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研究生: 黃啟奕
Huang, Chi-Yi
論文名稱: FAPbI3鈣鈦礦太陽能電池製程條件的優化及其添加劑的鈍化效應
Optimization of Fabrication Process for FAPbI3 Perovskite Solar Cell and Passivation Effects of Additives
指導教授: 李玉郎
Lee, Yuh-Lang
學位類別: 碩士
Master
系所名稱: 工學院 - 化學工程學系
Department of Chemical Engineering
論文出版年: 2024
畢業學年度: 112
語文別: 中文
論文頁數: 145
中文關鍵詞: 甲胺鹽酸鹽 、一步驟熱處理 、鈣鈦礦太陽能電池 、反溶劑體積
外文關鍵詞: Methylammonium chloride, one-step heat treatment, perovskite solar cell, antisolvent volume
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  • 本研究之第一部分為建立FAPbI3鈣鈦礦太陽能電池系統,過去文獻以多步驟熱處理方式(80℃,3min--120℃,5min--70℃,22min)來製備FAPbI3鈣鈦礦薄膜,以降低甲胺鹽酸鹽(MACl)的揮發速率,減少孔洞的產生,其效率高達20.2%。然而文獻並未描述製備過程中的細節,依照其實驗步驟製作,所展現的光電轉效率最高為16.5%。因此希望進透過調整熱處理程序以及反溶劑體積以控制鈣鈦礦薄膜的成核成長及相組成,進而製備出與文獻相當的光電轉換效率。結果發現,從多步驟熱處理調至一步驟熱處理(100℃, 60 min),其Voc與光電轉換效率與文獻相當(1.05 V),冠軍效率為20.1%。
    第二部分將甲胺鹽酸鹽(MACl)溶於氯仿和異丙醇的混合溶劑以作為鈣鈦礦層的表面修飾溶液,透過MA陽離子和氯陰離子分別鈍化負電缺陷(VFA-)與正電缺陷(VI+)。經MACl修飾,Voc從1.05 V提升至1.09 V,光電轉換效率從19.8%提升至20.7%(冠軍效率為21.03%)。

    The first part of this research is to establish a FAPbI3 perovskite solar cell system. In the past, the literature used a multi-step heat treatment method (80℃, 3min→120℃, 5min→70℃, 22min) to prepare FAPbI3 perovskite thin films to reduce the volatilization rate of MACl and reduce the generation of holes, and its efficiency is as high as 20.2%. However, the literature does not describe the details of the preparation process. According to the experimental steps, the photoelectric conversion efficiency displayed is up to 16.5%. Therefore, we want to control the nucleation,growth and phase composition of the perovskite film by adjusting the heat treatment procedure and antisolvent volume, thereby producing a photoelectric conversion efficiency comparable to the literature. The results showed that when the multi-step heat treatment was adjusted to one-step heat treatment (100°C, 60 min), the Voc and photoelectric conversion efficiency were equivalent to those in the literature (1.05 V), and the championship efficiency was 20.1%.
    In the second part, Methylammonium chloride (MACl) in a mixed solvent of chloroform and isopropyl alcohol as a surface modification solution for the perovskite layer, and the negative electron defects (VFA- ) and positively charged defects (VI+). After modification by MACl, Voc was increased from 1.05 V to 1.09 V, and the photoelectric conversion efficiency was increased from 19.8% to 20.7% (champion efficiency is 21.03%).

    摘要 i Extended abstract ii 誌謝 xiii 目錄 xv 表目錄 xix 圖目錄 xx 第一章 緒論 1 1-1 前言 1 1-2 研究目的與動機 4 第二章 文獻回顧 5 2-1 鈣鈦礦太陽能電池的發展歷程 5 2-2 鈣鈦礦太陽能電池的材料特性、工作原理與發展歷程 8 2-2-1 鈣鈦礦太陽能電池的半導體特性 8 2-2-2 鈣鈦礦太陽能電池的工作原理 17 2-2-3 鈣鈦礦太陽能電池元件結構 19 2-2-4 鈣鈦礦薄膜的製備方法 21 2-2-5 優化FA型鈣鈦礦太陽能電池的策略 24 2-2-5-1路易士鹼(Lewis Base)添加劑 25 2-2-5-2氯化物添加劑 26 2-2-5-3低維度鈣鈦礦 32 第三章 實驗方法與儀器分析 35 3-1 實驗藥品與材料 35 3-2 實驗步驟與方法 37 3-2-1 化學蝕刻(Chemical Etching) 38 3-2-2 二氧化鈦緻密層(Compact TiO2 Layer) 39 3-2-3 二氧化鈦多孔層(Mesoporous TiO2 Layer) 40 3-2-4 鈣鈦礦主動層(Perovskite Active Layer)與表面鈍化 42 3-2-5 Spiro-OMeTAD層(Spiro-OMeTAD Layer) 44 3-2-6 銀背電極 45 3-3 實驗儀器 45 3-3-1 氣氛控制手套箱(Purified Gas Glove Box) 45 3-3-2 旋轉塗佈儀(Spin Coater) 47 3-3-3 熱蒸鍍機(Thermal Evaporator) 48 3-3-4 高解析掃描式電子顯微鏡(SEM)與能量色散X射線光譜儀(EDS) 52 3-3-5 X射線繞射儀 (X-ray Diffraction, XRD) 54 3-3-6 X射線光電子光譜儀(XPS)與紫外光電子能譜儀(UPS) 55 3-3-7 螢光光譜(PL)與時間解析螢光光譜(TRPL) 56 3-3-8 太陽光模擬器(Solar Simulator)與電流密度-電壓曲線 57 3-3-9 入射光子轉換效率量測系統(Incident Photon to Charge Carrier Efficiency, IPCE) 61 第四章 結果與討論 63 4-1 FAPbI3鈣鈦礦太陽能電池基礎參數調控 63 4-1-1 優化鈣鈦礦薄膜的熱處理程序 64 4-1-2 探討熱處理程序對鈣鈦礦薄膜表面形貌的影響 70 4-1-3 能量色散X射線光譜儀分析(EDS) 74 4-1-4 經不同加熱程序處理的鈣鈦礦薄膜之PL和TRPL分析 75 4-1-5 鈣鈦礦太陽能電池的光伏性質整理與穩定性測試 80 4-1-6 反溶劑體積的最佳化 84 4-2 甲胺鹽酸鹽(MACl)作為鈣鈦礦薄膜的表面修飾劑 88 4-2-1 元素與鍵結分析(XPS) 88 4-2-2 鈣鈦礦的晶貌(Morphology)分析 90 4-2-3 鈣鈦礦薄膜之PL和TRPL分析 92 4-2-4 鈣鈦礦太陽能電池的光伏性質 95 4-2-5 鈣鈦礦太陽能電池的半導體性質 100 4-2-6 鈣鈦礦太陽能電池的穩定性測試(Stability test) 105 第五章 結論 107 5-1 FAPbI3鈣鈦礦太陽能電池基礎參數調控 107 5-2 甲胺鹽酸鹽(MACl)作為鈣鈦礦薄膜的表面鈍化劑 108 5-3 未來工作與建議 110 第六章 參考文獻 111 附錄 114

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