釕金屬光敏化劑的設計與合成及其在染料敏化太陽能電池之應用

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陳家原(Chia-Yuan Chen) 查詢紙本館藏

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論文名稱

釕金屬光敏化劑的設計與合成及其在染料敏化太陽能電池之應用
(Molecular-Engineering of Ruthenium Photosensitizers for Dye-Sensitized Solar Cells)

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★ 合成新穎輔助配位基於無硫氰酸釕金屬光敏劑在染料敏化太陽能電池上的應用	★ Design and Synthesis of Ruthenium Dyes for High Open-circuit Voltage Dye-sensitized Solar Cells

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摘要(中)

染料敏化太陽能電池(Dye-sensitized Solar Cells, DSCs)由於具有透光性、可繞曲性、色彩多樣性、良好的光電轉換效率及低製造成本等優點，是目前相當熱門的研究領域之一。在該種電池中，光電流的主要來源-光敏化劑(sensitizer)是影響電池光電轉換效能與元件穩定性的重要關鍵組成之一。本研究主要內容為設計並合成六個新的釕(Ruthenium)金屬錯合物光敏染料(photosensitizers): CYC-B5、CYC-B6S、CYC-B6L、CYC-B7、CYC-B11以及CYC-B13並探討其在染料敏化太陽能電池(Dye-Sensitized Solar Cells, DSCs)中的應用。所有的染料皆採用一鍋合成法（one-pot）合成，並利用NMR、IR、Mass光譜與元素分析確定其結構。這六個新染料皆展示了優異的吸光性質 (電子由中心金屬轉移至配位基之躍遷的莫爾吸收係數皆大於16100 M-1 cm-1)。初步的元件效能測試顯示，這些染料搭配揮發性電解質的電池元件在標準AM 1.5G的模擬太陽光照射下，光電轉換效率均可達到高於8.96 %。另外，在使用低揮發性電解質的電池元件部份，由CYC-B11或CYC-B13染料敏化的電池元件除了有高於8.3 %的光電轉換效能外，在連續光照與溫度為60度C的加速老化量測條件下，測試1000小時後元件穩定性大於93 %，亦達現今染料敏化太陽能電池之穩定性的最高水平。更重要的是，使用CYC-B11作為光電轉換中心、搭配高揮發性電解質之元件的光電轉換效率可高達11.5 %；此值是目前文獻報導之所有染料敏化太陽能電池的光電轉換效率中最高的。

摘要(英)

The dye-sensitized solar cell (DSC) is one of the most hot research topics in the photovoltaic technology, due to its colorfulness, transparence, flexibility, impressive conversion efficiency and low manufacture cost. The sensitizer, center for photon to electricity conversion, plays a vital role in the photovoltaic performance and long-term stability of the DSCs. In this study, six new ruthenium complexes, coded as CYC-B5, CYC-B6S, CYC-B6L, CYC-B7, CYC-B11, and CYC-B13 were designed and synthesized by using the one-pot synthetic procedure. After the structure was identified by NMR, IR, Mass spectroscopy and EA, the light absorption, electrochemical properties as well as the application of these new dyes in dye-sensitized solar cells (DSCs) were explored. It was found that all sensitizers have the molar absorption coefficient for the metal-to-ligand charge transfer transition higher than 16100 M-1 cm-1. The preliminary tests show that the cells based on these dyes with a volatile electrolyte have the conversion efficiency higher than 8.96 % under the illumination of AM 1.5G sunlight at 100 mW/cm2. The cells based on CYC-B11 or CYC-B13 in combination with a low-volatile electrolyte not only have a high efficiency (> 8.3 %) but also display the excellent stability (> 93 %) under prolonged light soaking at 60 oC, comparable with the state-of-the-art robust DSCs. Most importantly, under the illumination of AM 1.5G sunlight, the cell based on CYC-B11 in combination with a volatile electrolyte achieves a conversion efficiency of 11.5 %, the highest efficiency for DSCs reported in literature so far.

關鍵字(中)

★ 釕
★ 光敏化劑
★ 分子設計
★ 染料敏化太陽能電池

關鍵字(英)

★ Photosensitizer
★ Ruthenium
★ Dye-Sensitized Solar Cells (DSCs)
★ Molecular-Engineering

