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研究生:羅文甫
研究生(外文):Wen-Fu Lo
論文名稱:以交聯劑及陽離子表面改質交聯型釕金屬染料強化固態染料敏化太陽能電池性能之研究
論文名稱(外文):Interface Engineering of Crosslinkable Ruthenium Complex with Its Ligand Crosslinker and Cations to Enhance the Performance of Solid-State Dye Sensitized Solar Cells
指導教授:林金福林金福引用關係
口試委員:何國川邱文英
口試日期:2015-07-14
學位類別:碩士
校院名稱:國立臺灣大學
系所名稱:材料科學與工程學研究所
學門:工程學門
學類:材料工程學類
論文種類:學術論文
論文出版年:2015
畢業學年度:103
語文別:中文
論文頁數:134
中文關鍵詞:染料敏化太陽能電池可交聯型釕金屬染料離子吸附
外文關鍵詞:dye sensitized solar cellcrosslinkable ruthenium complexion absorption
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本研究利用合成出帶有苯乙烯基官能基的可交聯型釕金屬染料Ru (4,4’-dicarboxylic acid) (4,4''-bis((4-vinylbenzyloxy)methyl)- 2,2''-bipyridine-(NCS)2 (RuS) 經鑑定後應用至固態染料敏化太陽能電池。與N3染料相比開路電壓(Voc)和短路電流(Jsc)皆有明顯提升,惟填充因子受介面電阻較大而降低,效率值僅1.24%。經改良多孔二氧化鈦厚度至1.7µm可使效率提升至1.49%。為改良介面性質以4,4’-Bis((4-vinylbenzyloxy)methyl)-2,2''-bipyridine (ligand)作為交聯劑改變RuS化學結構,染料脫附測驗顯示鹼液浸泡後工作電極上可保留77%的染料,並初步檢驗元件效率可達到2.12%,其他光電特性也一併提升。接著以帶有lithium和1-ethyl-3-methylimidazolium離子之化合物吸附於經交聯ligand的RuS上,結果除了吸附lithium bis(trifluoromethylsulfonyl)imide (LiTFSI)能提升Voc和Jsc並讓效率達到2.55%外其他無法增進元件表現,照光交流阻抗證實吸附後電阻降低。下一步利用苯甲酸鎂與鈣吸附在經ligand交聯的RuS表面上,兩者之Jsc皆比吸附LiTFSI得到更大幅度的提升,吸附苯甲酸鎂後效率值更達到2.66%,照光交流阻抗分析中介面電阻比未吸附下降許多,也證實具有改良介面之效。再利用乙醯丙酮鎂、鈣、鋇吸附在ligand上作成元件,其中吸附乙醯丙酮鎂能得到最大的效率2.82%,交流阻抗中介面電阻也比吸附苯甲酸鎂小。最後以螢光光譜數據分析經交聯ligand的RuS吸附離子後放光能力下降,證明吸附的離子能加速被激發染料的電荷再生速率,FTIR光譜結果也說明吸附離子後會使未吸附二氧化鈦表面之羧酸基訊號產生紅位移,同時使雙吡啶官能基訊號增強,表示吸附離子確實產生鍵結並改善RuS與固態電解質間的介面相容性。


