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研究生： 李偉弘
Lee, Wei-Hung
論文名稱： 用於真空蒸鍍鈣鈦礦光伏元件之電荷傳輸與界面層
Carrier Transporting and Interfacial Layers for Vacuum Deposited Perovskite Photovoltaics
指導教授： 林皓武
Lin, Hao-Wu
口試委員: 朱治偉
Chu, Chih-Wei
周鶴修
Chou, Ho-Hsiu
張志宇
Chang, Chih-Yu
陳昭宇
Chen, Chao-Yu
學位類別： 碩士
Master
系所名稱： 工學院 - 材料科學工程學系
Materials Science and Engineering
論文出版年： 2017
畢業學年度： 105
語文別： 中文
論文頁數： 90
中文關鍵詞： 鈣鈦礦光伏元件 、傳輸層 、界面層
外文關鍵詞： Peroskitephotovoltaics, Transporting, Interfacial
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    • 本論文研究在順序型真空製備的鈣鈦礦太陽能電池的基礎下，對傳輸層進行改良，包括不同電洞傳輸層的搭配，電子界面層的應用，以及對鈣鈦礦的組成進行調整，製備成元件後最高能量轉換效率可達到18.8%。
    第一章，簡介太陽能電池的發展歷史，並且概述有機金屬鈣鈦礦太陽能電池的研究發展與現況。第二章，概述有機金屬鈣鈦礦太陽能電池之工作原理、光電特性，以及有機材料的準備與分析和元件的製備與量測方法。
    第三章，我們使用不同電洞傳輸層如poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS)、N,N′-di(1-naphthyl)-N,N′-diphenyl-(1,1′-biphenyl)-4,4′-diamine (NPB)、Tris[4-(5-phenylthiophen-2-yl)phenyl]amine (TPTPA)和Poly[N,N′-bis(4-butylphenyl)-N,N′-bisphenylbenzidine] (Poly-TPD)，與順序型真空製備鈣鈦礦薄膜搭配並做成元件，探討各種電洞傳輸層對元件效率的影響。其中，以TPTPA做為電洞傳輸層之元件具有最佳表現，其短路電流為22.1 mA/cm2，開路電壓為1.06 V，填充因子為0.71，能量轉換效率達16.7%。我們也將相同元件放在室內中，以室內照明常見的T5螢光燈管為量測光源，量測不同室內光強度下其效率參數。元件於1000 lux時元件的工作電壓為0.73 V，工作電流密度為146 μA/cm2，功率密度為99.0 μW/cm2，能量轉換效率為31.4%，且具有優異的元件穩定度。
    第四章，我們以上述TPTPA的應用做為基礎，引入有機小分子如 1,3,5-Tri(m-pyridin-3-ylphenyl)benzene (TmPyPB)、 4,6-Bis(3,5-di(pyridin-4-yl)phenyl)-2-methylpyrimidine (B4PyMPM) 、 Tris(2,4,6-trimethyl-3-(pyridin-3-yl)phenyl)borane (3TPYMB) 、 1,4,5,8-Naphthalenetetracarboxylic dianhydride (NTCDA) 和 Bathophenanthroline (Bphen) 做為電子界面層，透過分析儀器來探討其效率增益的機制。我們發現到若小分子具有吡啶 (pyridine) 基團如 TmPyPB、B4PyMPM 和3TPYMB，則可以增加元件效率，其中以3TPYMB做為電子界面層之元件具有最佳表現，其短路電流為22.7 mA/cm2，開路電壓為1.07 V，填充因子為0.77，效率達18.8%。若使用不具吡啶基團的分子如NTCDA和Bphen，則有負面的影響而造成元件效率下降。
    第五章，我們調變鈣鈦礦主動層的組成，以PbI2和PbCl2莫耳比1:1共蒸鍍膜層進行順序型真空製程反應成鈣鈦礦薄膜並製備成元件，此外也探討退火時間長短對元件效率的影響，以退火溫度攝氏100度加熱3分鐘的元件表現最好，其短路電流為22.7 mA/cm2，開路電壓為1.04 V，填充因子為0.71，效率達16.6%。
    最後，將綜合所有數據研究做個總結論，提供未來學者研究之參考依據。

