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完整後設資料紀錄
DC 欄位 | 值 | 語言 |
---|---|---|
dc.contributor.advisor | 何國川 | |
dc.contributor.author | Yeh-Yung Lin | en |
dc.contributor.author | 林燁雍 | zh_TW |
dc.date.accessioned | 2021-06-07T23:47:31Z | - |
dc.date.copyright | 2014-07-22 | |
dc.date.issued | 2014 | |
dc.date.submitted | 2014-05-13 | |
dc.identifier.uri | http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/16834 | - |
dc.description.abstract | 本論文主要研究方向是設計與發展不同類型有機染料,進而應用於染料敏化太陽能電池。同時,我們進一步使用共吸附、染料共敏化以及改變光電極材料的方式去提升與改善光電轉換效率。並且利用各種物理分析方法去解釋實驗的結果,以了解染料分子結構與元件效率之關聯性。
以二氫菲上9,10 位置為主的小分子染料建構染料敏化太陽能電池,其光電轉換效率介於5.21%至5.95%。我們選擇當中效率最高者(BP-2)與可吸收紅外光之染料方酸染料(SQ2),進行不同混摻比例(體積比)之共敏化太陽能電池。其光電轉換效率隨著BP-2混摻比例增加而上升﹔其中,當BP-2與SQ2體積比為8比2時,效率可以提升至8.14%。最後,我們利用歐傑電子顯微鏡探測所述染料分佈於二氧化鈦薄膜之情形。 接下來,我們合成含缺電子材料苯並噻二唑(BT)之染料。此系列染料設計,是將苯並噻二唑直接與2 -氰基丙烯酸做連結,並且搭配使用氧化鋅光電極材料,以期氧化鋅光電極的電子傳遞可加速電荷的分離。我們也開發新穎的氧化鋅奈米粒子當作散射層之應用。藉由搭配此新穎的氧化鋅材料,其光電轉換效率可更進一步提升。 我們合成了一系列以蔥之2,6位置為主體之光敏化染料分子,此係列染料分子皆具有高莫耳消光係數及寬廣的吸收波長(~600 nm),其薄膜吸收光譜更可延伸至700 nm。此系列染料於太陽能電池表現中皆達良好的光電轉換效率(4.69−7.52%)。我們進一步使用去氧鵝膽酸及SQ2染料與Ant3分子進行共敏化染料太陽能電池,使光電轉換效率可分別提升至9.11%與8.08%。於弱光下,光電轉換效率更可突破10%。 我們以2,3,5-取代位置的噻吩建構含有兩個錨基團的染料分子,D-π-(A)2。此系列染料表現出高莫耳消光係數和良好的光電轉換效率。進一步使用CDCA進行共吸附,此系列染料之光電轉換效率能提升1.03到2倍。其中,最佳效率表現(8.28%)可達到標準元件之95%。 | zh_TW |
dc.description.abstract | New organic dyes were developed and used as the sensitizers for the dye-sensitized solar cells (DSSCs). Different approaches (co-sensitized, co-adsorbent, zinc oxide photoanode) were used to improve the cell performance. Various physical measurements, including UV–vis absorption spectroscopy, electrochemical impedance spectroscopy (EIS), and incident photo–to–current conversion efficiency (IPCE) spectra, charge extraction method (CEM) and intensity-modulated photovoltage spectroscopy (IMVS) were used to obtain important parameters relevant to the cell performance for correlation between the molecular structure and the cell performance.
