| 姓名 |
鄧祥鴻(Xiang-Hong Deng)
查詢紙本館藏 |
畢業系所 |
機械工程學系 |
| 論文名稱 |
利用溶劑萃取法結合綠色溶劑製備鈣鈦礦太陽能電池
(Solvent-solvent Extraction for Perovskite Solar Cells Fabricated with Green Solvent)
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| 摘要(中) |
在本論文中，我們為了能在大氣環境下製備鈣鈦礦太陽能電池元件，選擇以溶劑萃取法來製作電池元件，並以乙酸乙酯以及正庚烷這兩種高安全性且低毒性的萃取溶劑，取代一般溶劑萃取製程所使用的乙醚。希望在維持元件效率的同時也能提高製程的安全性，使鈣鈦礦太陽能電池在未來能有機會以工業大量生產。
然而單純以乙酸乙酯或是正庚烷為萃取溶劑所製作的元件有著嚴重的缺陷，因此我們將乙酸乙酯和正庚烷以一定比例混合做為萃取溶劑，利用萃取過程中溶液過飽和度的差異控制鈣鈦礦的結晶過程與表面形貌；其中以乙酸乙酯：正庚烷體積比1:1.5的混合溶劑做為萃取溶劑表現最為穩定，並且較高比例的正庚烷會使鈣鈦礦主動層的表面形貌變得粗糙，有助於增加鈣鈦礦主動層與電洞傳輸層的接觸面積，提升電洞傳輸速率，使電池元件的電流密度有所增益。
最後，做為對照組之使用乙醚做為萃取溶劑的電池元件表現最佳可達到VOC=1.06V，JSC=20.10mA/cm2，FF=75.41%，PCE=16.12%；而使用乙酸乙酯：正庚烷體積比1:1.5的混合溶劑做為萃取溶劑的電池元件表現最佳為VOC=1.06V，JSC=20.58mA/cm2，FF=73.16%，PCE=15.99%。使用乙酸乙酯與正庚烷的混合溶劑做為萃取溶劑的元件，能夠得到與乙醚萃取的元件相近的表現，且在JSC方面能有所增益。 |
| 摘要(英) |
In this study, we used solvent-solvent extraction to fabricate perovskite solar cells under atmosphere. Moreover, because the traditional extraction solvent diethyl ether is unsafe and toxic, we choose two low-toxic extraction solvent ethyl acetate and n-heptane to replace it. We not only maintained the performance of the cell with different extraction solvent but also improved the safety of the fabrication process. The fabrication process can realize the application of industry in the future.
However, the cells with ethyl acetate or n-heptane as the extraction solvent had serious instability and defects. Therefore, we mixed ethyl acetate and n-heptane as the extraction solvent. We controlled the supersaturation of the solution during the extraction to change the crystallization process and surface morphology of perovskite. We found the mixed solvent of the ratio of ethyl acetate to n-heptane is 1:1.5 having best stability as the extraction solvent. On the other hand, the rough surface morphology rough could increase interface contact between the perovskite layer and the hole transport layer raised the opportunity of transporting holes.
Finally, the cells with diethyl ether as the extraction solvent had open-circuit voltage (VOC) of 1.06V, short-circuit current density (JSC) of 20.10 mA/cm2, fill factor (FF) of 75.41%, and power conversion efficiency (PCE) of 16.12%. In contrast, the cells with the ratio of ethyl acetate to n-heptane is 1:1.5 as the extraction solvent had VOC of 1.06V, JSC of 20.58mA/cm2, FF of 73.16%, and PCE of 15.99%.All in all, the performance of the cells with mixed solvent as extraction solvent was similar to diethyl ether, and an enhancement of JSC was obtained. |
