染料敏化太陽能電池（染敏電池）是一種最有希望的有機太陽能光電系統之一， 理論上借由n型和p型染敏電池的結合成串疊型電池， 其優化效率可以達到43% 。 事實上， n型染敏電池效率已可超過14%，然而另一半p型染敏電池的效率卻連其十分之一都不到。 因此，達到最優化效率的瓶頸自然是被p型這部分所限制住， 特別是在p型和n型兩端缺乏適合的光陰極半導體材料和有機染料。
在第三章中，我們報導了使用化學共沉澱方法進行氧化鎳納米材料的表面活性劑介導合成。 通過XRD、SEM、XPS、EDS和BET充分鑑定新材料。 BET結果指出用表面活性劑合成的氧化鎳納米顆粒獲得比常規表面積更高的表面積。 EDS結果表明，兩種材料中鎳和氧的原子組成百分比，在樣品NiO / DTAB中，氧含量略有減少，鎳的相對增加。使用新合成材料元件搭配市售的染料：C-343，測試 p型的性能，最高效率為0.0418％，高於不含DTAB的NiO所得元件性能的0.0253％。 通過表面活性劑介導的合成製備的NiO的染料吸附量，比不使用DTAB製備的材料高約35％。
在第四章中，用新製備的NiO作為光陰極，製備了用於p型染料敏化太陽能電池，其中染料分子結構為摻入缺電子二苯基喹喔啉的新型有機染料。新的有機染料由羧酸作為錨基團、三苯胺作為電子供體、2,3-二苯基喹喔啉作為輔助受體部分、2-亞甲基丙二腈作為電子受體，並使用噻吩、3,4-亞乙二氧基噻吩和2,2'-聯噻吩作為π-間隔基。具有單錨基團的敏化劑（EH166，EH122和EH174）比其相應的雙錨敏化劑（EH162，EH126和EH170）表現更好。其中，染料EH174的轉換效率最高可達0.207％，短路光電流密度為4.84 mAcm-2，開路光電壓為137 mV，填充因子為0.312。目前的結果表明，在D-A-π-A分子結構中，缺電子喹喔啉與合適的π-連接基的的p型敏化劑，對基於NiO的p-DSSC，是有前途的設計。我們還研究了具有n型光電陽極的串聯電池性能，其具有EH174的元件表現最佳，效率為2.05％，EH122達到1.99％。
在第五章中，我們報告了摻雜鎵的氧化鎳光電陰極材料，對高性能p型染料敏化太陽能電池的適用性。通過不同的表徵技術研究了不同鎵質量比（1％，5％和10％）的鎵摻雜的性質和影響。較高濃度的鎵離子改善了光電壓，但隨著鎵（III）量的增加，光電流顯著下降。電荷提取和費米能級分析表明，隨著鎵質量的增加，開路電壓也跟著增加，是由於價帶能量的正向移動。 p-DSSC結果表明，與NiO-0％Ga的元件相比，1％摻雜鎵的氧化鎳納米材料，顯示出約23％的效率增強。如XPS研究所證實，在較高的鎵濃度（5％和10％）下，載體濃度-Ni3+降低。根據EDS結果證實，鎵離子與氧化鎳納米晶體的結合調節載流子濃度，並誘導氧化鎳納米顆粒的氧缺乏和化學吸附氧的變化。因此，將鎵（III）摻雜到氧化鎳納米顆粒中，應是對於設計和製造p-DSSC高性能光電陰極來說，是相當有前景的材料，。
第六章評估了最近有前途的水性染料敏化太陽能電池，它結合了低成本和環境兼容性。 在本研究中，我們研究了鹼鹽濃度對基於碘化物 - 三碘化物的氧化還原介質的化學性質的影響，其為串聯染料敏化太陽能電池應用提供了完全水性環境。 我們使用方酸 - 芳基胺敏化劑（p-SQ2）作為p型染料和基於喹喔啉-三苯胺的n型染料（MA169）來構建串聯染料敏化太陽能電池。 在H3水性電解質組合中，獲得的串聯裝置的最佳效率為VOC = 0.655V，Jsc = 1.720 mAcm-2，FF = 0.432和η= 0.487％。
在第七章中，通過使用不同的π-間隔物，設計和合成了四種新的有機染料：GZ116、GZ121、G124和GZ126。調整D-A-π-A骨架染料設計中的每個組成，有助於提升染敏電池的光物理，電化學和功率轉換效率。共軛片段的類型和染料間隔物長度的變化，在吸收光譜中是有關鍵作用。所有這些新染料都是設計成D-A-π-A骨架，含有三苯胺（TPA）作為供體、缺電子的2,3-雙（5-丁基噻吩-2-基）喹喔啉作為輔助受體、2-氰基丙烯酸作為電子受體和各種π-間隔基（2-（9,9-二丁基-9H-芴-2-基）噻吩、4-（3-己基噻吩-2-基）-7-苯基苯並[c] [1,2,5]噻二唑、4-苯基-7-（噻吩-2-基）苯並[c] [1,2,5]噻二唑和9,9-二丁基-9H-芴）。在這四種新染料中，GZ124比其他染料獲得了廣泛和紅移的吸收。在模擬AM 1.5G輻照（100 mW /cm2）下，GZ124的敏化元件獲得最高功率轉換效率為8.42％、短路光電流密度（JSC）為18.30 mA /cm2、開路光電壓（VOC）為0.659 V、填充因子（FF）為0.698。我們還進行了低光照下的光伏性能測量，GZ124敏化的元件獲得最佳性能在7000 lux下為16.28％、在4000 lux時為14.42％、在1000 lux時為9.68％、在650 lux下為9.67％。在類似條件下，標準N719染料在7000 lux時效率約為16.86％、在4000 lux時達到15.02％、在1000 lux時達到11.08％、在650 lux時達到10.33％。

Dye-sensitized solar cells (DSSCs) are one of the most promising organic photovoltaics. The theoretically optimized efficiency of tandem cell combined with both n- and p-type DSSCs was predicted to be 43%. In this matter the efficiency of n-type DSSCs surpasses 14% however the performance of p-type half cells still more than ten times lower. Therefore, the bottleneck for reaching the optimized performance is limited by the p-type half-cell, particularly the lacking of an appropriate semiconducting material as the photocathode and also an appropriate organic dye in both p-type and n-type sides.
