優化含氯元素之多聯吡啶釕錯合物敏化太陽能電池與元件特性探討

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邱其楓(Chi-Feng Chiu) 查詢紙本館藏

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化學學系

論文名稱

優化含氯元素之多聯吡啶釕錯合物敏化太陽能電池與元件特性探討

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摘要(中)

染料敏化太陽能電池(Dye-sensitized Solar Cells，DSCs)具有可透光性、多彩性及低製造成本，可應用於建築物玻璃帷幕、天窗等，它們可透過吸附在多孔隙二氧化鈦(TiO2)薄膜表面的光敏化劑，搭配液態電解質將光能轉換為電能，且可透過調整敏化劑分子結構、氧化還原介質和元件結構提高元件的光電轉換效率(Power Conversion Efficiency，PCE)。為了使元件能展現最佳性能，本研究針對本實驗室所開發的新型含氯元素之多聯吡啶釕錯合物染料(CYC-42Cl與CYC-43Cl)進行元件優化，除了透過使用鵝去氧膽酸(Chenodeoxycholic Acid，CDCA)作為共吸附劑，也嘗試導入丁苯羥酸(2-(4-Butoxyphenyl)-N-hydroxyacetamide，BPHA)，以期望共吸附劑能減少染料在二氧化鈦薄膜上的聚集程度，進而增加元件的短路電流密度，若能一併鈍化裸露的二氧化鈦表面，則可抑制電荷再結合，以增加元件的開路電壓與填充因子。經優化後，在標準測試條件下(AM 1.5G，25 oC)，未添加共吸附劑的CYC-42Cl與CYC-43Cl染料敏化元件效率分別為6.67%和8.06%，添加CDCA的敏化元件則為7.49%及8.15%，而添加BPHA的敏化元件具有最高的光電轉換效率達7.99%與8.52%。透過比較CYC-42Cl及CYC-43Cl染料敏化元件發現，於多聯吡啶釕錯合物固著配位基上使用不同推(叔丁基-CYC-42Cl)、拉(氯原子-CYC-43Cl)電子基，會造成元件性能差異，其歸因於CYC-43Cl染料具有更強的抗聚集能力，且ATR-FTIR光譜數據顯示CYC-43Cl染料可於TiO2表面形成更強的架橋式鍵結。另外，IMPS、IMVS及CE測量結果表明，CYC-43Cl染料會使TiO2導電帶位能降低，此有助於提高電子注入驅動力，從而增加元件的短路電流密度，且對比而言，CYC-43Cl (BPHA)敏化元件具有更長的電荷再結合生命期與最高的電荷收集效率，因此本研究展現於固著配位基導入氯原子是設計高效能多聯吡啶釕錯合物的新方向。

摘要(英)

Dye-sensitized solar cells (DSCs) offer transparency, color variety, and low manufacturing costs, making them suitable for various building-integrated applications. This study optimizes devices using new chlorine-containing polypyridine ruthenium complex dyes (CYC-42Cl and CYC-43Cl), focusing on the role of co-adsorbents chenodeoxycholic acid (CDCA) and 2-(4-butoxyphenyl)-N-hydroxyacetamide (BPHA). These co-adsorbents aim to reduce dye aggregation, increase short-circuit current density (Jsc), and suppress charge recombination while improving open-circuit voltage (Voc) and fill factor (FF). Under standard testing conditions (AM 1.5G, 25 oC), devices without co-adsorbents showed efficiencies of 6.67% (CYC-42Cl) and 8.06% (CYC-43Cl). CDCA addition improved these to 7.49% and 8.15%, while BPHA yielded the highest efficiencies of 7.99% and 8.52%. The study revealed performance differences are due to the electron-donating group (tert-butyl: CYC-42Cl) and the electron-withdrawing group (chloro: CYC-43Cl) on the ruthenium complexes. This is attributed to the stronger anti-aggregation ability of CYC-43Cl. ATR-FTIR spectral data also shows that CYC-43Cl forms stronger bidentate bridging bonds on the TiO2 surface. Moreover, IMPS, IMVS, and CE measurements indicate that devices sensitized with CYC-43Cl exhibit a lower TiO2 conduction band potential. This characteristic is associated with an increased driving force for electron injection, which may contribute to these devices′ higher short-circuit current density. In contrast, the CYC-43Cl (BPHA) sensitized device has a longer charge recombination lifetime and the highest charge collection efficiency. Therefore, this study demonstrates that introducing chlorine atoms to the anchoring ligand is a new direction for designing high-performance polypyridine ruthenium complexes.

