醇溶性富勒烯衍生物的摻雜對低溫製備TiO2電子萃取能力的影響

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王秉承(Bing-Cheng Wang) 查詢紙本館藏

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醇溶性富勒烯衍生物的摻雜對低溫製備TiO2電子萃取能力的影響
(Effect of Doping of Alcohol-Soluble Fullerene Derivatives on Electron Extraction of TiO2 at Low Temperature)

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摘要(中)

鈣鈦礦太陽能電池(Perovskite Solar Cell，簡稱PSC)，光電轉換效率最高達24.2%(與矽晶圓太陽能電池的效率差不多)。以低溫方式所製備的TiO2(Lt-TiO2)膜作為一般式PSC的電子傳遞層(electron transporting layer，ETL)，雖然有利於低成本製造及軟性基材應用，但Lt-TiO2膜有高缺陷密度及低電子萃取能力之缺點，導致所組裝的一般式PSC有嚴重的遲滯現象，影響其商品化行程。本研究透過使用具有高導電度及醇溶性的富勒烯衍生物，如：C60-RT2、C60-RT6、C70-RT2作為添加劑，製備含富勒烯衍生物的TiO2的奈米複合物膜(Cx-RTy:Lt-TiO2)作為一般式PSC的電子傳遞層，結果以C60-RT6:Lt-TiO2為ETL之元件有最佳的光電轉換效率，C60-RT6的添加能增加Lt-TiO2 ETL的電子萃取能力、導電度，減少缺陷，增加緻密度及親水性。並使沈積在ETL上的鈣鈦礦(Psk)膜有較大顆粒。由於C60-RT6材料中胺基(R-NH3+)上的氫會與鈣鈦礦結構中I產生氫鍵作用力，因此沉積於C60-RT6:Lt-TiO2膜上的Psk膜的結晶度比沈積於Lt-TiO2上的高。不管C60-RT6:Lt-TiO2膜(含2.25 wt% C60-RT6的C60-RT6:Lt-TiO2)是在100℃或室溫下乾燥30分鐘所製備的，尤其為ETL所組裝成PSC元件的光電轉換效率分別為17.99%(室溫乾燥)及17.51%(100℃加熱乾燥)均比其相同條件下製備的純Lt-TiO2膜為ETL的元件之光電轉換效率分別為14.47%及15.52%高，且元件的遲滯現象小，在手套箱中的長時間穩定性也較好。

摘要(英)

Perovskite Solar Cell (PSC) has a power conversion efficiency of up to 24.2% (close to the efficiency of silicon wafer based solar cells). The TiO2 (Lt-TiO2) film prepared by low temperature method used as the electron transporting layer (ETL) in the regular PSC has the advantage of low-cost fabrication and flexible substrate applicable, nevertheless, it also has defect density. Furthermore Lt-TiO2 also has low electron extraction ability, resulting in a serious current hysteresis of the corresponding regular PSC. In this study, the fullerene derivatives (such as C60-RT2, C60-RT6, and C70-RT2) with alcohol solubility were prepared to be an additive for Lt-TiO2 electron transporting material (ETM). The additive all improve the photovoltaic performance of Lt-TiO2 ETL and amongst these three fullerene derivatives, C60-RT6 has the best performance. Comparing to Lt-TiO2 film, C60-RT6:Lt-TiO2 nanocomposite film has better electron extraction ability、higher conductivity、less defects and more hydrophilic no matter the ETL was heated at 100°C or dried at ambient atmosphere for 30 minutes. As a result perovskite (Psk) film deposited on the C60-RT6:Lt-TiO2 nanocomposite film has larger particles and better crystallinity than that deposited on Lt-TiO2 ETL. The power conversion efficiencies of the regular PSC besed on C60-RT6:Lt-TiO2 nanocomposite ETL increases to 17.99% (when the ETL was dried at room temperature) and 17.51% (ETL was heated at 100°C) respectively which are higher than those (14.47% and 15.52%, respectively) of the cells based on pure Lt-TiO2 ETL prepared under the same conditions. At the same time the current hysteresis is smaller and the long-term stability in the glove box is better for the cell based on C60-RT6:Lt-TiO2 nanocomposite ETL compared to those using Lt-TiO2 ETLs.

關鍵字(中)

★ 鈣鈦礦
★ 二氧化鈦
★ 富勒烯衍生物

關鍵字(英)