In chapter 3, we report the surfactant-mediated synthesis of nickel oxide nanomaterial using a chemical co-precipitation method. The new material was fully characterized by XRD, SEM, XPS, EDS, and BET. The BET result indicates the nickel oxide nanoparticles synthesized with surfactant attain higher surface area than the conventional one. The percentage atomic composition of nickel and oxygen in two materials from the result of EDS showed the slight deminish in oxygen amount and relative increament in nickel is observed in the sample NiO/DTAB.The performance of newly synthesized material based device tested by using the commercialized p-type dye: C-343 and achieved best efficiency of 0.0418% which higher than 0.0253% the device performance obtained from NiO without DTAB. The dye loading of the NiO prepared by the surfactant-mediated synthesis higher by about 35% than the material prepared without DTAB.
In chapter 4, the new organic dyes with electron-deficient diphenylquinoxaline incorporated within the molecular structure were prepared for p-type dye-sensitized solar cells with the newly prepared NiO as the photocathode. The new organic dyes consist of carboxylic acid as the anchoring group, triphenylamine as the electron donor, 2,3-diphenylquinoxaline as the auxiliary acceptor moiety, 2-methylenemalononitrile as electron acceptor, connected with thiophene, 3,4-ethylenedioxythiophene, and 2,2'-bithiophene as the π-spacer. Sensitizers with mono-anchoring group (EH166, EH122, and EH174) performed better than their corresponding double-anchoring sensitizers (EH162, EH126, and EH170). Among these, dye EH174 exhibited the best conversion efficiency up to 0.207% with a short-circuit photocurrent density of 4.84 mAcm-2, an open-circuit photovoltage of 137 mV, and a fill factor of 0.312. The current results indicate that the combination of electron-deficient quinoxaline motif with suitable -linker in a D-A--A molecular structure is a promising design of p-type sensitizers for NiO-based p-DSSCs. We have studied also the tandem cell performance with n-type photoanode, the device with EH174 performed best with the efficiency of 2.05% and EH122 achieved 1.99 %.
In chapter 5, we report the applicability of gallium doped nickel oxide photocathode material for high performance p-type dye sensitized solar cells. The property and effect of gallium doping with different ratio of gallium by mass (1%, 5% and 10%) investigated through different characterization techniques. The higher concentrations of gallium ion improved the photo-voltage however, there was a notable drop in photocurrent with increasing gallium (III) amount. Charge extraction and fermi level analysis revealed that the increased in open circuit voltage with the mass of gallium is due to a positive shift in the energy of the valence band. The p-DSSC results indicated that 1% gallium doped nickel oxide nanomaterial showed about 23% enhancement in efficiency compared to the device from NiO-0%Ga. At higher concentration of gallium (5% and 10%) the carrier concentration-Ni3+ decreases as confirmed from XPS study. The incorporation of gallium ions with nickel oxide nanocrystals adjusts the carrier concentration and induces the change of the oxygen deficiency and chemisorbed oxygen of nickel oxide nanoparticles as confirmed from EDS result. Thus, the doping of gallium (III) into nickel oxide nanoparticles should be a promising material for designing and fabricating the high performance photocathodes for p-DSSC.
