增加一般式鈣鈦礦太陽能電池光電轉換效率與長時間穩定性的探討

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詹識懷(Shih-Huai Chan) 查詢紙本館藏

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增加一般式鈣鈦礦太陽能電池光電轉換效率與長時間穩定性的探討

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至系統瀏覽論文 (2024-11-13以後開放)

摘要(中)

近幾年來，科學界對「有機-無機鈣鈦礦太陽能電池(PSC)」產生極大的關注，因為PSC製程簡單、材料價格便宜且具有高的光電轉換效率等優點。然而，若使用溶劑工程法製備鈣鈦礦膜，無法精準控制鈣鈦礦的結晶，所得膜有許多晶界(Grain boundary)，影響所組裝之元件的光伏表現和長時間穩定性。本研究將「釕金屬染料(N749、CYK-17、CYK-18、CYK-19)、有機染料(BTI-3、BTI-19、INDT-1)」旋轉塗佈於鈣鈦礦膜的表面，填補鈣鈦礦膜表面的缺陷，並擴大其在長波長的吸光能力，增加元件的光電轉換效率與穩定性。但是上述七種染料修飾物，只有釕金屬染料(N749、CYK-17)與有機染料(BTI-19)修飾鈣鈦礦膜所組裝之元件的光電轉換效率，比未經染料修飾Psk膜之元件高出1%以上。從IR光譜圖看到，染料結構中的羧基(R-COOH)與硫氰酸根(SCN)的波數，有紅位移的現象。證明染料會與鈣鈦礦的鉛離子產生作用力。從接觸角得知，鈣鈦礦膜經染料修飾後的接觸角為(Psk/N749：75.6o、Psk/CYK-17：75.6o、Psk/BTI-19：78.8o)大於未經修飾之鈣鈦礦膜(Psk：56.5o)，推得鈣鈦礦膜經染料修飾形成疏水的表面，減少水氣的吸附，延長鈣鈦礦膜的壽命。從光致螢光光譜圖得知，鈣鈦礦膜經染料修飾的螢光強度，皆比未經染料修飾的鈣鈦礦膜強。推得鈣鈦礦膜經染料修飾，能增加激子的生命期，減少電子與電洞發生再結合的機率。相較鈣鈦礦膜為吸收層所組裝之元件的光電轉換效率(17.70%)，染料修飾鈣鈦礦膜組裝之元件的光電轉換效率(Psk/N749(cell)：19.62%、Psk/CYK-17(cell)：18.66%、Psk/BTI-19(cell)：19.08%)，並且將元件放置於大氣環境與手套箱中，皆比Psk(cell)有較好的穩定性。因此使用染料塗佈於鈣鈦礦膜組裝之元件，是同時增加元件效率和穩定性的有效方法。

摘要(英)

Perovskite solar cells (PSCs) based on organic-inorganic hybrid lead halide perovskite absorber has attracted great attention from the new generation PV community. PSCs has the characteristics of simple process, cheap material, and high power conversion efficiency. However, perovskite film prepared with solvent engineering, the crystallization cannot be controlled precisely. As a result, the film has many grain boundaries which affect the photovoltaic performance and long-term stability of the resulting photovoltaic devices. In this study, several Ruthenium dyes (such as N749, CYK-17, CYK-18, CYK-19) and organic dyes (such as BTI-3, BTI-19, INDT-1) were spin-coated on the top of the perovskite film to remedy the defects on the surface of the perovskite film to enhance the efficiency and stability of the cells. Among the above seven dye modifications, only N749, CYK-17 (ruthenium dyes) and BTI-19 (organic dye) can increase the efficiency of the cell. IR spectra evidenced the shift of absorption peaks of the carboxyl group (R-COOH) and thiocyanate (SCN) in the dye molecule suggesting the interaction between dye molecules and Pb+2 in perovskite. The contact angle of the perovskite film increases after modifying with dye molecules (Psk : 56.5o, Psk/N749: 75.6o, Psk/CYK-17: 75.6o, Psk/BTI-19: 78.8o) to create more hydrophobic surface. Consequently, the stability of the modified perovskite film as well as the corresponding devices enhanced. The photoluminescence intensity and life-time proved that dye modification can increase the life of the exactions and reduce the charge recombination of the perovskite film. The efficiency of the cell based on unmodified perovskite is 17.70% which is smaller than those based on dye-modified perovskite solar cell (Psk/N749(cell) : 19.62%, Psk/CYK-17(cell) : 18.66%, Psk/BTI-19(cell) : 19.08%). Furthermore, the longer stability of the cell based on dye modified absorber is better than that used unmodified perovskite absorber both in ambient atmosphere and glove box.

