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完整後設資料紀錄
DC 欄位 | 值 | 語言 |
---|---|---|
dc.contributor.advisor | 林金福(King-Fu Lin) | |
dc.contributor.author | Jen-Shyang Ni | en |
dc.contributor.author | 倪偵翔 | zh_TW |
dc.date.accessioned | 2021-06-16T16:20:27Z | - |
dc.date.available | 2013-02-16 | |
dc.date.copyright | 2013-02-16 | |
dc.date.issued | 2013 | |
dc.date.submitted | 2013-01-31 | |
dc.identifier.citation | 1 高鴻翔,'後石油時代的新興商機--太陽光電產業',財團法人資訊工業策進會,2009.03.31
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dc.identifier.uri | http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/63052 | - |
dc.description.abstract | 染料敏化太陽能電池(DSSC)在各類有機太陽能電池中,擁有最佳的光電轉換效率,其結構包含工作電極、染料、電解質,以及對電極等四大部分,主要染料扮演著分離電子-電洞的重要角色,也是整體元件最重要的一環。因此,在本研究中,將設計出「帶單邊脂肪族鏈」的RuC9與RuEO3,與「可交聯型」RuAS等兩種類型的釕金屬錯合物染料,探討染料吸附於二氧化鈦工作電極後,對整體元件所造成的效應。
在第一部分中,合成了帶有單邊長烷碳鏈段的釕金屬錯合物染料RuC9〔Ru(4,4’-dicarboxyl-2,2’-bipyridine)(4-nonyl-2,2’-bipyridine)(NCS)2〕,除了利用NMR、IR、UV-vis與EIS-MASS等光譜鑑定出染料含有兩種結構異構物之外,還透過UV-vis光譜分析比較RuC9與Z907染料吸附於二氧化鈦之吸附量,從吸附量的表現上發現,單邊取代RuC9染料減少了染料之間長烷鏈段的團聚,得到比雙邊取代的Z907染料較高的吸附量,加上RuC9染料本身擁有較高的MLCT波段吸光係數,不僅表現在元件IPCE上,呈現較卓越的單波長光電轉換效率,而且在DSSC元件短路電流(Jsc)表現上,亦高出雙邊取代的Z907元件約6%。最後,透過EIS分析得知,由於RuC9元件呈現較高的電子與電解質進行再結合機率,致使整體元件的光電轉換效率表現稍低於Z907元件。另外,為了改善二氧化鈦與電解質之間的介面阻抗,合成了含有單邊乙烷氧(EO)鏈段的RuEO3〔Ru(4,4’-dicarboxyl-2,2’-bipyridine)(5-tri(ethylene glycol)-2,2’-bipyridine) (NCS)2〕染料,除了結構上基本的鑑定之外,在經由ATR-FTIR觀察染料上EO鏈段螯合Li+離子的效應,藉此改善DSSC元件的開環電壓(Voc)與整體的光電轉換效率。 第二部分主要在合成帶有可螯合I3-錯離子之醯胺官能基,以及可進行交聯反應的苯乙烯官能基之釕金屬染料RuAS〔Ru(4,4’-dicarboxyl-2,2’-bipyridine) [4,4’-bis(styrenylaminocarbonyl)-2,2’-bipyridine](NCS)2〕,在NMR與ATR-FTIR之結構鑑定中發現,RuAS擁有螯合I3-錯離子之特性。因此,搭配含有不同I2濃度的液態電解質,在DSSC元件之表現上觀察到,RuAS透過醯胺官能基螯合I3-錯離子,減緩二氧化鈦的電子與電解質進行再結合的機率,進而在高濃度I2濃度環境下,元件依然保有一定的Voc。接著,利用帶有EO鏈段的trimethylol- propane ethoxylate triacrylate(TET,Mn ~912)與PO鏈段的glycerol propoxylate triacrylate(GPTA,Mw ~528)等功能性單體與RuAS染料進行共聚合改質,並於ATR-FTIR光譜中觀察到,改質後的RuAS-co-TET 與RuAS-co-GPTA工作電極表面皆能與Li+、I3-離子進行螯合之特性。透過UV-vis吸收光譜觀察到,相對於未交聯的RuAS工作電極(39%),RuAS-co-TET 與RuAS-co-GPTA分別保有65%與75%的染料數未被0.1N NaOH溶液脫附。在元件的表現上,亦將原本RuAS自身聚合的crosslinked RuAS元件光電轉換效率從5.9%分別提升到6.9%與7.7%。最後,透過電化學阻抗頻譜(EIS)、開環電壓衰退之瞬態,以及IMVS/IMPS等技術,來分析經由改質後的工作電極對於整體元件所造成的影響。 | zh_TW |
dc.description.abstract | Dye-sensitized solar cells (DSSC), composed of working electrode, dye, electrolyte and counter electrode, have the highest power conversion efficiency among the organic solar cells at present. Notably, the ruthenium complex dyes play the most important role for separating the electron-hole pair by exciting the dye with light. In this research, by modifying the bipyridine ligand of the ruthenium complex with single alkyl-chain or crosslinkable functional group, we investigated the relation between molecular structure and photovoltaic performance of DSSC.
