本論文針對鈣鈦礦太陽能電池碳電極研究並且分為兩個部分，第一部份為大面積的設計與開發，我們探討串聯與並聯對元件效率的關係與影響，並且製作出面積為19 cm2之元件，其開路電壓可以達到3.3伏特，效率可以達到6.64%。並且在科技部的計畫下設計出了2X2的大面積碳電極鈣鈦礦太陽能電池，設計出最佳的模組後，我們探討了不同的滲透溫度，以及不同溶劑比例的影響。實際面積3 cm2時，效率可以達到9.77%。採用封裝後，其效率可以穩定的維持在9.5%上下超過2200小時。
第二部分則是在原本碳電極的基礎上，藉由更換使用om-TiO2來增加填充因子，添加NiO用以增加開路電壓，我們使用1000nm om-TiO2 /500nm Al2O3/ 500nm NiO /Carbon之元件，使用兩步沉積法在65度時滴塗3μL的二碘化鉛溶液(DMF/DMSO 9/1)，可以得到最好的效率。其光電轉換效率為14.32%，IPCE積分電流可達18.55 mA cm-2，元件的平均效率為13.98±0.34 %。

My thesis is focused on large scale and polymer-template carbon-based mesoscopic perovskite solar cells (CMPSC). For design and development of large scale CMPSC, the small modules of CMPSC were well studied. The VOC and power conversion efficiencies (PCE) have respectively reached 3.3 V and 6.64% of the devices with 19 cm2 area. For a 2*2 cm2 CMPSC devices, effects of different penetration temperatures as well as the different solvent ratios both were well studied. The PCE can reach 9.77% with actual working area of 3 cm2; moreover, the encapsulated CMPSC long-term stability can reach over 2200 hours.
The second part device engineering of polymer-template CMPSC, the polymer-template TiO2 was introduced, in order to improve the filtration of precursor solution. Moreover, one more NiO mesoporous layer was inserted between Al2O3 and carbon layer, which that served as hole extraction layer. The device structure of 1000nm polymer-template TiO2 / 500nm Al2O3 / 500nm NiO / Carbon showed the best PCE, 14.32% (average is 13.98 ± 0.34%) and IPCE integration current is up to 18.55 mA cm-2 with the modified two-step deposition method.

摘要 i
Abstract ii
誌謝 iii
目錄 iv
圖目錄 vii
表目錄 xiii
第一章 緒論 1
第二章 文獻回顧 3
2-1 鈣鈦礦太陽能電池 (Perovskite solar cell) 3
2-1-1 鈣鈦礦太陽能電池的發展 5
2-1-2 工作原理與機制 14
2-1-3 鈣鈦礦太陽能電池之優劣勢 16
2-1-4 鈣鈦礦太陽能電池結構 21
2-1-5 鈣鈦礦成膜方法 24
2-2 無電洞傳輸層之鈣鈦礦太陽能電池-碳電極 27
2-3 研究動機 38
第三章 實驗步驟與方法 39
3-1 實驗藥品與儀器 39
3-2 實驗步驟 45
3-2-1 導電玻璃FTO的蝕刻與清洗 46
3-2-2 緻密二氧化鈦層的製備 46
3-2-3 網印多孔性二氧化鈦薄膜 47
3-2-4 網印多孔性氧化鋁阻絕層和碳電極 47
3-2-5 沉積鈣鈦礦 48
3-3元件量測 50
3-3-1鈣鈦礦太陽能電池之光電轉換效率量測 50
3-3-2鈣鈦礦太陽能電池外部量子效率量測 52
第四章 鈣鈦礦太陽能電池碳電極-大面積 53
4-1 碳電極元件厚度優化 54
4-1-1不同二氧化鈦薄膜厚度對元件效率之影響 54
4-1-2 不同氧化鋁薄膜厚度對元件效率之影響 57
4-2 不同串聯並聯之大面積模組 60
4-3 2X2大面積電池模組優化 65
4-3-1 2X2大面積電池不同模組及滴塗方式對元件效率之影響 65
4-3-2 2X2大面積電池不同滲透溫度對元件效率之影響 70
4-3-3 2X2大面積電池不同溶劑比例對元件效率之影響 72
4-3-4 2X2大面積電池封裝及長效性測試 76
4-4 結論 79
第五章 鈣鈦礦太陽能電池碳電極元件優化 80
5-1 元件結構 80
5-2 二氧化鈦薄膜最佳化 82
5-2-1 不同二氧化鈦薄膜製作方法 82
5-2-2 不同二氧化鈦之效率比較 88
5-3 不同氧化鋁薄膜厚度對元件效率之影響 93
5-4 不同氧化鎳薄膜厚度對元件效率之影響 95
5-5 不同滲透溫度對元件效率之影響 98
5-6 滴加不同二碘化鉛溶液量對元件效率之影響 100
5-7 不同溶劑比例對元件效率之影響 103
5-8 不同二氧化鈦薄膜以及有無添加氧化鎳比較 106
5-9 結論 112
第六章 總結 115
參考文獻 116

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