利用馬倫哥尼效應製備高品質高效率鈣鈦礦太陽能電池

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紀仲嘉(Ji Zhong-Jia) 查詢紙本館藏

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能源工程研究所

論文名稱

利用馬倫哥尼效應製備高品質高效率鈣鈦礦太陽能電池
(High-Performance Perovskite Solar Cells Fabricated via Marangoni Effect)

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摘要(中)

新世代鈣鈦礦太陽能電池在短短幾年內效率已突破 22%，以非常快的速度逼近矽晶太陽能電池，而在高效率的鈣鈦礦太陽能電池中，緻密、無孔洞、大晶粒、高結晶品質的鈣鈦礦層，一直是科學家研究的重點。本研究中使用 Single-Step 配合反溶劑法製作高品質鈣鈦礦層，研究發現反溶劑甲苯旋塗後會與鈣鈦礦前驅液溶劑因表面張力差形成「馬倫哥尼應」，此效應會使 MAI-PbI2-DMSO 中間相分佈不均，造成孔洞與結晶缺陷，為解決此效應我們利用一種簡單的延遲熱退火機制，可有效使中間相均勻化，在 100℃退火後形成高品質高覆蓋率的鈣鈦礦結晶。研究藉由 SEM, XRD, AFM 與 EIS 等儀器分析，找出最佳的優化參數並製作成電池元件，電池效率從無延遲退火的 13.58%提升至最佳參數延遲 40min 退火的 18.02 %(增益 32.69%)。
此外，為了取代傳統高毒性的反溶劑與加快製程速度，本研究選用低毒性的反溶劑乙酸乙酯(EA)，利用其低表面張力高蒸發速度等優勢，快速製備高品質的鈣鈦礦層，研究發現藉由調整 EA 旋塗的用量可以有效解決 EA 揮發太快所造成的鈣鈦礦層孔洞缺陷現象，調整後以 500ul 反溶劑用量有最佳 16.39%的效率，雖然效率比不上優化後的甲苯，但在電池元件的製程中可縮短馬倫哥尼效應需要等待的時間，有助於降低大量製程鈣鈦礦太陽能電池的時間與製作成本。
最終，本研究結合延遲熱退火機制與奈米結構 FTO 基板技術，藉由提高鈣鈦礦層品質、電極與電子傳輸層接觸面積以及增益鈣鈦礦層吸光效率等優點，成功地製造出具有高電流(23.17mA/cm2)、高電壓(1.07V)、高 FF(77.62%)、低遲滯指數(0.05)以及效率高達 19.29%的高效率鈣鈦礦太陽能電池。

摘要(英)

In this study, we used Single-Step and anti-solvent methods to fabricate a MAPbI3-based perovskite solar cell. However, using the toluene as an anti-solvent will induce the "Marangoni effect" due to difference of the surface tension at the interface between the dripped solvent and the perovskite precursor. This effect will cause non-uniform distribution of the intermediate phase (MAI-PbI2-DMSO) which will form unexpected voids inside the perovskite layer leading to a low-quality perovskite film. Therefore, we introduce a simple delayed-annealing method to achieve a high-quality and high-coverage perovskite layer which can significant improve the non-uniform distribution of the intermediate phase. We use the
SEM(Scanning Electron Microscope), XRD(X-ray Diffractometer), AFM (Atomic Force Microscopic) and EIS（Electrochemical Impedance Spectroscopy） to observe and analyze the quality of perovskite films. In comparison with the control sample (without delayed-annealing), the power conversion efficiency (PCE) will increase from 13.58% to 18.02% (enhanced 32.69%) with the sample annealing at 100℃ for 40 min. Moreover, to replace the traditional toxic anti-solvent and realize a rapid process of forming a high-quality perovskite film, a low-toxic anti-solvent ethyl acetate (EA) is chosen to rapidly fabricate high-quality perovskite layers with the advantages of low surface tension and high evaporation rate. After using EA as the alternative anti-solvent, the highest PCE is 16.39% with dripping the EA of 500ul.
Although the PCE is lower than using traditional toluene as the anti-solvent, it’s unnecessary treating with annealing process for 40 mins to suppress the Marangoni effect which has benefits to reduce the time and cost of fabricate the perovskite solar cells.
Additionally, we further incorporate with nanostructures on the FTO surface to increase the absorption of perovskite layer and contact area between FTO surface and mesoporous layer which can effectively increase the electron transport efficiency.
Finally, the PCE will eventually increase to 19.29% while the sample treated with delayed-annealing method and introduced with the patterned-FTO substrate.