論文目次

Table of Contents
摘要……………….………………......…………...…...….....……...........i
Abstract…………………….………………..……………................….iii
Chapter I: Introduction………...............................................................1
I-1 Introduction of the Dye-sensitized Solar Cells (DSCs)………….1
I-2 The photovoltaic performance of solar cells: incident photon to current conversion efficiency (IPCE) and overall conversion efficiency (η)…………………………………..............................2
I-3 The state-of-the-art dye-sensitized solar cells (DSCs)……...........4
I-4 Development of ruthenium photosensitizers for DSCs (1)……..14
I-5 Development of ruthenium photosensitizers for DSCs (2): The family of heteroleptic ruthenium dyes incorporated thiophene or its derivatives…………………………………………………...21
Chapter II: The Strategy for Designing High Performance Ruthenium Sensitizers for DSCs………………………...26
II-1 Background and motivation……….…………………………...26
II-2 Strategies for molecular design………………………………...28
II-3 Embodiment of these strategies for molecular design…………31
Chapter III: Experimental Section…………………………………...35
III-1 Reagents………………………………………………………35
III-2 Physicochemical studies...........................................................35
III-3 Preparation of ligands………………………………………...36
III-3-1 Synthesis of the ligand-6S………………………...……36
III-3-2 Synthesis of the ligand-6L……………………………..37
III-3-3 Synthesis of the ligand-7……………………………….39
III-3-4 Synthesis of the ligand-11…………………………...…40
III-3-5 Synthesis of the ligand-13……………………………...43
III-4 Synthesis of ruthenium sensitizers……………………………45
III-4-1 Preparation of CYC-B5……………………………......45
III-4-2 Preparation of CYC-B6S …………………………...…45
III-4-3 Preparation of CYC-B6L………………………..…….46
III-4-4 Preparation of CYC-B7………………………………..47
III-4-5 Preparation of CYC-B11……………………………….47
III-4-6 Preparation of CYC-B13………………………………48
III-5 Semiempirical computation…………………………………...49
III-6 Dye desorption………………………………………………..50
III-7 Device fabrication and relative measurements (1)……………50
III-7-1 Device fabrication……………………………………...50
III-7-2 Photovoltaic characterization…………………………..52
III-7-3 Electrochemical impedance spectroscopy (EIS) measurement…………………………………………...53
III-7-4 Pulsed-laser-induced photovoltage transient measurement…………………………………………...53
III-8 Device fabrication and relative measurements (2)……………54
III-8-1 Device fabrication……………………………………...54
III-8-2 Photovoltaic characterization…………………………..56
III-8-3 Transient photoelectrical measurements……………….57
III-8-4 Electrochemical impedance spectroscopy (EIS) measurements…………………………………………..58
III-8-5 Stability test…………………………………………….58
Chapter IV: Results and Discussion………………………………….59
IV-1 CYC-B5………………………………………………………59
IV-1-1 Synthesis and characterization…………………………59
IV-1-2 Frontier orbitals and light absorption property………...62
IV-1-3 Energy level of the frontier orbitals……………………66
IV-1-4 Photovoltaic performance of CYC-B5, CYC-B1 and N3 sensitized cells…………………………………………67
IV-1-5 Electrochemical impedance spectra (EIS) of CYC-B5, CYC-B1 and N3 sensitized cells………………………70
IV-1-6 Photovoltaic performance of cell based on CYC-B5 and modified TiO2 electrode………………………………..71
IV-2 CYC-B6S and CYC-B6L…………………………………….74
IV-2-1 Synthesis and characterization…………………………74
IV-2-2 Light absorption property……………………………...76
IV-2-3 Energy level of the frontier orbitals……………………78
IV-2-4 Photovoltaic performance of cells based on CYC-B6S or CYC-B6L……………………………………………...79
IV-2-5 Pulsed-laser-induced photovoltage transient and in-situ photo-electrochemical measurements on the cell or TiO2 thin film sensitized by CYC-B6S………………..84
IV-3 CYC-B7……………………………………………………....88
IV-3-1 Synthesis and characterization…………………………88
IV-3-2 Frontier orbitals and light absorption property………...90
IV-3-3 Energy level of the frontier orbitals……………………93
IV-3-4 Photovoltaic performance of cells based on CYC-B7…94
IV-3-5 Performance improvement of cells based on CYC-B7..98
IV-3-6 The effect of the dye concentration on the photovoltaic performance of CYC-B7 sensitized cells…………….101
IV-4 CYC-B11……………………………………………………104
IV-4-1 Synthesis and characterization………………………..104
IV-4-2 Frontier orbitals and light absorption property……….106
IV-4-3 Energy level of the frontier orbitals…………………..109
IV-4-4 Photovoltaic performance of cells based on CYC-B11 in combination with a volatile electrolyte……………….110
IV-4-5 Photovoltaic performance of cells based on CYC-B11 combined with a low-volatile electrolyte……………..111
IV-4-6 Stability of cells based on CYC-B11 in combination with a low-volatile electrolyte……………………………..113
IV-4-7 Transient photovoltage decay and electrochemical impedance spectroscopy (EIS) measurements of fresh and aged devices based on CYC-B11…………………….115
IV-4-8 Photovoltaic performance of all-solid-state DSC based on CYC-B11……………………………………………..120
IV-5 CYC-B13……………………………………………………121
IV-5-1 Synthesis and characterization………………………..121
IV-5-2 Frontier orbitals and light absorption property……….123
IV-5-3 Energy level of the frontier orbitals…………………..125
IV-5-4 Photovoltaic performance of CYC-B13 sensitized cells…………………………………………………...126
IV-5-5 Stability of cells based on CYC-B13 in combination with a low-volatile electrolyte……………………………...130
IV-5-6 Transient photovoltage decay and electrochemical impedance spectroscopy (EIS) measurements of fresh and aged devices based on CYC-B13…………………….132
Chapter V: Conclusions.......................................................................135
References……………………………………...........................……...140
Appendix……………………………………………………………...151

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指導教授

吳春桂(Chun-Guey Wu)

審核日期

2009-7-15

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