Bipolar organic dyes containing a 9,10-dihydrophenanthrene entity in the conjugated bridge were synthesized as the sensitizers for DSSCs. The DSSC exhibits good cell efficiencies ranging from 5.21% to 5.95% under 1 sun condition. When combining the best performed dye (BP-2) with a squaraine dye (SQ2), the efficiency increment of the co-sensitized DSSCs is in compliance with the increased ratio of BP-2/SQ2. The co-sensitized DSSC in which the ratio of BP-2 and SQ2 was 8:2 (v/v) exhibited a high efficiency of 8.14%. The TiO2 film adsorbed with co-sensitizers was subjected to Auger electron spectroscopy (AES) for probing the dye distribution across the TiO2 film depth. We synthesized benzothiadiazole (BT)-containing sensitizers with BT entity directly connected to 2-cyanoacrylic acid for DSSCs using ZnO as the photoanode aiming at better charge separation because of better electron transport. The cells performed better than those using TiO2 as the photoanode. The cell efficiency can be further improved when a newly developed brush hierarchical ZnO nanoplates were used as the light back scattering layer (SL) of the cell. Dyes consisting of 2,6-conjugated anthracene segment as the conjugated spacer, 9,10-bishexyloxyanthracen-phenylamino as the electron donor, and cyanoacrylic acid as the acceptor and anchor as well were synthesized. DSSCs using these sensitizers exhibited efficiencies 4.69−7.52% under AM 1.5 illumination, and an impressively high efficiency (9.11%) surpassing the N719-based standard cell has also been achieved with the use of CDCA co-adsorbent. In order to enhance electron injection and dark current suppression, the dyes with two anchoring groups, D-π-(A)2, were synthesized from a 2,3,5-substituted thiophene motif. These dyes exhibit high molar extinction coefficient and good power conversion efficiency of the cells. With addition of co-adsorbent, CDCA, the device performance of all the DA-based DSSCs were improved by 1.03 to 2-fold, with the best efficiency reaching 95% of the N719-based standard cell (8.28%). | en |
dc.description.provenance | Made available in DSpace on 2021-06-07T23:47:31Z (GMT). No. of bitstreams: 1 ntu-103-D99524010-1.pdf: 38276370 bytes, checksum: 7dc4f7826c420d5d3b687d431e70f212 (MD5) Previous issue date: 2014 | en |
dc.description.tableofcontents | 中文摘要 I
Abstract III Table of contents V List of schemes IX List of tables X List of figures XII Nomenclatures XVIII Chapter 1 Introduction 1 1.1. Dye-Sensitized Solar Cells (DSSCs) 2 1.1.1. Basic working principles of DSSCs 2 1.1.2. Photovoltaic parameters of DSSCs 5 1.2. Construction of DSSCs 7 1.2.1. The mesoporous photoanode 7 1.2.2. Sensitizers 9 1.2.2.1. Spacer containing fluorine substituents 11 1.2.2.2. Spacer containing electron-deficient moieties 13 1.2.2.3. Near-Infrared organic sensitizers 16 1.2.2.4. Co-sensitization (panchromatic engineering) 19 1.2.3. Electrolyte 24 1.2.4. Counter electrodes (CEs) 27 1.3. Motivation 27 Chapter 2 Experimental 29 2.1. Materials 29 2.2. Instruments and methods 29 2.2.1. General information 29 2.2.2. Characterization of DSSCs 30 2.2.3. Quantum chemistry computation 31 2.3. Fabrication of DSSCs 32 2.4. Synthesis of Sensitizers 34 2.4.1. Synthesis of BP Sensitizers 34 2.4.2. Synthesis of Ant Sensitizers 40 2.4.3. Synthesis of RL Sensitizers 47 2.4.4. Synthesis of DA Sensitizers 50 Chapter 3 Dihydrophenanthrene-Based Metal-Free Dyes for Highly Efficient Co-sensitized Solar Cells 58 3.1. Introduction 58 3.2. Experimental 60 3.2.1. General Information 60 3.2.2. Assembly and characterization of DSSCs 60 3.2.3. Auger electron spectroscopy (AES) analysi 61 