In the first part of this research, Ru(4,4’-dicarboxyl-2,2’-bipyridine)(4-nonyl- 2,2’-bipyridine)(NCS)2 (denoted as RuC9) tethering single alkyl chain was synthesized and compared its adsorption behavior onto the mesoporous TiO2 film and photovoltaic properties with Z907, which has alike chemical structure but tethers two alkyl chains. The DSSC with RuC9 dye showed higher short-circuit photocurrent (Jsc) than that with Z907, attributing to its higher molar optical extinction coefficient (ε, 11,400 M-1cm-1), incident photon-to-current conversion efficiency (IPCE) and more adsorption amount onto the mesoporous TiO2 film. However, the DSSC with Z907 dye has higher open-circuit photovoltage (Voc) and power conversion efficiency (PCE), presumably because of the fact that more alkyl chains for Z907 form a molecular layer with higher hydrophobicity reduced the charge recombination at the interface between the dye-sensitized mesoporous TiO2 film and electrolyte, which has been verified by electrochemical impedance spectroscopy (EIS) and intensity modulated photocurrent and photovoltage spectroscopies (IMPS/IMVS). Additionally, Ru(4,4’-dicarboxyl-2,2’-bipyridine)(5-tri-(ethylene glycol)-2,2’-bipyridine)(NCS)2 (denoted as RuEO3) tethering single ethylene oxide (EO) chain was synthesized to improve the Voc of DSSC with its capability of coordinating Li+ ion, which was investigated by the ATR-FTIR. The DSSC with RuEO3 had higher Voc (0.7 V) than that with RuC9 (0.67 V), but lower Jsc (13.7 mAcm-2) and PCE (6.55%) due to its lower adsorption amount onto the mesoporous TiO2 film. In the second part, the crosslinkable ruthenium complex dye, Ru(4,4’-dicarboxyl- 2,2’-bipyridine)[4,4’-bis(styrylaminocarbonyl)-2,2’-bipyridine](NCS)2, denoted as RuAS, was synthesized and well characterized with 1H-NMR, 13C-NMR, HSQC, UV-vis, EA and ESI-MS spectra. Its capability of chelating triiodide anion with 4,4’-bis(styrylaminocarbonyl)-2,2’-bipyridine ligand (bsacbpy) was revealed by ATR-FTIR spectroscopy, which reduced the charge recombination by retarding the triiodide ions from closing to the mesoporous TiO2 film in DSSC. Therefore, the Voc of DSSC barely changed with the triiodide concentration in the electrolyte. Moreover, after polymerizing with trimethylolpropane ethoxylate triacrylate (TET) or glycerol propoxylate triacrylate (GPTA), the crosslinkable extent and ion-coordinating properties of RuAS were measured by ATR-FTIR and UV-vis