定、循環伏安法和質子核磁共振光譜法證實了電解質中形成了新的氧化還原物質，並研究了它們在對電極處對電荷轉移的電化學性質。
TBP對原本氧化還原對造成破壞的解決方法將在接下來的兩章中被介紹。第一種解決方法使用了一系列的吡啶衍生物來檢查電解液添加物之結構對配位的影響，並研究了它們對電化學特性的影響，以期能提高元件的穩定性；第二種解決方法是透過分子工程設計一個以dmodmbp作為螯合配位基之新的銅氧化還原介質，不僅提升了PCE，而且還提高了元件的穩定性。
最後一章介紹了一種用於銅氧化還原對的新型鉑對電極材料。PVA-Pt奈米團簇的合成採用化學還原法，並以一種新型聚合物作為穩定劑；而PVA-Pt對電極是在沒有表面活性劑幫助的情況下透過“一步”浸漬法製備而成的。結合沉積機制，對 PVA-Pt 對電極的電化學特性進行了評估，顯示出其在[Cu(dmp)2] 2+/+氧化還原對下具有良好的催化表現。

The study focuses on the preparation of high-efficiency dye-sensitized solar cells (DSSCs) from various perspectives. In including sensitizer innovation, Cu(I)/Cu(II) redox couple implantation and nanosized Pt counter electrode renovation.
The first section summarizes comprehensive investigation of four novel sensitizer systems. In chapter 2, we report a novel panchromatic ruthenium(II)-based sensitizer bearing tert-butyl substituted 6-quinolin-8-yl-2,2’-bipyridine ancillary with peripheral C3F7, which not only enhances light harvesting efficiency in visible and near-IR region, matching with fluorescent light spectrum but also suppresses interfacial recombination. The best-performing sensitizer TF36 with iodide/triiodide (I-/I3-) redox system exhibits efficiency of 10.37 % and 31.82 % under simulated sunlight and T5 fluorescent, respectively. It is worth to mention that the device does not require modification of fabrication or co-sensitization. In the following chapter, a donor-π-acceptor organic sensitizer DY2, featuring 1,2-di(anthracene-9-yl)ethyne as an extended π-bridge with a dual carboxylic group incorporated at 4,5-positions of the second anthracene moiety is introduced. The introduction of second anthracene moiety and double anchors is in order to (i) red shift the absorption spectra and (ii) improve device stability.
In chapter 4, a pioneering work on zinc-porphyrin-based sensitizer using novel “double fence” architecture, dye bJS2, bearing four β-phenyl porphyrin rings substituted with long alkoxyl groups at the ortho-positions is presented. The proposed “double fence” porphyrin sensitizer used with tris-(2,2’-bipyridine)cobalt(III/II) redox mediator outperforms to its “single fence” meso-substituted counter parts due to better suppression of aggregation and interfacial recombination. In chapter 6, a series of anthracene-bridged sensitizers, namely CXC12 and CXC22, designed for copper(II/I) complex mediator is introduced. Long alkyl chains substituted at 2,6-positions of the anthracene on CXC12 suppress dye aggregation and electron recombination, yielding remarkable high photo-voltage of 1.12V. Meanwhile, its counterpart sensitizer CXC22 exhibits record efficiency of 37 % under 6000 lux T5 fluorescent illumination.
The second section of this dissertation dives into the mechanism of 4-tert-butylpyridine (TBP) coordination with bis(2,9-dimethyl-1,10-phenanthroline) copper(II/I), [Cu(dmp)2] 2+/+, and its connection to device stability. In chapter 6, the formation of new redox species in the electrolyte is confirmed by photometric titration, cyclic voltammetry, and proton nuclear magnetic resonance spectroscopy. In addition, their electrochemical properties toward charge transfer at counter electrode are also investigated. The solutions for TBP poison effect on Cu(dmp)2] 2+ are presented in chapter 7, where we examine the effect of additive structure to coordination behavior by using a series of pyridine derivatives. Their effects on electrochemical properties are carefully investigated with the intention of improving long-term stability of device. The second approach is molecularly engineered a new copper(II/I) complex mediator, which is presented in chapter 8. By using 4,4-dimethoxy-6,6’-dimethyl-2,2’-bipyridine), dmodmbp, as chelating ligand, new copper(II/I) complex not only improves PCE but also long-term stability.