關鍵字(中)

★ 高效率
★ 鈣鈦礦太陽能電池
★ 馬倫哥尼效應
★ 低毒性反溶劑
★ 奈米結構

關鍵字(英)

★ High-Efficiency
★ Perovskite solar cells
★ Marangoni effect
★ Low toxicity anti-solvent
★ Nanostructure

論文目次

摘要 i
Abstract ii
致謝 iii
目錄 iv
圖目錄 vii
表目錄 xi
第1章緒論 1
1-1 前言 1
1-2 太陽能電池的分類與介紹 2
1-2-1 矽太陽能電池 2
1-2-2 化合物太陽能電池 3
1-2-3 有機太陽能電池 3
1-3 有機-無機鈣鈦礦太陽能電池 4
1-3-1 鈣鈦礦太陽能電池演進 6
1-3-2 鈣鈦礦太陽能電池製程方法 8
1.熱蒸鍍法(Thermal Vapor Deposition) 8
2.溶液法(Solution Deposition) 9
1-4 製備高品質高效率鈣鈦礦太陽能電池 10
1-4-1 熱退火優化鈣鈦礦太陽能電池 10
1. 溶劑蒸氣輔助退火(Solvent Annealing,SA) 11
2. 真空輔助熱退火(Vacuum-Assisted Thermal Annealing) 13
3. 溫度控制輔助退火(Thermal Control-Assisted Annealing) 15
1-4-2 反溶劑(Anti-Solvent)法優化鈣鈦礦太陽能電池 17
1-4-3 馬倫哥尼效應(Marangoni Effect)優化鈣鈦礦太陽能電池 21
1-5 研究動機 26
第2章實驗方法 27
2-1 實驗材料及儀器 27
2-1-1 實驗材料 27
2-1-2 實驗儀器 28
2-2 鈣鈦礦太陽能電池材料製備 29
2-2-1 甲基胺碘(CH3NH3I)合成 29
2-2-2 鈣鈦礦主動層(CH3NH3PbI3)溶液配製 29
2-2-3 二氧化鈦緻密層(TiO2 Compact)溶液配製 29
2-2-4 二氧化鈦介孔層(TiO2 Mesoporous)溶液配製 29
2-2-5 電洞傳輸層(Spiro-OMeTAD)溶液配製 29
2-3 鈣鈦礦太陽能電池元件製作 30
2-3-1 FTO玻璃基板清洗 30
2-3-2 二氧化鈦緻密層(TiO2 Compact)沉積 30
2-3-3 二氧化鈦介孔層(TiO2 Mesoporous)沉積 30
2-3-4 鈣鈦礦主動層(CH3NH3PbI3)沉積 30
2-3-5 電洞傳輸層Spiro-OMeTAD沉積 30
2-3-6 銀(Ag)電極蒸鍍 31
2-4 具奈米結構FTO基板製作 32
2-4-1 奈米結構光阻遮罩製備 32
2-4-2 奈米結構FTO基板蝕刻 32
第3章結果與討論 33
3-1 鈣鈦礦太陽能電池製程結果 33
3-2 製備高品質鈣鈦礦層 34
3-2-1 甲苯反溶劑後立即熱退火所帶來的缺陷 34
3-2-2 甲苯反溶劑後延遲熱退火優化鈣鈦礦層 36
1. 元件表面與SEM結晶形貌觀測 36
2. XRD晶格繞射分析 40
3. AFM形貌分析 42
4. 延遲熱退火對電池效能增益 44
3-2-3優化鈣鈦礦層對遲滯效應影響 47
3-3以低毒性反溶劑快速製備鈣鈦礦層 50
3-3-1 EA反溶劑用量測試 50
3-3-2 EA反溶劑延遲退火測試 54
3-4 以結構基板製備高效率鈣鈦礦太陽能電池 56
3-4-1 SEM觀測正光阻(S1805)製備奈米結構基板 56
3-4-2 SEM觀測負光阻(AZ-5214E)製備奈米結構基板 57
3-4-3具奈米結構基板效能分析 59
第4章結論 62
參考文獻 63

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指導教授

詹佳樺(Chan Chia-Hua)

審核日期

2018-6-25

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