spectroscopy after rinsed with 0.1 N NaOH solution. The PCE of DSSC with RuAS-co-TET and RuAS-co-GPTA was enhanced up to 6.9% and 7.7%, respectively than that with crosslinked RuAS (5.9%), attributed to the capability of coordinating Li+ ions by TET and GPTA. The enhanced photovoltaic performance was further examined by IPCE, EIS and open-circuit potential decay transient measurements. | en |
dc.description.provenance | Made available in DSpace on 2021-06-16T16:20:27Z (GMT). No. of bitstreams: 1 ntu-102-D95549011-1.pdf: 11383655 bytes, checksum: a8d9c81c0c115d0dabae9545f931c89a (MD5) Previous issue date: 2013 | en |
dc.description.tableofcontents | 摘要 I
目錄 V 圖目錄 XI 表目錄 XVII 第一章 緒論 1 1.1 前言 1 1.2 太陽能電池 1 1.2.1 第一代矽晶太陽能電池 4 1.2.2 第二代薄膜太陽能電池 5 1.2.3 第三代薄膜太陽能電池 5 1.2.4 染料敏化太陽能電池之競爭力 6 1.3 染料敏化太陽能電池 7 1.3.1 染料敏化太陽能電池工作原理 8 1.3.2 透明導電玻璃 11 1.3.3 工作電極 11 1.3.4 對電極 15 1.3.5 電解質 16 1.3.5.1 液態電解質 18 1.3.5.2 固態電解質 18 1.3.5.3 膠態電解質 19 1.3.5.4 離子液體 21 1.4 太陽能相關測定 25 1.4.1 太陽光模擬光源 25 1.4.2 太陽能電池光電轉換效率的計算 26 1.4.3 交流阻抗分析原理 28 1.4.4 強度調制光電壓與光電流譜(Intensity Modulated Photovoltage and Photocurrent Spectroscopy,IMVS/IMPS)量測 31 1.4.5 開環電壓衰退的瞬態與電量收集之量測 34 第二章 文獻回顧與研究目的 35 2.1 敏化型染料 35 2.2 釕金屬錯合物染料 37 2.3 實驗動機與架構 49 2.3.1 帶單邊脂肪族鏈型之釕金屬錯合物染料 50 2.3.2 帶可交聯官能基之釕金屬錯合物染料 50 第三章 實驗設備與方法 52 3.1 實驗儀器設備 52 3.2 合成方法 53 3.2.1 合成RuC9染料 53 3.2.2 合成RuEO3染料 56 3.2.3 合成RuAS染料 59 3.3 二氧化鈦鍍液的製備 61 3.4 各種量測樣品製備方法 61 3.4.1 測量UV-vis吸收光譜儀之樣品製備 61 3.4.1.1 染料於溶液中的吸收光譜之樣品製備 61 3.4.1.2 染料吸附於二氧化鈦上的吸收光譜之樣品製備 61 3.4.2 交聯之樣品製備與量測 62 3.5 薄膜電極之製備 62 3.5.1 導電玻璃之清洗 62 3.5.1.1 FTO導電玻璃之清洗 62 3.5.1.2 ITO導電玻璃之清洗 63 3.5.2 工作電極之製備 63 3.5.3 白金對電極之製備 64 3.6 液態電解質之製備 64 3.7 太陽能電池之組裝 65 3.8 太陽能電池光電化學測試 65 3.8.1 光電流-電壓特徵曲線 65 3.8.2 交流阻抗分析 66 3.8.3 入射光子電流轉換效率(IPCE) 66 3.8.4 強度調制光電壓與光電流譜(Intensity Modulated Photovoltage and Photocurrent Spectroscopy,IMVS/IMPS)之量測 67 3.8.5 開環電壓衰退的瞬態與電量收集之量測 67 第四章 帶單邊脂肪族鏈之釕金屬染料 68 4.1 引言 68 4.2 RuC9染料 68 4.2.1 RuC9染料結構上之鑑定 68 4.2.1.1 RuC9染料之NMR鑑定 69 4.2.1.2 RuC9和Z907染料之UV-vis吸收光譜鑑定 69 4.2.1.3 RuC9與Z907染料之FTIR光譜鑑定 72 4.2.2 RuC9與Z907染料之吸附量 74 4.2.3 RuC9與Z907染料之太陽能電池元件 75 4.2.4 RuC9與Z907染料之EIS分析 77 4-3 RuEO3染料 78 4.3.1 RuEO3染料結構上之鑑定 79 4.3.1.1 RuEO3染料之NMR鑑定 79 4.3.1.2 RuEO3染料之UV-vis吸收光譜鑑定 81 4.3.1.3 RuEO3染料之FTIR光譜鑑定,與其所表現的Li+離子效應 82 4.3.2 RuEO3染料之吸附量 83 4.3.3 RuEO3染料之DSSC元件探討 84 第五章 可交聯型釕金屬染料RuAS 87 5.1 引言 87 5.2 RuAS染料 87 5.2.1 RuAS染料之鑑定 88 5.2.2 RuAS染料之NMR鑑定 88 5.2.2.1 RuAS染料於D2O環境之NMR鑑定 90 5.2.2.2 功能性bsacbpy配位基於I-/I3-離子環境之NMR鑑定 91 5.2.3 RuAS染料與I-/I3-離子作用之ATR-FTIR光譜鑑定 