The final section of this dissertation is a renovation project on polymer-capped Pt nanocluster-based counter electrode. We publish a unprecedent efficient Pt-based counter electrode material for copper(II/I) complex mediator. By using chemical reduction method, together with a new polymer as a stabilizer, polyvinyl alcohol-capped Pt (PVA-Pt) nanoclusters are synthesized. PVA-Pt counter electrode is prepared by “one-step” dipping process without the help of surfactant. Together with deposition mechanism, the electrochemical properties of PVA-Pt counter electrode are evaluated, showing excellent catalytic performance to [Cu(dmp)2] 2+/+ redox couple.

Acknowledgement------------------------------------------------- i
Abbreviations--------------------------------------------------- ii
Abstract-------------------------------------------------------- iv
摘要------------------------------------------------------------ vi
Table of Contents----------------------------------------------- viii
List of Figures and Schemes------------------------------------- xv
List of Table----------------------------------------------------xxiii
Chapter 1 Introduction-------------------------------------------1
1.1 Evolution of Photovoltaics-----------------------------------1
1.2 Dye-Sensitized Solar Cells-----------------------------------2
1.2.1 Configuration and working mechanism of Dye-sensitized Solar Cells------------------------------------------------------------3
1.2.2 Key components of Dye-sensitized Solar Cells---------------4
1.3 Poison issues in copper complex-based electrolyte------------14
1.4 Counter electrode for copper complex-based electrolyte-------16
1.5 Development of dye-sensitized solar cells for indoor applications------------------------------------------------------------------17
1.6 Main characterization methods--------------------------------19
1.6.1 Current-voltage (I-V) characteristics----------------------19
1.6.2 Electrochemical Impedance Spectroscopy---------------------21
1.7 The Aim of This Study----------------------------------------24
Chapter 2 High Efficiency Thiocyanate-Free Ruthenium Dye for Both of Outdoor and Indoor Applications----------------------------------26
2.1 Introduction-------------------------------------------------27
2.2 Experimental-------------------------------------------------29
2.2.1 Photophysical measurements---------------------------------29
2.2.2 DSSC fabrication-------------------------------------------29
2.2.3 Photovoltaic performance characterization------------------30
2.2.4 Measurement of device performance under dim light:---------31
2.2.5 EIS measurement--------------------------------------------31
2.2.6 Stability Test---------------------------------------------31
2.3 Results and Discussion---------------------------------------31
2.3.1 Optical and electrochemical properties---------------------31
2.3.2 Photovoltaic performance under different light sources-----33
2.4 Conclusion---------------------------------------------------42
Chapter 3 Anthracene-based Sensitizers with Double Anchors for Efficient and Stable Dye-Sensitized Solar Cells------------------44
3.1 Introduction-------------------------------------------------45
3.2 Experimental-------------------------------------------------46
3.2.1 Optical and Electrochemical measurements-------------------46
3.2.2 Device Fabrication for DSCs--------------------------------46
3.2.3 Measurement of device performance under artificial sun simulator:-------------------------------------------------------47
3.2.4 EIS Measurement of device performance:---------------------48
3.2.5 Stability Test---------------------------------------------48
3.3 Results and discussions--------------------------------------48
3.3.1 Optical and electrochemical properties---------------------48
3.3.2 Photovoltaic performance-----------------------------------51
3.3.3 Electrochemical impedance spectroscopy study---------------53
3.3.4 Device stability-------------------------------------------54
3.4 Conclusions--------------------------------------------------56
Chapter 4 Novel Double Fence Porphyrins Sensitizers for High Efficiency Dye-Sensitized Solar Cells----------------------------57
4.1 Introduction-------------------------------------------------58
4.2 Experimental-------------------------------------------------59
4.2.1 Device fabrication-----------------------------------------60
4.2.2 Photovoltaic performance characterization------------------60
4.2.3 Electrochemical impedance spectroscopy (EIS) measurement---61
4.2.4 Electrochemical measurements-------------------------------61
4.3 Results and discussions--------------------------------------61
4.3.1 Optical and electrochemical properties---------------------62
4.3.2 Density functional theory study----------------------------64
4.3.3 Photovoltaic Performance of DSSCs--------------------------65
4.3.4 Electrochemical impedance spectroscopy study---------------68
4.4 Conclusion---------------------------------------------------70
Chapter 5 Molecular Engineering of Anthracene-Bridged Sensitizer for Indoor Dye-Sensitized Solar Cells--------------------------------71
5.1 Introduction-------------------------------------------------72
