以有機鹵化鉛為基礎的鈣鈦礦太陽能電池的效率在近幾年來節節攀升，與鈣鈦礦組成工程息息相關。通過調控鈣鈦礦ABX3晶體結構中陰陽離子的佔比，除了能夠改變能帶隙大小，更是對結構穩定性也有顯著的幫助，使其製成的光伏元件成功在短時間內實現與矽晶型太陽能電池互相比擬的轉換效率(25.5 %)。然而目前普遍用以製作有機鹵化鉛鈣鈦薄膜的製程技術依舊無法將所有前驅物反應完畢，導致薄膜中未反應前驅物會以殘留物的形式存在於元件內部進而干涉電池的運作。此現象對於混合鈣鈦礦中陰陽離子比例調控造成一定程度的困擾，像是前驅液中陰陽離子配比與最終薄膜中陰陽離子配比發生偏離，且其偏離的程度無從得知。正因如此，發展鈣鈦礦薄膜中組成物的定量技術可視為鈣鈦礦光伏技術進一步提升效率的重要一環，因為其不僅可以獲取薄膜中的真實組成資訊，同時也可以藉由了解鈣鈦礦薄膜的組成進行製程的優化調整。
本研究中發展了一個簡便的流程將鈣鈦礦薄膜的組成進行還原工程。藉由不同的溶劑分離，可將鈣鈦礦薄膜中存在的各項組成諸如有機殘留物、鈣鈦礦以及無機殘留物完全分離。接著使用普及率高以及檢測時間短的紫外光-可見光光譜儀進行定量的分析，成功地解析出鈣鈦礦薄膜實際的化學計量以及殘留物。運用此技術，對一步法製程與兩步法製備的鈣鈦礦薄膜組成進行比較，結果顯示薄膜中鈣鈦礦的陰陽離子組成與前驅溶液的比例確有偏差，且對其元件性能造成直接影響。另一方面，對於相同批次的薄膜中利用一步法所製備的鈣鈦礦含量存在發散的情形，該情形在兩步法中則是以無機殘留物含量為主，並且兩種製程幾乎都取決於多孔支架層塗佈基板的表面性質，此問題終將會影響到太陽能電池的效率差異，未來必須對薄膜元件進行適當的控制以利於提升相同批次元件之間的效率一致性，有望幫助未來商業應用的發展。

Compositional engineering of organo-lead halide perovskite determines the reproducibility and versatility of device performance, which is a crucial threshold toward commercialization. A tuneable band-gap and material stability can be easily achieved by manipulating ion composition in perovskite ABX3 crystal structure within a reasonable tolerance factor range. Although perovskite solar cells have been approved showing comparable performance as silicon crystalline solar cells, the stoichiometry on final perovskite film attracts little attention from worldwide research groups.
This study provides a simple method that can identify the actual composition of the perovskite material. By the analysis of UV-Vis spectra, all the components consisting of the final perovskite file can be quantified, including organic/inorganic residue. The result of the analysis shows a composition mismatch between precursor solution and solid-state perovskite film. We also find that the devices containing mesoporous TiO2 layer display a higher variation on perovskite chemical composition. Further investigation indicates that the surface property of the mesoporous TiO2 layer determines the different composition signatures on the device prepared by the one-step or two-step method. By using this composition analysis, we can control to improve the efficiency consistency of the same batch, which is expected to help develop future commercial applications.

摘要 I
ABSTRACT II
誌謝 III
目錄 V
圖目錄 VIII
表目錄 X
第一章 緒論 1
1-1 前言 1
1-2 太陽能電池的原理 2
1-3 太陽能的發展 3
第二章 文獻回顧 7
2-1 鈣鈦礦太陽能電池 7
2-1.1鈣鈦礦的發現與特性 7
2-1.2鈣鈦礦太陽能電池的發展 9
2-1.3鈣鈦礦太陽能電池的原理 16
2-1.4肖克利-奎伊瑟極限 19
2-1.5鈣鈦礦太陽能電池結構 20
2-1.5.1多孔型電池結構 20
2-1.5.2多孔超結構型電池結構 21
2-1.5.3平面異質型電池結構 22
2-1.5.4反式電池結構 23
2-2 有機鹵化鉛鈣鈦礦之材料化學 24
2-2.1 MAPbI3 24
2-2.2 FAPbI3 24
2-2.3 CsPbI3 24
2-2.4組成工程 25
2-2.4.1 A位陽離子組成 25
2-2.4.2 X位陰離子組成 26
2-3 鈣鈦礦薄膜的製備方式 28
2-3.1一步沉積法 28
2-3.2兩步沉積法 30
2-3.2.1兩步浸泡沉積法 30
2-3.2.2兩步旋塗沉積法 31
2-3.3熱蒸鍍沉積法 33
2-3.4蒸氣輔助溶液加工法 33
2-4 鈣鈦礦薄膜製備過程的化學計量 34
2-4.1一步沉積法 34
2-4.2兩步旋塗沉積法 37
2-5 鈣鈦礦薄膜之殘留物 38
2-5.1無機殘留物 38
2-5.2有機殘留物 39
2-6 鈣鈦礦薄膜的組成標示 41
2-7 鈣鈦礦薄膜組成的定量研究 42
2-7.1鈣鈦礦薄膜化學計量組成 42
2-7.2鈣鈦礦薄膜A位離子組成 43
2-7.3定量技術之探討 45
2-8 研究動機 46
第三章 實驗方法與儀器分析 47
3-1 實驗藥品與材料 47
3-2 實驗儀器與分析設備 48
3-3 分析儀器介紹 49
3-3.1紫外光-可見光光譜儀 49
3-3.2場發射掃描式顯微鏡 49
3-3.3太陽光模擬器 50
3-4 鈣鈦礦薄膜元件流程 54
3-4.1 FTO導電玻璃基板前處理 54
3-4.2電子傳輸層製備流程 54
3-4.3多孔支架層製備流程 54
3-4.4一步法鈣鈦礦薄膜製備 55
3-4.4.1前驅液配備 55
3-4.4.2鈣鈦礦薄膜製備流程 55
3-4.5兩步法鈣鈦礦薄膜製備 55
3-4.5.1前驅液配備 55
3-4.5.2鈣鈦礦薄膜製備流程 55
3-4.6電洞傳輸層與背電極製備流程 56
3-5 定量模型設計理論 56
3-5.1分析儀器的選擇 56
3-5.2比爾定律的原理 57
3-5.3比爾定律之限制與假設 58
3-5.4比爾定律的加成性質 59
3-6 定量實驗流程 59
3-6.1鈣鈦礦薄膜組成分離 59
3-6.2檢測溶液轉換 59
第四章 結果與討論 60
4-1 量化模型設計 60
4-1.1標準前驅物檢定 60
4-1.1.1標準前驅物之吸收曲線 60
4-1.1.2標準前驅物之線性迴歸 61
4-1.1.3標準混合前驅物 62
4-1.2實驗設計 65
4-1.2.1有機殘留物分離 65
4-1.2.3有機前驅物分離 67
4-1.2.4無機殘留物與無機前驅物分離 70
4-1.3檢測溶劑限制 70
4-1.4溶劑轉換 72
4-1.5薄膜組成計算方式 72
4-2 量化結果分析 73
4-2.1鈣鈦礦薄膜品質與元件性能 73
4-2.2鈣鈦礦薄膜定量結果 75
4-2.3陰陽離子組成與元件性能之探討 77
4-2.4陰陽離子組成比例偏差之原因 78
4-2.5製程可重複性探討 80
第五章 結論 85
第六章 未來工作 86
第七章 參考文獻 87

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