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研究生： 葉宏祥
Yeh, Hung-Hsiang
論文名稱： 低壓氣相溶液輔助高效率2D/3D鈣鈦礦太陽能電池
High efficiency 2D/3D perovskite solar cell by Low-Pressure Vapor-Assisted Solution Process
指導教授： 陳昭宇
Chen, Chao-Yu
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： 2017
畢業學年度： 105
語文別： 中文
論文頁數： 88
中文關鍵詞： 鈣鈦礦太陽能電池 、苯乙基碘化銨 、低壓氣相沉積 、2D/3D鈣鈦礦 、穩定性
外文關鍵詞： Perovskite solar cell, PEAI (Phenylethylammonium iodide), Low-Pressure Vapor-Assisted Solution Process, 2D/3D Perovskite solar cell, Stability
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    • 鈣鈦礦太陽能電池的光電轉換效率發展迅速，使再生能源的研究展露出一道曙光。 因此為了達到商業化生產，除了優異的光電轉換效率之外，電池的長時間工作穩定性以及大面積元件的表現都是重要的關鍵，因此本篇論文的研究動機為提升鈣鈦礦太陽能電池的穩定性。
    本篇論文的研究主要探討添加不同比例的有機材料PEAI(Phenylethylammonium iodide)對於其合成的鈣鈦礦太陽能電池元件長時間穩定性的影響。鈣鈦礦吸光層的製備是藉由低壓氣相沉積法氣化MAI (Methylamine iodide)粉末與PEAI/PbI2混合旋塗沈積的薄膜進行氣固反應，調變反應時間、溫度以及壓力條件得到優化後的鈣鈦礦薄膜。使用氣相沉積法所形成的鈣鈦礦薄膜具有晶粒較大以及均勻性較佳的優點，而添加微量的PEAI則有助於晶體的成核以及成長，減少缺陷以及漏電流的產生。利用吸收圖譜(UV-vis)、受激螢光放光(Photoluminescence)以及GIWAXS (Grazing-Incidence Wide-Angle X-ray Scattering)等光學儀器分析添加PEAI後形成的鈣鈦礦薄膜其結構以及光學性質的變化。在添加高濃度的PEAI發現，元件的效率並無明顯的差異，因此發現MA+和PEA+在反應的過程中會相互的競爭，在長時間的反應，MA+能逐漸取代PEA+使電性以及結構發生改變。結果顯示適量的添加PEAI後，其鈣鈦礦元件在電壓以及電流的數據都有顯著的提升，最佳的元件效率能達到19.1%。而在穩定性表現方面，封裝後的元件(無光照條件下)在將近一千小時的測試都能維持原先的效率，此結果也證明PEAI的添加對於鈣鈦礦元件的長時間穩定性的助益。

    In this study, the formation of layered 2D structure perovskites which have been proved to be highly stable structure is performed by vapor deposition with larger organic cation iodide, phenylethylammonium (PEAI, C8H9NH3I). We mix lead iodide (PbI2) and PEAI in the dimethylformamide (DMF) solvent and react with methylammonium iodide (MAI) vapor in the low pressure heating oven. The number of the perovskite layers have been varied (n) from n = 1 through n = ∞ in the series of (PEA)2(MA)n-1PbnI3n+1. The stoichiometry of PEAI in perovskite has impact on the photoluminescence (PL) intensity and the bandgap. The scanning electron microscope images show that the PEAI-containing perovskite film has more uniform morphology and larger grain size than that of MAPbI3. The device employing PEA2(MA)39Pb40I121 (n=40) achieves a champion power conversion efficiency (PCE) of 19.10 % with a open-circuit voltage (VOC) of 1.084 V, current density (Jsc) of 21.91mA/cm2 and fill factor (FF) of 80.36%.

