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研究生:藍振倫
研究生(外文):Chen-LunLan
論文名稱:利用甲脒為陽離子以提升低能隙鈣鈦礦太陽能電池之穩定性
論文名稱(外文):Stability Improvement of Low-bandgap Perovskite Solar Cell Using Formamidinium as Cation
指導教授:許渭州
指導教授(外文):Wei-Chou Hsu
學位類別:碩士
校院名稱:國立成功大學
系所名稱:微電子工程研究所
學門:工程學門
學類:電資工程學類
論文種類:學術論文
論文出版年:2018
畢業學年度:106
語文別:英文
論文頁數:66
中文關鍵詞:鈣鈦礦太陽能電池高穩定錫替換低能隙
外文關鍵詞:Perovskite solar cellhigh stabilitytin substitutionlow band gap
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本論文中,為了增加鈣鈦礦太陽能電池之穩定度,捨棄傳統鈣鈦礦太陽能電池常使用之陽離子甲基胺,而使用結晶所需溫度較高之陽離子甲脒,由於以甲脒為陽離子之鈣鈦礦其結晶溫度較高,提供鈣鈦礦較高之鍵結能,進而增加鈣鈦礦太陽能電池對於水氧環境的抵抗能力,達到增強元件之可靠度的目的。使用甲脒作為陽離子更使鈣鈦礦更能達到低能隙之效果,希望利用此特性用以製作串聯是太陽能電池之低能隙部分。然而由於甲脒之半徑過大,導致無法形成良好鈣鈦礦結晶,會形成額外六方晶體,因此在前驅物中加入些許半徑較小之甲基胺以減少半徑,藉此穩定鈣鈦礦之結構。此外,為進一步提升鈣鈦礦太陽能電池之穩定性及效率,本論文於前驅物中加入少量硫氰化鉛,藉由硫氰化鉛的加入可以增加鈣鈦礦之結晶大小以及結晶品質,並且於結果中顯示,硫氰化鉛並不會影響鈣鈦礦的組成。最後,為達到環境的永續性,減少鈣鈦礦太陽能電池中鉛之含量,本論文使用錫取代鉛的含量,希望藉由二原子組成相近的特性製作出不破壞鈣鈦礦結構ABX3的太陽能電池,並且藉由錫的取代鉛可以獲得更低能隙之鈣鈦礦太陽能電池,而其中以37.5%錫取代鉛是最好的比例,並表現在所有錫取代中擁有最高的效率。藉由使用FA作為陽離子並輔以錫取代鉛製作出超低能隙之鈣鈦礦太陽能電池可為未來製作串聯式太陽能電池奠定良好基石。
In this thesis, in order to improve the stability of the perovskite solar cells, we substituted original cation of typical perovskite solar cells, Methylammonium (MA) with Formamidinium (FA). Because of the higher crystallization temperature of FA perovskite solar cells, we assumed that the binding energy of FA perovskite solar cells was higher than MA perovskite solar cells, enhancing the resistance of oxide and moisture, and finally enlarging its stability. Moreover, using formamidinium as the cation can reduce the bandgap of the perovskite solar cells, which means its absorption edge shifts to longer wavelength. We can apply this type of solar cells on tandem-structure perovskite solar cells, since it can absorb near-IR wavelength light of sunlight. In addition, so as to enhance its stability further, we used lead thiocyanate (Pb(SCN)2) as additive, which can enlarge grain size and crystallinity of perovskite phase. For FA-based perovskite solar cell has a tolerance factor larger than 1, it’s difficult to form high quality black phase FAPbI3 and easy to become yellow phase, an unfavorable phase for perovskite solar cells. Therefore, adding small amount of methylammonium and lead thiocyanate can restrain perovskite from forming yellow phase and it can be confirmed by X-ray diffraction measurement. Meanwhile, since tin and lead have similar atomic arrangement, we applied tin as replacement to reduce the content of lead in perovskite solar cells with a view to being less toxicity. We partially substituted lead with tin content of 12.5%, 25%, 37.5% in this work and we observed the more tin we substituted, the lower bandgap it became. Moreover, 37.5% tin substitution provides the best alternative because of the highest efficiency and tin percentage. In the end of this thesis, we successfully improved the stability of perovskite material by using formamidinium as cation and adding lead thiocyanate in perovskite layer. Formamidinium and partially tin substitution based perovskite solar cells lead to a red shift of optical absorbance compared to methylammonium and pure lead based solar cells and we hope we can apply this type of perovskite solar cells on tandem-structure solar cells.
摘 要 I
Abstract II
誌謝 IV
Content VI
Table Captions IX
Figure Captions X
Chapter 1 Introduction 1
1-1 Background 1
1-2 Perovskite 3
1-3 Motivation 4
1-4 Organization of thesis 8
Chapter 2 Operation Principle 9
2-1 Solar Spectrum 9
2-2 Mechanism of Perovskite Solar Cell 10
2-3 Solar Cell Characteristics 11
2-3-1 I-V curve 11
2-3-2 Open-Circuit Voltage (Voc) 11
2-3-3 Short-Circuit Current (Isc) 12
2-3-4 Fill Factor (FF) 12
2-3-5 Power Conversion Efficiency (PCE) 13
Chapter 3 Experiment 14
3-1 Device Structure 14
3-2 Materials Preparation 16
3-3 Process for Device Fabrication 18
3-3-1 Pre-Cleaning ITO Substrate 18
3-3-2 UV Ozone Treatment of ITO Surface 18
3-3-3 Fabrication of Hole Transport Layer 19
3-3-4 Fabrication of Active Layer 19
3-3-5 Fabrication of Electron Transport Layer and Hole Blocking Layer 21
3-3-6 Fabrication of Hole Blocking Layer and Cathode 21
3-4 Measurements 22
3-4-1 Current-Voltage Measurement System 22
3-4-2 Atomic Force Microscope 22
3-4-3 Scanning Electron Microscope 23
3-4-4 UV-Vis-NIR Absorption spectrum 23
3-4-5 X-ray Diffraction 24
3-4-6 X-ray Photoelectron Spectroscopy 25
Chapter 4 Results and Discussions 26
4-1 Comparison Between MAPbI3 and FAPbI3 and Its Derivatives 26
4-1-1 Stability Testing 26
4-1-2 Absorption Spectrum 28
4-1-3 Scanning Electron Microscope 29
4-1-4 X-ray Diffraction 30
4-1-5 Atomic Force Microscope 32
4-2 Pb-Sn Binary Formamidinium Perovskite 33
4-2-1 Variation of Annealing Temperature 33
4-2-2 Performance of Tin-substitution Perovskite Devices 36
4-2-3 Absorption Spectrum 38
4-2-4 Scanning Electron Microscope 39
4-2-5 X-ray Diffraction 40
4-2-6 Atomic Force Microscope 41
4-2-7 X-ray Photoelectron Spectroscopy 42
Chapter 5 Conclusion 43
Reference 44
Figure 50
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