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姓名	郭喬育(Chiao-Yu Kuo)  查詢紙本館藏	畢業系所	化學學系
論文名稱	有機陽離子之鉛鹵素鈣鈦礦長晶研究
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摘要(中)	以鉛鹵素鈣鈦礦做為主動層之鈣鈦礦太陽能電池(Perovskite solar cell, PSC) ，因其高的光電轉換效率獲得大家高度的重視。而為了瞭解應用於太陽能電池之鈣鈦礦的物理性質，科學家們合成出各種組成的鈣鈦礦單晶進行研究。本研究以能夠快速長晶的逆溫長晶法，用GBL或GBL與DMF的混合溶液作為溶劑，搭配不同比例的陽離子、鉛與鹵素混合成長晶母液，在不同加熱溫度下成長出不同組成之混陰陽離子鉛鈣鈦礦單晶。研究結果顯示， 以MA(0.93-x)FAxCs0.07PbI3母液所長出一系列單晶的晶體內沒有Cs離子的存在，並且其最大放光波長略低於MAxFA(1-x) PbI3母液所長出單晶的最大放光波長。當長晶母液中鈣鈦礦的劑量為MAxFA(1-x)PbBr1.5I1.5時，溶液中FA比例增加時所長出晶體中的FA比例同樣增加，而溴離子則隨之減少。從劑量為MA0.5FA0.5PbBraI(3-a)長晶母液中所製備之單晶，當母液中之碘離子占鹵素離子的比例大於60%時，晶體中碘離子的比例會大幅增加，晶體形狀也從cubic逐漸變為tetragonal，而晶體放光波長也隨著晶體中碘離子比例增加而變長。以含MA(1-y)CsyPbBr0.6I2.4長晶母液所製備之單晶以能量色散X-射線譜(Energy Dispersive Spectrometer, EDS)所測得之晶體中各個原子之含量，顯示當母液中Cs離子為2%時得到的晶體中並沒有Cs離子，而母液中Cs離子為5%時得到的晶體中Cs離子也只占了0.4%，但當母液中Cs離子為7%時得到的晶體中Cs離子含量迅速增加至8%。
摘要(英)	Abstract Perovskite solar cells (PSCS) based on lead-halide perovskite absorber have attracted great attention due to their high power conversion efficiency and non-expensive solution fabrication processes. To be understand better the instrinic properties of lead-halide perovskite, single crystals were prepared and studied. In this study, inverse temperature crystallization method was used to grow perovskite with various components. GBL or the mixture of GBL and DMF was used as solvents to dissolve several starting materials with various mole ratios to form a mother solutions for single crystals. We found that even the mother solution contains MA(0.93-x), FAx, Cs0.07, Pb, and l3 but the single crystal grown from it did not have Cs+ ion. Furthermore, the λEM of the PL is shorter than that of the crystal from from MaxFA(1-x)PbBr3-xIx. The FA content for the crystal increase as the FA in the mother solution increases and Br ion in the crystal decreases. For the mother solution containing MA05FA05PbBr(3-a)Ia, the I- content increase sharply when I/Br ratio is higher than 1.5, at the same time the morphology of the crystal change from cubic to tetragonal and the λEM of the PL shifts to longer wavelength. For the mother solution with the content of MA(1-x)CsxPbBr0.6I2.4, when the Cs/MA is less than 2%, the crystal grown from it contains no Cs as revealed with EDS analysis. Increasing the Cs content in the mother solution to 5%, the Cs content in the crystal increases to 0.4%, nevertheless, when the Cs in the mother solution increases to 7%, the Cs in crystal increases rapidly to 8%.
關鍵字(中)	★ 鉛鹵素鈣鈦礦 ★ 長晶	關鍵字(英)
論文目次	摘要 I Abstract II 摘要圖 III 謝誌 IV 目錄 V 圖目錄 VIII 表目錄 XII 附圖目錄 XIV 壹、 序論 1 1-1、 前言 1 1-2、 鈣鈦礦的結構 1 1-3、 鈣鈦礦太陽能電池主動層主要成分 2 1-4、 鈣鈦礦單晶 4 1-5、 混合鹵素與混合陽離子之鈣鈦礦單晶 8 1-6、 本實驗室先前的長晶研究 15 1-7、 研究動機 19 貳、 實驗 20 2-1、 實驗藥品 20 2-2、 儀器分析與樣品製備 20 2-2-1、 核磁共振光譜儀(Nuclear Magnetic Resonance)儀器型號：Bruker 300 & Bruker 500 20 2-2-2、 紫外光/可見光吸收光譜儀(UV/Vis Spectrometer)儀器型號：Cary 300 Bio 21 2-2-3、 顯微拉曼螢光光譜儀(Micro-Raman/PL Spectrometer, UniRAM) 21 2-2-4、 X光繞射儀(X-Ray Diffraction, Bruker D8 Discover) 22 2-2-5、 掃描電子顯微鏡(Scanning Electron Microscope, HITACHI S-800)與能量色散X-射線光譜(Energy Dispersive Spectrometer) 22 2-3、 實驗步驟 24 2-3-1、 起始物的合成 24 1. 甲基碘化銨 24 2. 甲脒氫碘酸鹽 24 2-3-2、 長晶條件 25 1. 混陽離子Fa(1-x) MAxPbI3之鈣鈦礦晶體的製備 25 2. 混陽離子FAxMA(0.93-x)Cs0.07PbI3之鈣鈦礦晶體的製備 26 3. 混陰陽離子FaxMA(1-x)PbI1.5Br1.5之鈣鈦礦晶體的製備 27 4. 混陰陽離子Fa0.5MA0.5I(3-a)Bra之鈣鈦礦晶體的製備 28 5. 混陰陽離子MA(1-x)CsxPbBr0.6I2.4之鈣鈦礦晶體的製備 29 參、 結果與討論 30 3-1、 混陽離子之鈣鈦礦晶體的製備 30 3-1-1、 混陽離子FA(1-x)MAxPbI3之鈣鈦礦晶體的製備 30 3-1-2、 混陽離子FAxMA(0.93-x)Cs0.07PbI3之鈣鈦礦晶體的製備 36 3-2、 混陰陽離子之鈣鈦礦晶體的製備 41 3-2-1、 FAxMA(1-x)PbI1.5Br1.5單晶的製備 41 3-2-2、 FA0.5MA0.5PbI(3-a)Bra單晶的製備 50 3-2-3、 MA(1-x)CsxPbBr0.6I2.4單晶的製備 60 肆、 結論 65 伍、 參考文獻 66 附錄 73 附錄 1、tolerance factor計算 73 附錄 2、1H-NMR圖譜 74 附錄 3、螢光光譜圖 83 附錄 4、UV-vis吸收光譜圖 92 附錄 5、能量色散X-射線譜 99
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指導教授	吳春桂	審核日期	2019-10-16
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