    摘要 P.I Extended Abstract P.II 致謝 P.X 目錄 P.XI 表目錄 P.XIV 圖目錄 P.XV 第一章 緒論 P.1 1.1 前言 P.1 1.2 太陽能電池的演進以及發展 P.1 1.2.1第一世代太陽能電池 P.2 1.2.2第二世代太陽能電池 P.3 1.2.3第三世代太陽能電池 P.3 1.3 太陽能電池的基本原理 P.5 1.3.1半導體的能帶 P.5 1.3.2 PN接面 P.7 1.3.3太陽光對於太陽能電池之影響 P.8 1.3.4太陽能電池的量測參數 P.10 1.4研究動機 P.13 第二章 文獻回顧 P.14 2.1有機無機混成鈣鈦礦發展 P.14 2.2 氣相沉積鈣鈦礦 P.18 2.2.1共蒸鍍(Dual-source thermal evaporation) P.18 2.2.2 Sequential Vacuum Deposition P.21 2.2.3蒸氣輔助之溶液製程(Vapor-Assisted Solution Process, VASP) P.22 2.2.4化學氣相沉積(Chemical Vapor Deposition, CVD) P.23 2.2.5 低壓化學氣相沉積(Low Pressure Hybrid Chemical Vapor Deposition) P.24 2.3 主動層鈣鈦礦的結構 P.26 2.3.1多元混和鈣鈦礦 P.26 2.3.2二維鈣鈦礦 P.29 第三章 實驗方法與儀器分析 P.36 3.1 實驗儀器與藥品 P.36 3.2 實驗流程 P.38 3.3鈣鈦礦電池元件製作 P.39 3.3.1 基板製備 P.39 3.3.2阻擋層(Compact layer TiO2)製備 P.39 3.3.3 TiO2多孔層 P.39 3.3.4 TiCl4後處理 P.39 3.3.5低壓氣相沉積鈣鈦礦薄膜 P.39 3.3.6電動傳輸層(Spiro-OMeTAD) P.40 3.3.7電極製備 P.40 3.4薄膜製程工作原理 P.41 3.4.1真空加熱爐 P.41 3.5樣品分析 P.42 3.5.1 I-V特性曲線量測分析 P.42 3.5.2 量子轉換效率 P.42 3.5.3 吸收光譜量測(UV-vis) P.43 3.5.4 光致螢光激發(Photoluminescene,PL) P.43 3.5.5掃描式電子顯微鏡(Scanning Electron Microscopic,SEM) P.43 3.5.6 X光繞射分析(X-Ray Diffration,XRD) P.44 3.5.7 傅立葉轉換紅外光光譜分析(Fourier Transform Infrared Spectrometer,FTIR) P.45 3.5.8 低掠角大角度X光散射分析(Grazing-Incidence Wide-Angle X-ray Scattering, GIWAXS) P.46 第四章 結果與討論 P.47 4.1 MAPbI3鈣鈦礦 P.47 4.2 不同濃度的PEAI對鈣鈦礦的影響 P.49 4.2.1不同比例的PEAI的薄膜分析:XRD P.49 4.2.2不同比例的PEAI的薄膜分析:FTIR P.51 4.2.3不同比例的PEAI的薄膜分析:UV-vis、PL P.53 4.2.4不同比例的PEAI的薄膜分析:GIWAXS P.55 4.2.5不同比例的PEAI的薄膜分析:SEM P.57 4.2.6 n=1(PEA)2PbI4薄膜分析:TEM P.61 4.2.7不同比例的PEAI元件表現 P.62 4.3改變n=40的反應溫度 P.65 4.4改變n=40的反應時間 P.68 4.5改變n=40的溶液濃度 P.72 4-6探討氣相過程結構的變化 P.75 4-7穩定性測試 P.79 4.7.1未封裝電池在未照光環境的穩定性測試 P.79 4.7.2封裝電池在未照光環境的穩定性測試 P.81 4.7.3封裝電池在照光下的穩定性測試 P.81 第五章 結論與未來展望 P.83

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