關鍵字(中)

★ 染料敏化太陽能電池
★ 多聯吡啶釕錯合物

關鍵字(英)

論文目次

中文摘要 I
Abstract II
目錄 IV
圖目錄 VIII
表目錄 XIV
第一章、緒論 1
1.1 前言 1
1.2 太陽光譜的介紹 2
1.3 太陽能電池光伏參數的介紹 3
1.4 染料敏化太陽能電池的工作原理與元件架構 6
1.5影響染料敏化太陽能電池效率的因素 8
1.5-1光電極 9
1.5-2染料分子的結構設計 13
1.5-3電解質的類型及作用 23
1.5-4電解質組成所使用的添加劑 25
1.6改善染料在TiO2上的聚集程度 31
1.6-1導入共吸附劑鵝去氧膽酸 31
1.6-2導入預吸附劑丁苯羥酸 34
1.7研究動機 38
第二章、實驗方法 39
2.1實驗藥品、材料與儀器 39
2.1-1實驗藥品 39
2.1-2實驗材料 40
2.1-3實驗儀器 41
2.2合成與製備二氧化鈦球珠漿料 42
2.2-1二氧化鈦球珠漿料的合成步驟 42
2.2-2製備塗布於網印機之二氧化鈦奈米球珠漿料 43
2.3 配製染料溶液 44
2.4 配製最佳組成的電解質 44
2.5 製備TiO2光電極的流程 45
2.6 製備Pt對電極 47
2.7 染料敏化太陽能電池的元件組裝與光伏參數量測 47
2.8 量測儀器分析與所需樣品製備 48
2.8-1太陽光模擬器與光電轉換效率量測 48
2.8-2太陽能電池外部量子效率量測系統 49
2.8-3紫外光/可見光/近紅外光吸收光譜 51
2.8-4交流阻抗分析儀 53
2.8-5光強度調制光電流/光電壓分析儀；電荷萃取 55
2.8-6衰減全反射式傅立葉轉換紅外光譜 57
第三章、結果與討論 58
3.1 TiO2自製層漿料應用於Black dye染料敏化元件的優化與分析 58
3.2 CYC-42Cl染料敏化元件的共吸附劑條件優化 61
3.2-1搭配不同濃度的共吸附劑CDCA 61
3.2-2搭配不同濃度的共吸附劑BPHA 62
3.3 CYC-43Cl染料敏化元件的共吸附劑條件優化 65
3.3-1搭配不同濃度的共吸附劑CDCA 65
3.3-2搭配不同濃度的共吸附劑BPHA 66
3.4 CYC-42Cl、CYC-43Cl染料敏化元件的條件優化 69
3.4-1使用不同染料濃度對CYC-42Cl、CYC-43Cl敏化元件的影響 69
3.4-2調整TiO2透明層厚度對CYC-42Cl、CYC-43Cl染料敏化元件的影響 73
3.4-3改變浸泡時間對CYC-42Cl、CYC-43Cl染料敏化元件的影響 76
3.4-4調整TiO2散射層厚度對CYC-42Cl、CYC-43Cl染料敏化元件的影響 79
3.5電解質組成變化影響CYC-43Cl染料敏化元件的光伏參數 82
3.5-1添加不同濃度BMII的電解質對元件光伏參數的影響 82
3.5-2添加不同濃度LiI的電解質對元件光伏參數的影響 85
3.5-3添加不同濃度I2的電解質對元件光伏參數的影響 87
3.5-4添加不同濃度GuSCN的電解質對元件光伏參數的影響 90
3.6採用最佳優化條件所組裝元件之光伏參數 92
3.6-1使用最佳化條件的CYC-42Cl與CYC-43Cl敏化元件光伏參數 92

3.6-2使用最佳化條件下CYC-42Cl、CYC-43Cl及Black dye敏化元件的光伏參數再現性測試：有無添加BPHA 96
3.7染料的光物理及元件電荷轉移性質探討 99
3.7-1 CYC-42Cl、CYC-43Cl及Black dye染料的UV/Vis吸收光譜圖 99
3.7-2 CYC-42Cl、CYC-43Cl及Black dye染料的ATR-FTIR光譜圖 106
3.7-3電子在TiO2薄膜上的電荷再結合生命期影響因素 108
3.7-4電子在TiO2薄膜上的有效擴散係數 110
3.7-5電子在TiO2薄膜上的電子擴散長度及電子收集率 112
3.7-6影響填充因子的因素 114
3.8元件長時間穩定性測試結果 115
第四章、結論 116
參考文獻 119
附錄 130
附圖1不同光強度下有無導入BPHA的CYC-42Cl與CYC-43Cl染料敏化元件的IMVS-Nyquist阻抗電路圖，及對應Bode頻率圖譜 130
附圖2不同光強度下有無導入BPHA的CYC-42Cl與CYC-43Cl染料敏化元件的IMPS-Nyquist阻抗電路圖，及對應Bode頻率圖譜 131
附1.1 CYC-42Cl、CYC-43Cl染料敏化元件的優化條件 132
附1.1-1有無添加NBB的電解質對CYC-43Cl染料敏化元件光伏參數的影響 133
附1.1-2搭配不同溶劑對CYC-43Cl染料敏化元件光伏參數的影響 134
附1.1-3 TiCl4後處理次數或H2PtCl6多寡對CYC-43Cl染料敏化元件的影響 136
附1.1-4使用不同批次染料對CYC-42Cl、CYC-43Cl染料敏化元件光伏參數的影響 138
附2.1 Ligand-65與CYC-65染料敏化元件的優化條件 141
附2.1-1 Ligand-65染料敏化元件的染料濃度與共吸附劑條件優化 141
附2.1-2 CYC-65染料敏化元件使用不同溶劑並搭配不同電解質組成的條件優化 145
附2.1-3 CYC-65染料敏化元件的TiO2透明層層數與共吸附劑條件優化 147
附2.1-4 Ligand-65與CYC-65染料敏化元件的吸附溫度條件優化 150

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指導教授

陳家原(Chia-Yuan Chen)

審核日期

2024-8-19

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