關鍵字(中)

★ 鈣鈦礦太陽能電池
★ 染料

關鍵字(英)

★ Perovskite Solar Cell
★ Dye

論文目次

目錄
摘要 I
ABSTRACT III
GRAPHICAL ABSTRACT V
謝誌 VI
目錄 VII
圖目錄 XIII
表目錄 XVIII
第一章、緒論 1
1-1、前言 1
1-2、鈣鈦礦結構(Perovskite structure) 3
1-3、鈣鈦礦太陽能電池(Perovskite solar cell, PSC) 5
1-3-1. 鈣鈦礦太陽能電池的架構 5
1-3-2. 一般式鈣鈦礦太陽能電池的工作原理 6
1-3-3. 鈣鈦礦太陽能電池的光電轉換效率 7
1-4、鈣鈦礦太陽能電池之研究歷史 11
1-4-1. 第一個將鈣鈦礦材料應用於太陽能電池的文獻 11
1-4-2. 固態電解質應用於鈣鈦礦太陽能電池 12
1-5、鈣鈦礦太陽能電池的研究方法 14
1-5-1. 以一步驟(Single-step)合成法製備鈣鈦礦吸光層 14
1-5-2. 以兩步驟(Two-step)合成法製備鈣鈦礦吸光層 15
1-5-3. 一步驟反溶劑處理法製備鈣鈦礦吸光層 16
1-6、鈣鈦礦太陽能電池之吸光層材料 18
1-6-1. 二元陽離子之鈣鈦礦吸光層 18
1-7、鈣鈦礦膜的優化 21
1-7-1. 添加高分子於鈣鈦礦起始溶液製備缺陷較少的鈣鈦礦膜 21
1-7-2. 添加雙功能陽離子(GABA+)製備穩定性較好的鈣鈦礦膜 22
1-7-3. (D35)染料敏化電子傳遞層(TiO2)製備高效率且穩定性較好的鈣鈦礦太陽能電池 24
1-7-4. 有機染料(AQ310)當作Anti-solvent製備缺陷較少的鈣鈦礦膜 25
1-7-5. 使用硫氰酸鹽修飾鈣鈦礦奈米粒子，減少晶體表面的缺陷 27
1-7-6. 有機分子修補鈣鈦礦膜表面的缺陷增加元件穩定性 29
1-8、本研究所使用之染料分子的特性介紹 31
1-8-1. N749染料 31
1-8-2. CYK-17、CYK-18及CYK-19染料 33
1-8-3. BTI-3及BTI-19染料 36
1-8-4. INDT-1染料 38
1-9、研究動機 39
第二章、實驗方法 40
2-1、實驗藥品與儀器 40
2-1-1. 藥品 40
2-1-2. 儀器設備 43
2-2、一般式鈣鈦礦太陽能電池組裝步驟 44
2-2-1. 藥品的配製 44
2-2-2. 元件組裝步驟(如圖2-2-1所示) 47
2-3、儀器分析 51
2-3-1. 太陽光模擬器及光電轉換效率量測(Solar Simulator, DENSO KXL-500F) 51
2-3-2. 掃描式電子顯微鏡(Scanning Electron Microscope, Hitachi S-800) 52
2-3-3. X-ray繞射光譜儀(X-Ray Diffractometer, BRUKER D8 Discover) 53
2-3-4. 熱蒸鍍系統(Thermal evaporation system, 高敦Thermal).. 54
2-3-5. 太陽能電池外部量子效率量測系統(Incident Photon to Current Conversion Efficiency (IPCE), Enlitech PVCS-I) 55
2-3-6. 光激發螢光光譜儀(Photoluminescence Spectrometer, Uni think Uni-RAM) 57
