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研究生： 施璟葵
Shih, Ching-Kuei
論文名稱： 聚焦式微波合成銦鋅氧物應用於鈣鈦礦太陽能電池載子傳輸層之研究
Studies of Microwave-Assisted Synthesized Indium Zinc Oxide as Charge Extraction Layer for Perovskite Solar Cells
指導教授： 陳昭宇
Chen, Peter
學位類別： 碩士
Master
系所名稱： 理學院 - 光電科學與工程學系
Department of Photonics
論文出版年： 2016
畢業學年度： 104
語文別： 中文
論文頁數： 85
中文關鍵詞： 銦鋅氧化物 、微波合成 、鈣鈦礦太陽能電池 、溶膠凝膠法
外文關鍵詞： Idium zinc oxide, Perovskite solar cells, Microwave-Assisted, sol-gel
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    • 本論文目的是利用聚焦式微波合成加熱法製備銦鋅氧化物(Indium zinc oxide,IZO)，應用於反置型(p-i-n 異質結構) 鈣鈦礦太陽能電池(Perovskite solar cell)之研究。
    本研究中探討微波反應加熱溫度與持溫時間對合成銦鋅氧化物粒徑之變化，透過前驅物溶解溫度與反應溫度的界定，提高產物粒徑均勻性以及實驗再現性。反應溫度提升(160度、180度、210度) 與粒徑尺寸呈線性上升關係，反應持溫時間亦與粒徑尺寸呈線性上升。研究不同濃度銦摻雜於氧化鋅之結構與鍵結趨勢，由XRD 分析，主要晶格峰值隨摻雜濃度提升而寬化。以XPS 分析元素摻雜的情形，在全能譜中顯示In3d 的峰值，再由氧O1s 軌域中531.2 eV 鍵結峰值強度的增加證明In 原子透過摻雜與氧化鋅之間產生鍵結。
    以溶液製程(solution process) 搭配旋轉塗佈(spin coating) 方式將IZO 奈米顆粒應用於p-i-n 異質結構之元件。根據摻雜對元件工作表現之趨勢，以5% 摻雜之銦鋅氧化物最佳。進一步以薄膜緻密性改善降低崩潰電流的發生，厚度優化達到最高光電流，最後使最高轉換效率達9.8%，在溫度25度，濕度50% 環境下，經過100 小時穩定度測試，電壓與電流表現只有20% 的損耗。

    The rapidly boosted conversion efficiencies of perovskite solar cells (PSCs) has attracted tremendous attention, however, the poor device stability must be overcame for the future applications. The inorganic electron transport materials (ETMs) of metal oxide were employed for the p-i-n heterojunction PSCs to replace the organic ETMs and improve the device stability under ambient atmosphere. an which had high stability under atmospheric and good charge transport properties by doping. By further improving the electrical properties, indium-doped zinc oxide (IZO) nanoparticles were prepared via sol-gel microwave-assisted fabrication which was a facile, clean and time-effective
    method. The best conversion efficiency of the IZO-based device was 9.84% with an aperture area of 0.2 cm2 under one sun illuminated. The as-fabricated device exhibited decent stability with 60% of initial PCE for 100 hours.