| 關鍵字(中) |
★ 鈣鈦礦
★ 溶劑萃取
★ 過飽和度
★ 表面形貌
★ 電洞傳輸 |
關鍵字(英) |
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| 論文目次 |
目錄
摘要 i
Abstract ii
誌謝 iii
目錄 iv
圖目錄 vi
表目錄 viii
第1章 緒論 1
1-1 前言 1
1-2 太陽能電池的演進 1
1-3 鈣鈦礦太陽能的原理 3
1-4 鈣鈦礦太陽能的原理 3
1-5 鈣鈦礦太陽能電池文獻回顧 4
1-5-1 鈣鈦礦太陽能電池的起源與演進 4
1-5-2 鈣鈦礦太陽能電池的製程改變相關研究 5
1-5-3 鈣鈦礦太陽能電池的材料改變相關研究 9
1-5-5 鈣鈦礦太陽能電池的表面形貌相關研究 13
1-5-6 鈣鈦礦太陽能電池的溶劑萃取製程相關研究 17
1-6 研究動機 21
第2章 實驗 22
2-1 實驗藥品與儀器 22
2-1-1 實驗藥品 22
2-1-2 實驗儀器 23
2-2 鈣鈦礦太陽能電池材料合成 24
2-3 鈣鈦礦太陽能電池製程 25
第3章 結果與討論 27
3-1材料成分分析 27
3-2鈣鈦礦主動層塗佈結果 28
3-2-1不同萃取溶劑之鈣鈦礦主動層塗佈結果 35
3-3-2混合萃取溶劑之鈣鈦礦主動層塗佈結果 35
3-3鈣鈦礦主動層之表面形貌分析 35
3-3-1 X光繞射分析 35
3-3-2電化學阻抗頻譜分析 37
3-4混合萃取溶劑應用於鈣鈦礦電池元件之結果 39
第4章 結論 45
參考文獻 46
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圖目錄
圖 1 1太陽能電池工作原理示意圖 4
圖 1 2基本鈣鈦礦結構圖 4
圖 1 3 CH3NH3PbI3與CH3NH3PbBr3的IV曲線比較 5
圖 1 4快速沉積結晶(FDC)與一步沉積法之比較圖 7
圖 1 5中間相的XRD、FTIR圖譜與生成機制示意圖 7
圖 1 6調節膜厚與鹵素元素的比例對於鈣鈦礦薄膜之透明度與顏色的變化 8
圖 1 7滴加不同溫度之溶劑的結晶過程 9
圖 1 8碳基鈣鈦礦太陽能電池之製造流程、功函數匹配與結構圖 10
圖 1 9不同溶劑做為(b)電洞傳輸層之溶劑與(c)鈣鈦礦溶液之反溶劑的研究 12
圖 1 10不同比例的正己烷/乙醚混合溶劑用於溶劑製程之比較圖 13
圖 1 11滴加非極性溶劑時鈣鈦礦薄膜的生長過程 14
圖 1 12 UFCEA結構與一般薄膜之吸光度與光捕捉效率比較 15
圖 1 13 UFCEA結構與一般薄膜之PL量測結果與載子萃取權重 15
圖 1 14利用CD?R和DVD?R在鈣鈦礦薄膜上轉印光柵結構流程圖 16
圖 1 15不同厚度的電洞傳輸層對於元件光學性能的影響比較圖 17
圖 1 16元件在不同面積下的轉換效率比較 18
圖 1 17鈣鈦礦層與TiO2阻擋層間的介面在(a)無退火處理(b)熱退火處理(c)溶劑 退火處理後的改變 20
圖 1 18溶劑萃取法結合溶劑工程之製程示意圖 20
圖 2 1鈣鈦礦太陽能電池製作流程圖 26
圖 3 1 CH3NH3I之XRD分析結果 27
圖 3 2 PbI2之XRD分析結果 28
圖 3 3 CH3NH3PbI3之XRD分析結果 28
圖 3 4過飽合度與成核方式之關係圖 30
圖 3 5不同萃取溶劑用於鈣鈦礦主動層之表面形貌與截面SEM圖 (a)乙醚(b)乙酸乙酯(c)正庚烷 32
圖 3 6不同比例的混合萃取溶劑用於鈣鈦礦主動層之表面形貌與截面SEM圖 (a)1:1(b)1:2(c)1:3(d)1:1.5 34
圖 3 7不同萃取溶劑用於鈣鈦礦主動層之流程示意圖 35
圖 3 8不同萃取溶劑用於鈣鈦礦主動層之X光繞射分析圖 36
圖 3 9不同萃取溶劑用於鈣鈦礦太陽能電池之EIS分析圖 38
圖 3 10不同萃取溶劑之電池元件VOC表現 40
圖 3 11不同萃取溶劑之電池元件JSC表現 40
圖 3 12不同萃取溶劑之電池元件FF表現 41
圖 3 13不同萃取溶劑之電池元件PCE表現 42
圖 3 14最佳元件效率比較(乙醚與乙酸乙酯：正庚烷=1:1.5) 43
圖 3 15最佳元件之外部量子效率比較(乙醚與乙酸乙酯：正庚烷=1:1.5) 43
圖 3 16最佳元件效率之正逆掃比較(乙醚) 44
圖 3 17最佳元件效率之正逆掃比較(乙酸乙酯：正庚烷=1:1.5) 44
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表目錄
表 3 1各溶劑之溶解度參數與氫鍵傾向表 29
表 3 2不同萃取溶劑之(110)晶格面強度、半高寬與晶粒大小 37
表 3 3不同萃取溶劑用於鈣鈦礦太陽能電池之阻抗表 38
表 3 4不同萃取溶劑製備之電池元件表現 40 |
| 參考文獻 |
參考文獻
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| 指導教授 |
詹佳樺
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審核日期 |
2018-7-27 |
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