混合陰或陽離子之鉛鹵素鈣鈦礦的長晶研究

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姓名

徐睿謙(Jui-Chien Tsu) 查詢紙本館藏

畢業系所

化學學系

論文名稱

混合陰或陽離子之鉛鹵素鈣鈦礦的長晶研究

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摘要(中)

以鉛鹵化物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。若能合成出具有高純度之鈣鈦礦單晶，可幫助我們了解此材料之物理性質。本研究使用可快速長晶的逆溫度結晶法，搭配不同溶劑及不同比例的陽離子或鹵素混合，製備出含混合鹵素或混合陽離子之鈣鈦礦單晶。結果顯示，所長之單晶與其起始溶液中之溶質的組成不同。在含有I-/Br-之系統中，起始溶質組成為MABr : PbI2 = 1 : 1時，所長成之晶體組成為MAPbI0.78Br2.22，單晶中所含之Br比例高於起始物，可能是Br-與MA+可形成較穩定的晶格。在含有Br-/Cl-之系統中，起始溶質組成為MABr : PbCl2 = 1 : 1時，所成長之晶體組成為MAPbCl2.77Br0.23。而在起始溶質為MACl : PbBr2 = 1 : 1時，所得晶體組成則為MAPbCl1.35Br1.65，晶體中Cl-之比例皆較其起始溶質之比例高，推測因溶解度較小之氯化物在長晶過程中較快沉澱出來。在含Cs+與MA+或FA+之混摻陽離子系統中，以0.24 M CsI + 0.65 M MAI + 0.89 M PbBr2或是0.22 M CsI + 0.71 M FAI + 0.93 M PbBr2為起始物時，所長出之晶體經EDS測量得到之組成分別為CsPbI0.05Br2.95以及CsPbI0.15Br2.85，因Cs+與Br-離子半徑之比率有利於形成純Cs陽離子之鈣鈦礦結構。

摘要(英)

Perovskite solar cell (PSC) based on lead halide perovskite has attract highly attention due to its high power conversion efficiency. Being able to prepare perovskite single crystal with high purity will help us to understand the physical properties of these materials. In this study, we use inverse temperature crystallization method to grow perovskite single crystal with various stoichiometries by using different solvents, various cations and halides. It was found that the compositions of the crystals and the solutes in the precursor solution are different. The composition of crystal grown from 1.3 M MABr + 1.3 M PbI2/DMF : GBL = 2 : 1 solution is MAPbI0.78Br2.22, the bromide ratio in crystal is higher than that in solute, indicating that bromide ion is more suitable to form bromide perovskite structure. Crystal grown from 1.0 M MABr + 1.0 M PbCl2/DMF : DMSO = 2 : 1 is MAPbCl2.77Br0.23, from 0.8 M MACl + 0.8 M PbBr2 /DMF : DMSO = 9 : 1 is MAPbCl1.35Br1.65. Both results show that the chloride content in the crystal is higher than that in the solute, probably due to Cl- ion containing perovskite has lower solubility. In mixed cation cases when the precursor solutions are 0.24 M CsI + 0.65 M MAI + 0.89 M PbBr2/DMF : GBL : DMSO =14 : 7 : 5 and 0.22 M CsI + 0.71 M FAI + 0.93 M PbBr2/DMF : GBL : DMSO = 8 : 12 : 8, the compositions of the resulting crystals estimated from EDS analysis are CsPbI0.05Br2.95 and CsPbI0.15Br2.85, respectively. Probably due to the radium ratio of Cs+ and Br- is proper to form perovskite structure.

關鍵字(中)

★ 鈣鈦礦結構
★ 單晶
★ 混合鹵素

關鍵字(英)

★ Perovskite structure
★ single crystal
★ mix halide

論文目次

中文摘要I
英文摘要II
謝誌IV
目錄V
圖目錄VIII
表目錄XIV
第一章緒論 1
1-1 前言 1
1-2 鈣鈦礦結構 1
1-3 鈣鈦礦單晶 2
1-4 大尺寸鈣鈦礦單晶的製備方法 8
1-5 混合鹵素之鈣鈦礦單晶 12
1-6 研究動機 18
第二章實驗 19
2-1 實驗藥品 19
2-2 起始物的合成 20
2-2-1 合成甲基碘化銨 20
2-2-2 合成甲基溴化銨 20
2-2-3 合成甲基氯化銨 21
2-2-4 合成甲脒氫碘酸鹽 21
2-3 長晶溶液配置 21
2-3-1 含單一鹵素之長晶溶液配置 21
2-3-2 混合鹵素鈣鈦礦之長晶溶液配置 22
2-3-2-1 MAPbIxBr3-x長晶溶液的配置 22
2-3-2-2 MAPbClxBr3-x長晶溶液的配置 24
2-3-3 混合陽離子之長晶溶液配置 25
2-3-4 同時混合陰陽離子之長晶溶液配置 26
2-4 實驗儀器 27
2-4-1 紫外-可見光-近紅外光分光光譜儀(UV-Vis-IR
Spectophotometer, HITACHI U-4100) 27
2-4-2 螢光光譜儀(Fluorescence Spectrometer, HITACHI F-7000) 28
2-4-3 顯微拉曼螢光光譜儀(Micro-Raman / PL Spectrometer,
UniRAM) 29
2-4-4 X光繞射儀(X-Ray Diffraction, Bruker D8 Discover) 30
2-4-5 掃描式電子顯微鏡(Scanning Electron Microscope,
HITACHI S-800)與能量色散X-射線光譜(Energy
Dispersive Spectrometer) 32
第三章結果與討論 34
3-1 含單一鹵素之鈣鈦礦單晶的製備 34
3-2 混合鹵素之鈣鈦礦單晶 37
3-2-1 混合鹵素之鈣鈦礦單晶的製備 37
3-2-1-1 MAPbIxBr3-x單晶的製備與性質探討 37
3-2-1-2 FAPbIxBr3-x單晶的製備與性質探討 44
3-2-1-3 MAPbBrxCl3-x單晶的製備與性質探討 45
3-2-1-4 MAPbIxCl3-x單晶的製備 52
3-2-2 改變起始物組成對單晶組成之影響 53
3-2-3 起始物之組成與由其所旋轉塗佈之膜的組成間之差異 59
3-3 混合陽離子鈣鈦礦單晶的製備 61
第四章結論 68
第五章參考文獻 69
附圖 74

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指導教授

吳春桂(Chun-Guey Wu)

審核日期

2017-8-17

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