    摘要i Extended Abstract ii 英文延伸摘要ii 誌謝viii 目錄ix 表格xi 圖片xii 第一章緒論1 1.1. 前言. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1 1.2. 太陽光譜. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 2 1.3. Shockley-Queisser 理論. . . . . . . . . . . . . . . . . . . . . . . . . . . 3 1.4. 太陽能電池總類. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 6 1.4.1. 結晶矽太陽能電池. . . . . . . . . . . . . . . . . . . . . . . . . . 6 1.4.2. 薄膜太陽能電池. . . . . . . . . . . . . . . . . . . . . . . . . . . 8 1.4.3. 有機太陽能電池. . . . . . . . . . . . . . . . . . . . . . . . . . . 8 1.4.4. 鈣鈦礦太陽能電池(Perovskite solar cell) . . . . . . . . . . . . . . 10 1.5. 實驗動機與目的. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 13 第二章文獻回顧15 2.1. 金屬氧化物. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 15 2.1.1. 氧化鋅. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 15 2.1.2. 銦鋅氧化物(Indium zinc oxide) . . . . . . . . . . . . . . . . . . . 16 2.2. 鈣鈦礦太陽能電池發展. . . . . . . . . . . . . . . . . . . . . . . . . . . 19 2.2.1. n-i-p 鈣鈦礦太陽能電池演進. . . . . . . . . . . . . . . . . . . . 19 2.2.2. p-i-n 反置型太陽能電池演進. . . . . . . . . . . . . . . . . . . . 21 2.2.3. n 型電子傳輸層. . . . . . . . . . . . . . . . . . . . . . . . . . . 24 2.3. 微波合成原理. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 27 2.3.1. 偶極矩轉動(Dipole rotation) . . . . . . . . . . . . . . . . . . . . 27 2.3.2. 離子遷移(Ionic conduction) . . . . . . . . . . . . . . . . . . . . . 28 2.4. 溶膠凝膠法. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 30 2.4.1. 膠體的定義. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 30 2.4.2. 膠體的分散以及團聚. . . . . . . . . . . . . . . . . . . . . . . . 30 2.4.3. 溶膠凝膠製成. . . . . . . . . . . . . . . . . . . . . . . . . . . . 32 第三章實驗方法及分析儀器33 3.1. 實驗藥品. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 33 3.2. 實驗儀器. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 34 3.3. 實驗設計與流程. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 34 3.3.1. 微波合成銦鋅氧化物. . . . . . . . . . . . . . . . . . . . . . . . 34 3.3.2. 鈣鈦礦電池製作. . . . . . . . . . . . . . . . . . . . . . . . . . . 36 3.4. 光學分析. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 39 3.4.1. 吸收光譜量測（Ultraviolet–visible spectroscopy，UV-Vis） . . . 39 3.4.2. 動態光散射分析. . . . . . . . . . . . . . . . . . . . . . . . . . . 40 3.5. 薄膜及粉末結構分析. . . . . . . . . . . . . . . . . . . . . . . . . . . . 41 3.5.1. 元素分析. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 42 3.5.2. 表面形貌分析. . . . . . . . . . . . . . . . . . . . . . . . . . . . 43 3.5.3. 光致發光分析. . . . . . . . . . . . . . . . . . . . . . . . . . . . 44 3.6. 太陽能電池量測. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 45 3.6.1. I-V 量測. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 45 3.6.2. IPCE 量測. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 47 第四章實驗結果與討論49 4.1. 微波合成. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 49 4.1.1. 合成溫度之選擇. . . . . . . . . . . . . . . . . . . . . . . . . . . 49 4.1.2. 不同合成溫度對銦鋅氧化物合成之影響. . . . . . . . . . . . . . 51 4.1.3. 不同合成時間對銦鋅氧化物合成之影響. . . . . . . . . . . . . . 53 4.1.4. 溶劑置換. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 55 4.2. 合成材料分析. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 56 4.2.1. 不同摻雜濃度對粒徑之影響. . . . . . . . . . . . . . . . . . . . 56 4.2.2. 不同摻雜濃度之XPS 分析. . . . . . . . . . . . . . . . . . . . . 58 4.2.3. 不同摻雜濃度之XRD 結構分析. . . . . . . . . . . . . . . . . . 60 4.2.4. IZO 薄膜特性. . . . . . . . . . . . . . . . . . . . . . . . . . . . . 62 4.3. 銦鋅氧化物應用於鈣鈦礦太陽能電池. . . . . . . . . . . . . . . . . . . 65 4.3.1. 不同摻雜濃度對元件表現之影響. . . . . . . . . . . . . . . . . . 65 4.3.2. 銦鋅氧化物薄膜之優化. . . . . . . . . . . . . . . . . . . . . . . 65 4.3.3. 金屬功函數的匹配. . . . . . . . . . . . . . . . . . . . . . . . . . 73 4.3.4. 穩定度. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 75 4.3.5. IZO 應用於新穎鈣鈦礦. . . . . . . . . . . . . . . . . . . . . . . 78 第五章結論80 5.1. 結論. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 80 5.2. 未來展望. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 81 參考文獻83

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