In this study the crosslinkable ruthenium complex with styryl groups, denoted as RuS, was synthesized and characterized and applied to solid-state dye sensitized solar cell. The resulting open circuit voltage (Voc) and short circuit current (Jsc) were substantially enhanced compared to N3 dye, but efficiency was only 1.24% due to large interface resistence, leading to lower filled factor. After optimizing the thickness of titanium oxide to 1.7µm, the efficiency was slightly increased to 1.49%. To improve the interface, 4,4’-Bis((4-vinylbenzyloxy)methyl)-2,2''-bipyridine (BVP) ligand was introduced to crosslink with RuS. The crosslinked dye which attached on titanium oxide was more sustainable according to the desorption test. The efficiency rose to 2.12% with enhancement of all the photovoltaic properteis. Then the compounds which consist of Li+ and EMI+ were adsorbed onto the BVP-crosslinked RuS. The efficiency increased to 2.55% as LiTFSI was adsorbed. Not only Voc and Jsc increased, but the interfacial resistence in light condition dramatically decreased. Next, magnesium benzonate and calcium benzonate were individually adsorbed onto the BVP-crosslinked RuS. Both of them could increase the device efficiency, especially for magnesium benzonate. The efficiency was up to 2.66. It is owing to the interface resistence drastically decreased compared to the unadsorbed device. After that, magnesium, calcium and barium acetylacetonate salts were individually adsorbed onto the BVP-crosslinked RuS. By using the optimized amounts of magnesium acetylacetonate, efficiency raised to 2.82%. Compared to magnesium benzonate, the interface resistence with magnesium acetylacetonate was even smaller. Finally, the PL spectra showed that the adsorbed ion could acclerate dye regenegation in view of the decreased PL intensity of dye. IR spectra also showed that the carboxylate signal of RuS became red shift and bpyridine signal enhanced. This results indicated that the ions indeed had the strong interactions with BVP-crosslinked RuS and improved the compatibility between RuS and solid-state electrolyte.

目錄

口試委員會審定書 #
誌謝 i
摘要 iii
Abstract iv
目錄 vi
圖目錄 x
表目錄 xv
Chapter 1 緒論 1
1.1 背景 1
1.1.1 有機高分子太陽能電池 3
1.1.2 染料敏化太陽能電池 4
1.2 太陽光模擬光源與量測 5
1.2.1 太陽光模擬光源 5
1.2.2 太陽能電池光電轉換效率的計算 7
Chapter 2 文獻回顧與研究目的 10
2.1 染料敏化太陽能電池 10
2.2 染料敏化太陽能電池工作原理 10
2.3 光敏化劑 13
2.4 透明導電基板 20
2.5 工作電極 20
2.6 電解質 24
2.6.1 液態電解質 24
2.6.2 離子液體 26
2.6.3 膠態電解質 27
2.6.4 固態電解質 27
2.7 對電極 30
2.8 交流阻抗(AC-impedence) 分析原理 31
2.9 照光強度調制光電壓與光電流圖譜 (Intensity Modulated Photovoltage and Photocurrent Spectroscopy,IMVS/IMPS) 34
2.10 開環電壓衰退的瞬態(open-circuit potential decay transients)與電量收集 (charge extraction)之量測 36
2.11 實驗動機與架構 37
Chapter 3 實驗設備與方法 39
3.1 實驗藥品 39
3.2 實驗儀器與設備 41
3.3 合成方法 42
3.3.1 合成 RuS 42
3.4 二氧化鈦鍍液製備 46
3.5 薄膜電極製備 47
3.5.1 導電玻璃之清洗 47
3.5.2 二氧化鈦緻密層(compact layer)製備 47
3.5.3 多孔性二氧化鈦電極 47
3.5.4 電洞傳輸層(Hole-transporting material, HTM)製備 48
3.5.5 對電極製備 48
3.5.6 量測樣品製備方法 48
3.5.7 太陽能電池光電化學測試 49
Chapter 4 結果與討論 52
4.1 RuS 52
4.1.1 RuS鑑定 52
4.2 未改質RuS之固態染料敏化太陽能電池元件分析 53
4.3 BVP ligand經交聯對RuS元件之影響 63
4.3.1 含有BVP ligand經交聯後之元件表現 67
4.3.2 含有BVP ligand經交聯並以正一價離子吸附之元件表現 74
4.3.3 含有BVP ligand經交聯並以含苯甲酸根之正二價離子吸附後元件表現 89
4.3.4 含有BVP ligand經交聯並以含乙醯丙酮根之正二價離子吸附後元件表現 101
4.3.5 比較經苯甲酸根和乙醯丙酮根之鎂離子吸附後元件表現 111
Chapter 5 結論 124
參考文獻 126
附錄 133


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