論文目次

摘要 I
Abstract VII
Graphical Abstract IX
謝誌 X
目錄 XI
圖目錄 XVI
表目錄 XXII
第一章、緒論 1
1-1、前言 1
1-2、鈣鈦礦太陽能電池(Perovskite solar cell, PSC) 4
1-2-1. 鈣鈦礦太陽能電池的架構 4
1-2-2. 一般式鈣鈦礦太陽能電池的工作原理 5
1-2-3. 鈣鈦礦太陽能電池的光電轉換效率 6
1-3、鈣鈦礦太陽能電池之研究歷程 9
1-3-1. 第一個將鈣鈦礦材料應用於太陽能電池的研究 9
1-3-2. 固態電解質應用於鈣鈦礦太陽能電池 12
1-4、鈣鈦礦活性層的製備方法 14
1-4-1. 以一步驟合成法製備鈣鈦礦活性層 15
1-4-2. 以兩步驟合成法製備鈣鈦礦活性層 16
1-4-3. 一步驟反溶劑處理法製備鈣鈦礦活性層 18
1-5、 TiO2作為鈣鈦礦太陽能電池中電子傳輸層的發展 20
1-5-1. 高溫鍛燒製備TiO2膜(Ht-TiO2) 20
1-5-2. 低溫方式製備的TiO2 膜(Lt-TiO2) 20
1-5-3. Li-TFSi應用於Ht-TiO2 22
1-5-4. C60衍生物應用於Lt-TiO2 23
1-5-5. C70應用於Lt-TiO2 31
1-5-6. 水溶性C60衍生物-應用於Ht-TiO2 34
1-6、胺基上的氫會與鈣鈦礦中的碘產生氫鍵作用 39
1-7、研究動機 42
第二章、實驗部分 43
2-1、實驗藥品與儀器設備 43
2-1-1. 藥品 43
2-1-2. 儀器設備 44
2-2、一般式鈣鈦礦太陽能電池組裝步驟 45
2-2-1. 藥品配製 45
2-2-2. 元件組裝步驟 48
2-3、儀器分析及樣品製備 52
2-3-1. 太陽光模擬器及光電轉換效率量測 (Solar Simulator, KXL-500F) 52
2-3-2. 掃描式電子顯微鏡 (Scanning Electron Microscope, Hitachi S-800) 53
2-3-3. X-ray 繞射光譜儀 (X-Ray Diffractometer, BRUKER D8 Discover ) 54
2-3-4. 熱蒸鍍系統(Thermal evaporation system) 55
2-3-5. 太陽能電池外部量子效率量測系統 (Incident Photon to Current Conversion Efficiency (IPCE), PVCS-I) 55
2-3-6. 光激發螢光光譜儀(Photoluminescence Spectrometer) 56
2-3-7. XPS光電子能譜儀 (X-ray photoelectron spectroscopy) 57
2-3-8. UPS紫外光電子能譜儀(Ultraviolet photoelectron spectroscopy) 58
2-3-9. 接觸角量測儀(contact angle) 58
第三章、結果與討論 59
3-1、最佳Cx-RTy:Lt-TiO2 ETM的篩選 59
3-1-1. Cx-RTy:Lt-TiO2及Lt-TiO2 ETM以100℃加熱30分鐘作為ETL的光伏表現 59
3-1-2. Cx-RTy:Lt-TiO2及Lt-TiO2 ETM以室溫乾燥30分鐘作為ETL的光伏表現 60
3-2、以100-Lt-TiO2、R-Lt-TiO2、100-C60-RT6:Lt-TiO2及R-C60-RT6:Lt-TiO2為ETL所組裝之元件的IPCE量測 63
3-3、以100-Lt-TiO2、R-Lt-TiO2、100-C60-RT6:Lt-TiO2及R-C60-RT6:Lt-TiO2為ETL所組裝之元件的電流遲滯現象 64
3-4、 2.25 wt% C60-RT6 : Lt-TiO2 ETL之XPS縱深分析 66
3-5、 C60-RT6:Lt-TiO2與Lt-TiO2膜的光學性質及前置軌域能階 68
3-5-1. UV-vis吸收光譜 68
3-5-2. C60-RT6:Lt-TiO2與Lt-TiO2層的前置軌域能階 70
3-6、 C60-RT6的添加對Lt-TiO2導電度影響 74
3-7、加入C60-RT6於Lt-TiO2中對Lt-TiO2膜接觸角表面親疏水性的影響 76
3-8、添加C60-RT6於Lt-TiO2對Lt-TiO2膜表面形貌的影響 77
3-9、添加C60-RT6於Lt-TiO2對Lt-TiO2膜表面粗糙度的影響 79
3-10、沈積在四個ETLs膜上的鈣鈦礦膜之SEM表面形貌 81
3-11、沈積在100-Lt-TiO2、R-Lt-TiO2、100-C60-RT6:Lt-TiO2及R-C60-RT6:Lt-TiO2膜上的鈣鈦礦膜之光學性質 84
3-12、沈積在100-Lt-TiO2、R-Lt-TiO2、100-C60-RT6:Lt-TiO2及R-C60-RT6:Lt-TiO2膜上的鈣鈦礦膜之結晶度 84
3-13、沈積在100-Lt-TiO2、R-Lt-TiO2、100-C60-RT6:Lt-TiO2及R-C60-RT6:Lt-TiO2膜上的鈣鈦礦膜之PL及TRPL光譜圖 90
3-14、以100-Lt-TiO2、R-Lt-TiO2、100-C60-RT6:Lt-TiO2及R-C60-RT6:Lt-TiO2為ETL之一般式鈣鈦礦太陽能電池之長時間穩定性 92
3-15、優化以R-C60-RT6:Lt-TiO2為ETL所組裝之元件的光電轉換效率及在大氣下長時間穩定性 94
3-15-1. 降低R-C60-RT6:Lt-TiO2的膜厚 94
3-15-2. 以P3HT作為電洞傳輸層 95
第四章、結論 98
參考文獻 100

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指導教授

吳春桂

審核日期

2019-8-21

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