92 5.2.4 RuAS染料之UV-vis吸收光譜鑑定 93 5.2.5 RuAS染料之FTIR光譜鑑定 94 5.2.6 RuAS染料之交聯性質鑑定 95 5.2.7 RuAS染料之太陽能電池元件 96 5.2.8 RuAS染料之EIS分析 99 5.2.9 RuAS染料之開環電壓衰退瞬態分析 101 5.5 RuAS染料藉由AIBN進行聚合反應 102 5.5.1 RuAS染料與其聚合後之元件I-V測量 102 5.5.2 RuAS染料與其聚合後之元件EIS分析 103 5.5.3 RuAS染料與其聚合後之元件IMVS/IMPS分析 105 第六章 可交聯型釕金屬染料RuAS與功能性單體GPTA與TET 107 6.1 前言 107 6.1.1 RuAS-co-TET、RuAS-co-GPTA工作電極表面與I-/I3-離子對作用之ATR-FTIR量測 109 6.2 RuAS染料交聯功能性單體TET之太陽能電池元件 110 6.2.1 RuAS-co-TET之I-V元件測量 110 6.2.2 RuAS-co-TET之元件EIS分析 112 6.2.3 RuAS-co-TET在不同LiI電解質濃度之元件I-V測量 114 6.2.4 RuAS-co-TET在不同LiI電解質濃度之元件EIS分析 116 6.2.5 RuAS-co-TET在不同LiI電解質濃度之元件開環電壓衰退瞬態分析 118 6.2.6 RuAS-co-TET在不同I2電解質濃度之元件I-V測量 119 6.2.7 RuAS-co-TET在不同I2電解質濃度之元件EIS分析 121 6.2.8 RuAS-co-TET在不同I2電解質濃度之元件開環電壓衰退瞬態分析 122 6.3 RuAS染料交聯功能性單體GPTA之太陽能電池元件 123 6.3.1 RuAS-co-GPTA之元件I-V測量 123 6.3.2 RuAS-co-GPTA之元件EIS分析 125 6.3.3 RuAS-co-GPTA在不同LiI電解質濃度之元件I-V測量 127 6.3.4 RuAS-co-GPTA在不同LiI電解質濃度之元件EIS分析 129 6.3.5 RuAS-co-GPTA在不同LiI電解質濃度之元件開環電壓衰退瞬態分析 131 6.3.6 RuAS-co-GPTA在不同I2電解質濃度之元件I-V測量 132 6.3.7 RuAS-co-GPTA在不同I2電解質濃度之元件EIS分析 133 6.3.8 RuAS-co-GPTA在不同I2電解質濃度之元件開環電壓衰退瞬態分析 135 6.4 RuAS染料交聯功能性單體TET與GPTA之綜合分析 136 6.4.1 不同濃度單體濃度改質所呈現之趨勢 136 6.4.2 不同LiI電解質濃度之影響趨勢 137 6.4.3 不同I2電解質濃度之影響趨勢 139 6.5 RuAS染料交聯功能性單體TET與GPTA之IPCE分析 141 6.6 RuAS染料交聯功能性單體TET與GPTA之開環電壓衰退分析 142 6.7 RuAS染料交聯功能性單體TET與GPTA之電量收集分析 143 6.8 RuAS染料交聯功能性單體TET與GPTA之IMVS/IMPS分析 143 第七章 結論 146 7.1 帶單邊鏈段之釕金屬錯合物染料 146 7.2 可交聯型之釕金屬錯合物染料RuAS 147 7.3 可交聯型之釕金屬錯合物染料RuAS與單體TET、GPTA 148 7.4未來研究之展望 150 參考文獻 151 附錄A RuC9與Z907微結構 163 附錄B RuEO3染料元件特性之探討 164 附錄C List of Publilcation 166 | |
dc.language.iso | zh-TW | |
dc.title | 帶單邊脂肪族鏈與可交聯型釕金屬錯合物在染料敏化太陽能電池之合成與應用 | zh_TW |
dc.title | Synthesis and Applications of Tethering Single Alkyl-chain type and Crosslinkable type Ruthenium Complex Dyes on Dye-sensitized Solar Cells | en |
dc.type | Thesis | |
dc.date.schoolyear | 101-1 | |
dc.description.degree | 博士 | |
dc.contributor.oralexamcommittee | 何國川(Kuo-Chuan Ho),王立義(Lee-Yih Wang),林宏洲(Hong-Cheu Lin),鄭弘隆(Horng-Long Cheng) | |
dc.subject.keyword | 染料敏化太陽能電池,單邊取代,釕金屬染料,交聯,螯合,鋰離子,三碘錯離子, | zh_TW |
dc.subject.keyword | dye-sensitized soalr cells,crosslinkable,ruthenium,lithium ion,triiodide,coordinating,chelating, | en |
dc.relation.page | 166 | |
dc.rights.note | 有償授權 | |
dc.date.accepted | 2013-01-31 | |
dc.contributor.author-college | 工學院 | zh_TW |
dc.contributor.author-dept | 高分子科學與工程學研究所 | zh_TW |
顯示於系所單位: | 高分子科學與工程學研究所 |
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