2-3-7. 傅立葉轉換紅外光光譜儀(Fourier transform infrared spectrometer, Jasco 4100) 58
2-3-8. 接觸角量測儀器(contact angle, Grandhand Ctag01) 59
2-3-9. UPS紫外光電子能譜儀(Ultraviolet photoelectron spectroscopy) 60
第三章、結果與討論 61
3-1、不同染料以不同方式修飾鈣鈦礦膜所組裝之元件 61
3-1-1. 篩選適合應用於鈣鈦礦表面處理之染料 63
3-1-2. 將(N749、CYK-17、CYK-18、CYK-19、BTI-3、BTI-19及INDT-1)染料配置成(0.1 mg/ml)修飾鈣鈦礦膜 63
3-1-3. 染料濃度的優化 65
3-1-4. 染料修飾鈣鈦礦膜所組裝之PSC元件的IPCE表現 67
3-1-5. 染料修飾鈣鈦礦膜所組裝之元件的電流遲滯現象 68
3-1-6. (N749、CYK-17、BTI-19)染料修飾鈣鈦礦膜所組裝之PSC元件的長時間穩定性 70
3-1-7. (CYK-18、CYK-19)染料修飾鈣鈦礦膜所組裝之PSC元件的長時間穩定性 72
3-1-8. 使用貼膠帶的方式製備電子傳遞層所組裝之元件的光伏表現 74
3-1-9. (CYK-17、CYK-17H)染料修飾鈣鈦礦膜組裝之元件的光伏表現 75
3-2、染料修飾後之鈣鈦礦膜的光學性質與表面形貌 76
3-2-1. IR穿透光譜圖 76
3-2-2. 染料修飾後之鈣鈦礦膜的EDS圖 79
3-2-3. (N749)染料修飾後之鈣鈦礦膜的元素分析 81
3-2-4. (N749、CYK-17)染料修飾鈣鈦礦膜後經氯苯清洗之鈣鈦礦膜的EDS圖 82
3-2-5. 染料修飾後之鈣鈦礦膜的UV-vis吸收光譜圖 83
3-2-6. 染料修飾前後之鈣鈦礦膜的UV-VIS吸收光譜圖 84
3-2-7. 低濃度(1M)鈣鈦礦起始溶液製備鈣鈦礦膜經(N749)染料修飾後之鈣鈦礦膜的UV圖及所組裝之元件的IPCE圖 85
3-2-8. 染料修飾後之鈣鈦礦膜的前置軌域能階 87
3-2-9. 染料修飾後之鈣鈦礦膜的螢光光譜圖(PL)與瞬態吸收光譜圖(TRPL) 93
3-2-10. (CYK-18、BTI-3、INDT-1)染料修飾後之鈣鈦礦膜的螢光光譜圖(PL)與瞬態吸收光譜圖(TRPL) 95
3-2-11. 染料修飾後之鈣鈦礦膜的(SEM)表面形貌與剖面圖 98
3-2-12. 染料修飾後之鈣鈦礦膜的X-Ray繞射圖(XRD) 101
3-2-13. 染料修飾後之鈣鈦礦膜的接觸角 102
3-2-14. 染料修飾後之鈣鈦礦膜放置於大氣環境下的穩定性 103
3-2-15. N749染料修飾後之鈣鈦礦膜放置於大氣環境的X-Ray繞射圖 104
第四章、結論 105
參考資料 106
附錄 111
附錄1. (CYC-33O、CYC-37、Y-1)染料修飾鈣鈦礦膜所組裝之元件的光伏表現 111
附錄2. (CYC-33O、CYC-37、Y-1)染料修飾後之鈣鈦礦膜的UV圖與所組裝之元件的IPCE圖 113

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指導教授

吳春桂(Chun-Guey Wu)

審核日期

2019-11-14

推文