    In this thesis, we focus on the modification of transporting layers, such as utilization of various hole transporting layers (HTLs), applications of electron interfacial layers (EILs), and adjustment of the composition of the perovskites.
    In the first part of this thesis, we briefly review the development of photovoltaics and organometallic perovskite solar cells.
    　　In the second part of thesis, we explicate the operation principle and characteristics of organometallic perovskite solar cells.
    In the third part, different HTLs used in organometallic perovskite solar cells were studied. The device with tris[4-(5-phenylthiophen-2-yl)phenyl]amine) (TPTPA) as HTL exhibited the highest power conversion efficiency (PCE) of 16.7% with a short circuit current density (Jsc) of 22.1 mA/cm2, an open circuit voltage (Voc) of 1.06 V and a fill factor (F.F.) of 0.71. Additionally, the device was also measured under 6500 K color temperature Philips T5 fluorescent lamp illumination. The device exhibited a PCE of 31.4% with a maximum power point current density (JMPP) of 146 μA/cm2, a maximum power point voltage (VMPP) of 0.73 V and maximum power density of 99.0 μW/cm2, corresponding to a PCE up to 31.4%.
    　　In the fourth part, we demonstrate that the performance of perovskite solar cells can be boosted with sub-nm pyridine-containing small-molecule EILs such as TmPyPB, B4PyMPM and 3TPYMB. These vacuum-deposited sub-nm layers between perovskites and electron transport layers create a permanent dipole moment that improves the interfacial energy level alignment and facilitates a fast electron sweep-out. With 3TPYMB used as interfacial layer, the device exhibited a PCE of 18.8% with a Jsc of 22.1 mA/cm2, a Voc of 1.07 V and a F.F. of 0.77. However, as we utilized the non-pyridine-containing small-molecule EILs such as NTCDA or Bphen, it would have a poor effect on the performance of the devices. The device with Bphen as EIL exhibited a poor PCE of 9.31% compared with reference cell of 16.7%
    In the fifth part, the composition of perovskite active layers was studied. Lead chloride (PbCl2) and lead iodide (PbI2) were co-evaporated and reacted with Methylammonium iodide (MAI) for transforming into the perovskites (MAPbI3-xClx). By tuning the appropriate post-annealing time, the device exhibited a PCE of 16.6% with a Jsc of 22.68 mA/cm2, a Voc of 1.04 V and a F.F. of 0.71.
    Finally, a brief summary of this study is presented with some guidelines for the related future studies.

    中文摘要 I Abstract III 目錄 V 圖目錄 VIII 表目錄 XII Chapter1 序論 1 1-1 前言 1 1-2 太陽能電池發展簡介 2 1-2.1 第一代太陽能電池 3 1-2.2 第二代太陽能電池 3 1-2.3 第三代太陽能電池 4 1-3 染料敏化太陽能電池發展 4 1-4 有機薄膜太陽能電池發展 5 1-5 有機金屬鈣鈦礦太陽能電池發展 5 1-6 論文結構 9 Chapter 2 有機金屬鈣鈦礦太陽能電池之工作原理與特性量測 10 2-1　簡介 10 2-2 太陽光光譜 10 2-3 有機金屬鈣鈦礦太陽能電池之工作原理 12 2-4 有機金屬鈣鈦礦太陽能電池之光電特性 13 2-4.1　光電轉換效率 (power conversion efficiency, PCE)： 13 2-4.2　開路電壓 (open circuit voltage, Voc)： 13 2-4.3　短路電流密度 (short circuit current density, Jsc)： 13 2-4.4　填充因子 (fill factor, FF)： 14 2-4.5　外部量子效率 (external quantum efficiency,E.Q.E.)： 14 2-5 有機金屬鈣鈦礦太陽能電池之元件結構 16 2-5.1　依元件型態分類 16 2-5.2 依載子傳輸方向分類 16 2-6 有機金屬鈣鈦礦太陽能電池之準備與分析 17 2-6.1　有機材料的純化 17 2-6.2　光物理性質量測 17 2-6.3　元件製備方法 18 2-6.4　元件量測 19 Chapter 3 電洞傳輸層應用於有機金屬鈣鈦礦太陽能電池 21 3-1　電洞傳輸層之發展與簡介 21 3-2　導電高分子材料 PEDOT:PSS 24 3-2.1 PEDOT:PSS材料性質 24 3-2.2 使用PEDOT:PSS做為HTL製備正結構鈣鈦礦太陽能電池 24 3-3　有機小分子材料 NPB 25 3-3.1 NPB材料性質 25 3-3.2 使用NPB做為HTL製備正結構鈣鈦礦太陽能電池 25 3-4.　有機小分子材料 TPTPA 26 3-4.1　TPTPA 材料性質 26 3-4.2　使用TPTPA做為HTL製備正結構鈣鈦礦太陽能電池 26 3-4.3　使用TPTPA做為HTL，調變不同厚度的鈣鈦礦太陽能電池 27 3-5　室內光應用 28 3-5.1　前言 28 3-5.2　以TPTPA 為電洞傳輸層之元件於室內光響應 30 3-6　高分子材料 Poly-TPD 30 3-6.1　Poly-TPD材料性質 30 3-6.2　使用Poly-TPD做為HTL製備正結構鈣鈦礦太陽能電池 31 3-7　結論 33 3-8　圖表附錄 34 Chapter 4 電子界面層應 用於有機金屬鈣鈦礦太陽能電池 49 4-1　電子界面層之發展與簡介 49 4-2　電子界面層之應用 50 4-2.1　加入電子界面層製備正結構鈣鈦礦太陽能電池 50 4-2.2　元件結果與討論 50 4-3　分析儀器的量測 52 4-3.1　AFM、UPS、XPS 分析 52 4-3.2　瞬態電性量測 53 4-3.3　模擬軟體計算 54 4-4　結論 55 4-5　圖表附錄 56 Chapter 5 鈣鈦礦組成應用於有機金屬鈣鈦礦太陽能電池 69 5-1　鈣鈦礦組成之發展與簡介 69 5-2　MAPbI3-xClx 71 5-2.1　以等莫耳比的PbI2和PbCl2製備成鈣鈦礦太陽能電池 71 5-2.2　調變MAPbI3-xClx退火時間 72 5-3　結論 73 5-4　圖表附錄 74 Chapter 6 結論與未來展望 79 參考文獻 81

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