以CsPbI2Br為吸光層所製備出的無機鈣鈦礦太陽能電池因具備良好的先天熱穩定性以及合理的能隙(Eg=1.92eV)，引起了極大的關注。然而，傳統的一步法製備CsPbI2Br鈣鈦礦吸光層，通常會有低結晶性、鈣鈦礦薄膜形貌差等問題，從而影響其鈣鈦礦元件之光伏表現。
在本研究中，我們開發一種全新的三步驟浸泡法，並結合甲胺蒸氣修補技術，不僅加強了無機鈣鈦礦之相穩定性，同時改善了薄膜形貌。首先透過兩步驟浸泡法製備無機鈣鈦礦CsPbI2Br，再將黃相的無機鈣鈦礦CsPbI2Br刻意浸泡於有機MAX溶液中(MAX = MAI/ MABr)用以形成有機無機的鈣鈦礦化合物，以增加對後續甲胺修補步驟時之甲胺吸收度。接著將此刻意製作的有機無機的鈣鈦礦化合物暴露於甲胺蒸氣中形成一透明的液態中間相薄膜，使其具流動性達到平坦化以改善薄膜的形貌。最後將此有機無機的薄膜置於280℃下退火15分鐘釋放有機分子，同時也進行相轉變形成黑相的α-CsPbI2Br。通過甲胺蒸氣修補的鈣鈦礦薄膜能具有較佳的結晶性以及較好的薄膜形貌，使得後續的光伏元件特性得以提升。此外，我們改善退火流程，採取梯度熱退火的方式以減少薄膜上的孔洞以及缺陷。目前以此三步法製備的CsPbI2Br無機鈣鈦礦太陽能電池效率可達到10.9%。
隨後，我們將此製程推展至本實驗室特有的水性硝酸鉛前驅物系統中。有別於PbI2/DMF系統，水性硝酸鉛前驅物系統將低毒性的水性硝酸鉛薄膜浸泡於以異丁醇(i-BuOH)為溶劑的碘液中，使之先行轉化為片狀多孔之碘化鉛薄膜，接著再接續第一階段的研究成果之流程，利用有機MAX溶液浸泡以及甲胺蒸氣法改善薄膜形貌與結晶性，最終元件效率達到8%，分析其原因為硝酸鉛起始塗層覆蓋率不足致使鈣鈦礦層形貌更加難以控制，雖然經過甲胺蒸氣修補，最終CsPbI2Br薄膜的形貌仍不夠緻密所致，儘管如此，此製程為無機鈣鈦礦電池研究中第一個完全使用低毒性的醇類與水為溶劑的製程，希望未來經由後人的努力能有所突破。

All-inorganic perovskite solar cells (PSCs) based on CsPbI2Br absorber have attracted tremendous attention due to their promising intrinsic thermal stability and reasonable bandgap (1.92eV). Nevertheless, traditional one-step spin-coated CsPbI2Br film usually suffers from low crystallinity and poor morphology which impedes its photovoltaic performance. Herein, a novel three-step dipping method combined with methylamine (MA) gas healing is unprecedentedly developed to improve phase stability and film morphology. In this study, we prepared inorganic perovskite CsPbI2Br film through a two-step dipping approach. Following by dipping inorganic perovskite intentionally into MAX solution (MAX = MAI/ MABr) to form a hybrid organic-inorganic perovskite compound to increase the absorbance of MA gas; this intermediate compound was then treated by MA gas healing to further improve the film morphology. Finally, the hybrid film was annealed at 280℃ for 15 minutes to release the organic components and form the black phase. Through MA healing, the resulting perovskite film with higher crystallinity, better morphology, and enhanced photovoltaic performance was achieved. Besides, we adopted the gradient thermal annealing method to minimize the defects and pinholes on the film. Currently, the conversion efficiency of 10.9% is achieved in all-inorganic CsPbI2Br-based PSC.
Later on, we promoted this procedure into the Pb(NO3)2/ H2O system. The Pb(NO3)2 film was firstly dipped into iodine solution to transform it into mesoporous flake-shaped lead iodide. Then, we followed the procedure in the previous investigation. The film was treated with MA gas healing to improve the film morphology and crystallinity. The resulting cell conversion efficiency reached 8%. It results from the low coverage of Pb(NO3)2 layer leading to low compactness of inorganic perovskite film. Nevertheless, this is the first-ever low toxicity fabrication of inorganic PSCs.