Chapter 6 assessed about aqueous dye-sensitized solar cells which emerged as promising devices recently, which combine low cost and environmental compatibility. In the present study, we investigate the influence of alkali salt concentration on the chemistry behind the iodide-triiodide based redox mediator, which presents a completely aqueous environment for tandem dye sensitized solar cell applications. We used squaraine-arylamine sensitizer (p-SQ2) as p-type dye and quinoxaline-TPA based n-type dye (MA169) to construct tandem dye sensitized solar cell. The best efficiency of tandem device obtained at H3 aqueous electrolyte combination as VOC 0.655V, Jsc 1.720 mAcm-2, FF 0.432 and of 0.487%.
In chapter 7, Herein, four new organic dyes: GZ116, GZ121, G124, and GZ126 designed and synthesized by using variable π-spacers. Tuning each component in the D-A-π-A framework dye design, contributes for photophysical, electrochemical and power conversion efficiency of the dye sensitized solar cells. The type of conjugated spacer units and variation of the spacer lengths of dyes play a critical role in absorption spectra. All these new dyes designed in D-A-π-A framework containing triphenylamine (TPA) as a donor, an electron deficient 2,3-bis(5-butylthiophen-2-yl) quinoxaline as the auxiliary acceptor, 2-cyanoacrylic acid as the electron acceptor and various -spacers (2-(9,9-dibutyl-9H-fluoren-2-yl)thiophene, 4-(3-hexylthiophen-2-yl)-7-phenylbenzo[c][1,2,5] thiadiazole, 4-phenyl-7-(thiophen-2yl)benzo[c][1,2,5]thiadiazole, and 9,9-dibutyl-9H-fluorene) respectively. Among these four new dyes, GZ124 achieved broad and red shifted absorption than other dyes. The highest power conversion efficiency of 8.42% with a short circuit photocurrent density (JSC) of 18.30 mA/cm2, an open-circuit photovoltage (VOC) of 0.659 V and a fill factor (FF) of 0.698 under simulated AM 1.5G irradiation (100 mW/cm2) obtained from the device sensitized from GZ124. We did also photovoltaic performance measurement at low light and the best performance about 16.28% at 7000 lux, 14.42% at 4000 lux, 9.68% at 1000 lux and 9.67% at 650 lux obtained from the device sensitized with GZ124. Under similar conditions, the standard N719 dye achieved the efficiencies about 16.86 % at 7000 lux, 15.02% at 4000 lux, 11.08% at 1000 lux and 10.33 % at 650 lux.

抽象.............................................................i
ABSTRACT....... ..............................................iv
AKNOWLADGMENTS ..............................................viii
LIST OF FIGURES ..............................................xvi
LIST OF TABLES ..............................................xxi
LIST OF SCHEMES ..............................................xxii
LIST OF ABBREVIATIONS .......................................xxiii
CHAPTER 1 ....................................................1
GENERAL INTRODUCTION .........................................1
1.1. Photovoltaics ........................................1
1.1.1. Dye-sensitized solar cells .........................3
1.1.2. Parameters in Dye Sensitized Solar Cells...............8
1.2. P-Type Semiconductor Oxides............ ..............10
1.2.1. Doping in Semiconductor Oxides. ....................13
1.3. Nanomaterials.. ......................................14
1.3.1. Strategies for Nanoparticles Synthesis .............15
1.3.2. Role of Surfactants in Nanomaterial Synthesis..........16
1.4. Chemistry of Nickel Oxide Nanoparticles ..............18
1.4.1. Synthesis Methods of Nickel Oxide......................19
1.5. Objectives of the Thesis.................................22
1.6. Overview of the Thesis...................................23
CHAPTER 2 .......................................................25
CHARACTERIZATION TECHNIQUES .....................................25
2.1. X-Ray Powder Diffraction...................................25
2.2. Scanning Electron Microscopy...............................26
2.3. Energy Dispersive X-Ray Spectroscopy.......................26
2.4. X-Ray Photoelectron Spectroscopy...........................27
2.5. Brunauer-Emmett-Teller (BET) Surface Area Analysis.........27
2.6. Photoelectron Spectroscopy: AC2 Model......................28
2.7. UV-vis Absorption Spectroscopy.............................28
2.8. Cyclic Voltammetry..........................................29
2.9. Solar Simulator.............................................30
2.10. Zahner Zennium Electrochemical Workstation.................30
CHAPTER 3........................................................31
SYNTHESIS AND CHARACTERIZATION OF SURFACTANT MEDIATED NICKEL OXIDE PHOTOCATHODE MATERIAL FOR P-TYPE DYE-SENSITIZED SOLAR CELLS..... 31
3.1. Introduction................................................31
3.2. Results and Discussion.....................................33
3.2.1. Synthesis of Nickel Oxide Photocathode Material...........33
3.2.2. Surfactant Assisted Nickel Oxide Nanoparticle Synthesis and Efficiency of P-DSSC.............................................36