3.3. Results and Discussion 62 3.3.1. Synthesis of the Materials 62 3.3.2. Optical properties 64 3.3.3.Electrochemical properties 66 3.3.4. Theoretical Approach 68 3.3.5. Photovoltaic devices 69 3.3.6. Co-sensitized and Co-adsorbed DSSCs 70 3.3.7. Auger electron spectroscopy (AES) analysis 73 3.4. Conclusions 74 Chapter 4 2,6-Conjugated Anthracene Sensitizers for High-Performance Dye-sensitized Solar Cells 75 4.1. Introduction 75 4.2. Experimental 77 4.2.1. General Information 77 4.2.2. Assembly and characterization of DSSCs 77 4.3. Results and Discussion 78 4.3.1. Synthesis of the Materials 79 4.3.2. Optical properties 81 4.3.3. Electrochemical properties 83 4.3.4. Theoretical Approach 85 4.3.5. Photovoltaic devices 89 4.3.6. Co-sensitized and Co-adsorbed DSSCs 78 4.4. Conclusions 93 Chapter 5 Benzothiadiazole-Containing Donor-Acceptor-Acceptor Type Organic Sensitizers for Solar Cells with ZnO Photoanodes 94 5.1. Introduction 94 5.2. Experimental 95 5.2.1. General Information 96 5.2.2. Assembly and characterization of DSSCs 96 5.2.3. ZnO nanoparticles synthesis 96 5.2.4. Synthesis of hierarchical ZnO nanostructures 97 5.3. Results and Discussion 97 5.3.1. Synthesis of the Materials 97 5.3.2. Optical properties 99 5.3.3. Electrochemical properties 101 5.3.4. Theoretical Approach 103 5.3.5. Photovoltaic devices 105 5.3.6. Characterization of hierarchical ZnO 108 5.3.7. Photovoltaic devices with ZnO scattering layer (SL) 109 5.4. Conclusions 111 Chapter 6 Y-shaped Meal-Free D-π-(A)2 Sensitizers for High-Performance Dye-sensitized Solar Cells 112 6.1. Introduction 112 6.2. Experimental 114 6.2.1. General Information 114 6.2.2. Assembly and characterization of DSSCs 114 6.3. Results and Discussion 115 6.3.1. Synthesis of the Materials 115 6.3.2. Optical properties 117 6.3.3. Electrochemical properties 119 6.3.4. Theoretical Approach 121 6.3.5. Photovoltaic devices 123 6.3.6. CEM and IMVS characterization 127 6.3.7. Co-adsorbed DSSCs 129 6.4. Conclusions 131 Chapter 7 Suggestions and Prospects 132 References 134 Appendix A: High-Performance Dye-sensitized Solar Cells Based on Phenothiazinedioxide-conjugated Sensitizers and Dual-TEMPO/Iodide Redox Mediator 159 A.1. Introduction 159 A.2. Experimental 161 A.2.1. General Information 161 A.2.2. Assembly and characterization of DSSCs 161 A.2.3. Synthesis 162 A.3. Results and Discussion 169 A.3.1. Synthesis of the Materials 169 A.3.2. Characterizations of IL-I electrolyte 170 A.3.3. Optical properties 174 A.3.4. Electrochemical properties 176 A.3.5. Theoretical Approach 178 A.3.6. Photovoltaic devices 183 A.3.7. CEM and IMVS characterization 186 A.3.8. Co-adsorbed DSSCs 187 A.3.9. DSSCs using the IL-I electrolyte 189 A.4. Conclusions 190 Appendix B: Supporting information 191 Appendix C: NMR spectra 204 Appendix D: Curriculum vitae 267 | |
dc.language.iso | en | |
dc.title | 有機染料分子設計與高效能染料敏化太陽能電池 | zh_TW |
dc.title | Metal-free Sensitizers Approach for High Performance Dye-sensitized Solar Cells | en |
dc.type | Thesis | |
dc.date.schoolyear | 102-2 | |
dc.description.degree | 博士 | |
dc.contributor.coadvisor | 林建村 | |
dc.contributor.oralexamcommittee | 戴子安,廖英志,衛子健,林家裕 | |
dc.subject.keyword | 染料敏化太陽能電池,共吸附,共敏化,有機染料,雙錨之染料,去氧鵝膽酸,氧化鋅電極, | zh_TW |
dc.subject.keyword | Co-adsorbent,Co-sensitized,Dye-sensitized solar cells,Dyes with dianchors,Organic sensitizers,Squaraine,Zinc oxide photoanode, | en |
dc.relation.page | 270 | |
dc.rights.note | 未授權 | |
dc.date.accepted | 2014-05-14 | |
dc.contributor.author-college | 工學院 | zh_TW |
dc.contributor.author-dept | 化學工程學研究所 | zh_TW |
顯示於系所單位: | 化學工程學系 |
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