摘要 I
ABSTRACT II
誌謝 III
圖目錄 VII
表目錄 XI
第一章 緒論 1
1-1 前言 1
第二章 文獻回顧 4
2-1 鈣鈦礦太陽能電池（Perovskite solar cell） 4
2-1.1 鈣鈦礦的發現與結構 4
2-1.2 鈣鈦礦太陽能電池的發展 5
2-1.3 鈣鈦礦太陽能電池的結構與運作原理 6
2-2. 鈣鈦礦吸光層的製備方式 9
2-2.1旋轉塗佈法 9
2-2.2 甲胺蒸氣修飾法 14
2-3 無機鈣鈦礦太陽能電池 (Inorganic PSC) 15
2-3.1 無機鈣鈦礦太陽能電池的起源 15
2-3.2 無機鈣鈦礦太陽能電池的發展 18
2-3.3 無機鈣鈦礦CsPbX3太陽電池技術發展的迷思 23
2-3.4銫鉛鹵化物CsPbX3之結構與光電特性 25
2-3.5 CsPbX3之製備方式 29
2-3.5.1一步溶液法旋塗製備CsPbX3 29
2-3.5.2 一步法製程中使用甲胺蒸氣改良 32
2-3.5.3 兩步溶液法製備CsPbX3 35
2-4 低毒性硝酸鉛製程 38
2-4.1 高毒性溶劑的隱憂 38
2-4.2 硝酸鉛水溶液為鈣鈦礦前驅物之發展 39
2-5 研究目的與動機 43
第三章 研究方法與儀器分析 45
3-1 實驗儀器與分析設備 45
3-2 實驗藥品和相關材料 46
3-3 實驗方法與步驟 47
3-3.1 FTO導電玻璃前處理與製備TiO2電子傳輸層 47
3-3.2 鈣鈦礦前驅液、HTM(Spiro-OMeTAD)溶液配製 48
3-3.3 鈣鈦礦層製作流程 49
3-3.4 製備電洞傳輸層(HTL)與對電極 50
3-4 儀器分析 52
3-4.1 X光繞射儀(X-ray diffractometer, XRD) 52
3-4.2 紫外光-可見光光譜儀(Ultraviolet-visible spectrometer, UV-vis) 53
3-4.3 場發射掃描式顯微鏡(Field emission scanning electron microscope, FESEM) 55
3-4.4 太陽光模擬器(Solar simulator)和J-V曲線 56
3-4.4.1 I-V特性曲線 57
3-4.4.2 短路電流(Short-circuit current, Jsc) 59
3-4.4.3 開路電壓(Open-circuit voltage, Voc) 59
3-4.4.4 填充因子(Fill factor, FF) 60
3-4.4.5 光電轉換效率(Power conversion efficiency, PCE, η%) 60
第四章 實驗結果與討論 61
4-1無機鈣鈦礦CsPbX3之系統建立 61
4-1.1 一步法製備CsPbI3 61
4-1.2 PMMA塗佈技術 62
4-1.3 一步法製備CsPbI2Br 63
4-2 碘化鉛/DMF系統下製備CsPbI2Br 64
4-2.1兩步法製備CsPbI2Br 64
4-2.1.1 CsX鹵素比例的調整 64
4-2.1.2 CsX浸泡時間之優化 65
4-2.2 CsPbI2Br鈣鈦礦薄膜之修飾 67
4-2.2.1 MA蒸氣法 67
4-2.2.2 MAX浸泡時間優化 71
4-2.3 梯度熱退火法(Gradient Thermal Annealing Method, GTA) 73
4-2.3.1梯度熱退火法設計流程與目的 73
4-2.3.2 梯度熱退火法之成果 76
4-3 Pb(NO3)2/H2O系統下製備CsPbI2Br 80
4-3.1 三步法製備CsPbI2Br無機鈣鈦礦 81
4-3.1.1 以硝酸鉛起始層製備碘化鉛薄膜 81
4-3.1.2 製備CsPbI2Br無機鈣鈦礦薄膜 83
4-3.2 硝酸鉛系統下的MA蒸氣修飾法 88
第五章 結論 100
第六章 未來工作 102
第七章 參考文獻 103

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