3.2.3. P-DSSC Performance Study..................................43
3.3. Conclusions.................................................46
3.4. Experimental Section........................................46
3.4.1. Materials and Characterization Methods....................46
3.4.2. Solar Cell Device Fabrication and Measurements............47
CHAPTER 4 .......................................................48
NEW 2,3-DIPHENYLQUINOXALINE CONTAINING ORGANIC D-A--A DYES WITH NICKEL OXIDE PHOTOCATHODE PREPARED BY SURFACTANT-MEDIATED SYNTHESIS FOR P-TYPE AND TANDEM DYE-SENSITIZED SOLAR CELLS................48
4.1. Introduction...............................................48
4.2. Results and Discussion.....................................50
4.2.1. Photophysical Properties.................................50
4.2.2. Electrochemical Properties...............................52
4.2.3. Theoretical Calculations.................................54
4.2.4. Photovoltaic Performance.................................58
4.2.5. Tandem DSSC Performance Study............................62
4.2.6. Long-Term Stability Test.................................65
4.3. Conclusions................................................66
4.4. Experimental Section.......................................67
4.4.1. Materials and Characterization Methods.................. 67
4.4.2. Synthesis of Surfactant Assisted Nickel Oxide............68
4.4.3. Solar Cell Device Fabrication and Measurements...........68
CHAPTER 5.......................................................70
GALLIUM DOPED NICKEL OXIDE AS EFFICIENT PHOTOCATHODE MATERIAL FOR P-TYPE DYE SENSITIZED SOLAR CELLS.................................70
5.1. Introduction...............................................70
5.2. Results and Discussion.....................................71
5.2.1. Gallium Containing Nickel Oxide Nanomaterials
Characterizations........................................71
5.2.2. Photophysical Properties ................................77
5.2.3. Electrochemical Properties...............................78
5.2.4. Photovoltaic Performances................................80
5.2.5. Electrochemical Impedance Spectroscopy Study of Gallium Doped Nickel Oxide Based p-DSSC.......................................84
5.2.6. Injection efficiency analysis using time correlated single photon counting.................................................85
5.3. Conclusions................................................89
5.4. Experimental Section.......................................91
5.4.1. Synthesis of Gallium Containing Nickel Oxide Nanomaterials
........................................................91
5.4.2. Characterization of Materials............................91
5.4.3. Solar Cell Device Fabrication and Measurements...........92
CHAPTER 6.......................................................94
TANDEM DYE SENSITIZED SOLAR CELLS BASED ON AQUEOUS ELECTROLYTES.94
6.1. Introduction...............................................94
6.2. Results and Discussion.....................................96
6.2.1. Photophysical Properties of MA169 and p-SQ2..............96
6.2.2. Photovoltaic Performance Study of Aqueous Electrolyte Based Tandem Dye Sensitized Solar Cells...............................97
6.2.3. Influence of Salt Concentration on Aqueous Based Tandem Dye Sensitized Solar Cells Performance.............................99
6.2.4. Long-Term Stability Study..............................109
6.3. Conclusions..............................................110
6.4. Experimental Section.....................................111
6.4.1. Characterization of Materials..........................111
6.4.2. Solar Cell Device Fabrication and Measurements.........112
CHAPTER 7.....................................................113
THE INFLUENCE OF π-SPACERS ON THE PERFORMANCE OF NEW 2,3-BIS(5-BUTYLTHIOPHEN-2-YL) QUINOXALINE BASED SENSITIZERS FOR DYE SENSITIZED SOLAR CELLS ................................................113
7.1. Introduction.............................................113
7.2. Results and Discussion...................................115
7.2.1. Photophysical Properties...............................115
7.2.2. Electrochemical Properties.............................119
7.2.3. Photovoltaic Performances..............................122
7.2.4. Photovoltaic Performances under dim-light conditions...126
7.3. Conclusions..............................................128
7.4. Experimental Section.....................................128
7.4.1. Analytical Instruments and Measurements................128
7.4.2. Solar Cell Device Fabrication..........................129
CHAPTER 8.....................................................131
CONCLUSION AND OUTLOOKS.......................................131
8.1. Conclusions from our work................................131
8.2. Future Outlooks..........................................135
REFERENCES....................................................136

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