5.2 Experimental-------------------------------------------------74
5.2.1 DFT calculations-------------------------------------------74
5.2.2 Electrochemical measurements-------------------------------74
5.2.3 Device fabrication-----------------------------------------74
5.2.4 Photovoltaic performance characterization------------------75
5.2.5 Measurement of device performance under dim light----------75
5.2.6 Electrochemical impedance spectroscopy (EIS) measurement---76
5.3 Results and Discussion---------------------------------------76
5.3.1 Optical and electrochemical properties---------------------76
5.3.2 Theoretical investigation----------------------------------80
5.3.3 Photovoltaic performance of CXC-based DSSCs with copper-based electrolyte------------------------------------------------------81
5.3.4 Electrochemical Impedance Spectroscopy study.--------------85
5.3.5 Device stability ------------------------------------------87
5.4 Conclusion.--------------------------------------------------88
Chapter 6 Tert-butylpyridine Coordination with [Cu(dmp)2]2+/+ Redox Couple and its Connection to the Stability of the Dye-sensitized Solar Cell-------------------------------------------------------------90
6.1 Introduction-------------------------------------------------91
6.2 Experimental Section-----------------------------------------92
6.2.1 Synthesis of copper complex--------------------------------92
6.2.2 DSSC fabrication-------------------------------------------92
6.2.3 Solar cell characterization--------------------------------94
6.2.4 UV-Vis measurement-----------------------------------------94
6.2.5 Electrochemical Characterization---------------------------94
6.2.6 NMR measurement--------------------------------------------94
6.3 Results and Discussion---------------------------------------95
6.4 Conclusions--------------------------------------------------108
Chapter 7 Stable Lewis base additive for copper complex-mediated dye-sensitized solar cells-------------------------------------------109
7.1 Introduction-------------------------------------------------110
7.2 Experimental-------------------------------------------------111
7.2.1 DSSC fabrication-------------------------------------------112
7.2.2 Characterization methods-----------------------------------112
7.3 Results and Discussions--------------------------------------113
7.3.1 Photophysical study----------------------------------------113
7.3.2 1H-NMR spectroscopy study----------------------------------117
7.3.3 Cyclic voltammetry measurement-----------------------------119
7.3.4 Electrochemical impedance spectroscopy---------------------121
7.3.5 Photovoltaic performance-----------------------------------122
7.3.6 Electron transport and recombination study-----------------123
7.3.7 Device stability-------------------------------------------125
7.4 Conclusions--------------------------------------------------127
Chapter 8 Stable Dye-Sensitized Solar Cells Based on New Copper(II/I) Complex Redox Mediator-------------------------------------------128
8.1 Introduction-------------------------------------------------129
8.2 Experimental-------------------------------------------------130
8.2.1 Optical and electrochemical properties---------------------130
8.2.2 Device fabrication-----------------------------------------131
8.2.3 Photovoltaic performance characterization------------------131
8.3 Results and discussions--------------------------------------131
8.3.1 Optical properties-----------------------------------------131
8.3.2 Electrochemical properties---------------------------------133
8.3.3 Photovoltaic performance-----------------------------------136
8.3.4 Device stability-------------------------------------------137
8.4 Conclusions--------------------------------------------------137
Chapter 9 Efficient polyvinyl alcohol-capped platinum counter electrode for copper complex-mediated dye-sensitized solar cells-139
9.1 Introduction-------------------------------------------------140
9.2 Experimental-------------------------------------------------141
9.2.1 Preparation of polymer-capped Pt nanoclusters--------------141
9.2.2 Preparation of counter electrode---------------------------141
9.2.3 Fabrication of DSSC----------------------------------------143
9.2.4 Characterizations------------------------------------------144
9.3 Results and Discussion---------------------------------------145
9.3.1 Characterization of Pt nanoclusters------------------------145
9.3.2 Deposition mechanism of PVA-Pt and PVP-Pt on FTO-----------146
9.3.3 Optical property, morphology and Pt loading of CEs---------149
9.3.4 Electrochemical catalytic performance of CEs---------------153
9.3.5 Photovoltaic performance and electrochemical stability-----156
9.4 Conclusion---------------------------------------------------158
Chapter 10 Conclusions-------------------------------------------159
Appendix---------------------------------------------------------163
References-------------------------------------------------------167
Curriculum Vitae-------------------------------------------------180

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