應用於高效率體異質介面反式錫鈣鈦礦太陽能電池之離子性富勒烯衍生物

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羅振銘(Zhen-Ming Luo) 查詢紙本館藏

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應用於高效率體異質介面反式錫鈣鈦礦太陽能電池之離子性富勒烯衍生物
(Ionic Fullerene Derivatives for High Performance Bulk Heterojunction Tin Perovskite Solar Cell)

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摘要(中)

錫鈣鈦礦太陽能電池(Tin Perovskite solar cells, TPSC)由於其吸收層的毒性低、能隙小(Eg  1.41 eV)與吸收係數高等優點，且光伏表現佳而受重視。然而，錫鈣鈦礦(Tin Perovskite, T-Psk)層中的Sn2+容易與空氣中的水氣及氧氣反應氧化成Sn4+，且T-Psk膜的結晶速度快，不易形成緻密的膜，導致所組裝之元件的效率及長時間穩定性差。本研究探討於FA0.98EDA0.01SnI3前驅溶液中添加三種弱酸性離子性富勒烯衍生物C60-(RT2+)6(12X-) (X = Cl, Br, I) (簡稱6-X (X = Cl, Br, I))製備體異質介面的T-Psk膜(稱為6-X@FA0.98EDA0.01SnI3膜)，其中以6-Br@FA0.98EDA0.01SnI3膜作為吸收層所組裝之元件的光電轉換效率達10.09%比以FA0.98EDA0.01SnI3膜作為吸收層所組裝之元件的光電轉換效率(8.21%)高約20%。在未封裝的條件下，以6-Br@FA0.98EDA0.01SnI3膜作為吸收層的TPSC元件放置在手套箱中2520小時後光電轉換效率仍可維持原來效率的84%；而以FA0.98EDA0.01SnI3膜作為吸收層的TPSC元件之光電轉換效率僅剩原來效率的53%。添加6-Br可填補T-Psk膜的晶界，且有部份的Br-進入T-Psk膜的晶格中調整T-Psk層的前置軌域能階，減少載子傳遞至載子傳遞層所造成的能量損失，使所組裝之元件的Voc值由0.59 V增加至0.62 V。此外，添加6-Br也能延緩T-Psk膜的結晶速度，使所製備之T-Psk膜的顆粒大、平整、緻密且結晶度高。而添加6-Br可增加T-Psk前驅溶液的酸性，因此T-Psk前驅溶液中的Sn2+不易氧化成Sn4+，故6-Br@FA0.98EDA0.01SnI3膜的Sn2+/Sn4+比例比FA0.98EDA0.01SnI3膜高。

摘要(英)

Tin Perovskite solar cells (TPSC) are the topic under extensive studies due to the absorber has low toxicity, small energy gap (Eg  1.41 eV) and high absorption coefficient as well as the cell has good photovoltaic performance. However, Sn2+ in the Tin Perovskite (T-Psk) easily reacts with moisture and oxygen in the air to be oxidized to Sn4+ easily as well as the crystallization rate of the T-Psk film is very fast thus it is difficult to form a dense and smooth T-Psk film, resulting in poor efficiency and long-term stability of the device. This study explores the effect of adding three weakly acidic ionic fullerene derivatives C60-(RT2+)6(12X-) (X = Cl, Br, I) (named 6-X (X = Cl, Br, I)) in T-Psk to prepare bulk-heterojunction film (named 6-X@FA0.98EDA0.01SnI3 film). The power conversion efficiency (PCE) of the cell based on 6-Br@FA0.98EDA0.01SnI3 film achieves the highest of 10.09% which is about 20% higher than the that (8.21%) of the device using FA0.98EDA0.01SnI3 film as the absorption layer. Without encapsulation, TPSC with 6-Br@FA0.98EDA0.01SnI3 as the absorber maintains 84% of the initial efficiency when it was placed in the glove box for 2520 hours. While the PCE of the TPSC with FA0.98EDA0.01SnI3 absorber lost 47% of the original efficiency. 6-Br can fill the grain boundaries of the T-Psk film, and some Br- ions can enter the lattice of the T-Psk film to adjust to energy level to reduce the energy loss caused by the transfer of carriers to the carrier transport layer. As a result the Voc of the device increased from 0.59 V to 0.62 V. In addition, the addition of 6-Br can also slow the crystallization of the T-Psk film, so that 6-Br@FA0.98EDA0.01SnI3 film has large grain size, flat, dense and high crystallinity. 6-Br can also increase the acidity of the T-Psk precursor solution to stabilize Sn2+. Therefore, the Sn2+/Sn4+ ratio of the 6-Br@FA0.98EDA0.01SnI3 film is higher than that of FA0.98EDA0.01SnI3 film.

關鍵字(中)

★ 錫鈣鈦礦
★ 太陽能電池

關鍵字(英)

論文目次

摘要 vi
Abstract viii
Graphical Abstract x
謝誌 xi
目錄 xii
圖目錄 xix
表目錄 xxxi
附錄 xxxvii
第一章、緒論 1
1-1、前言 1
1-2、鈣鈦礦太陽能電池(PEROVSKITE SOLAR CELL, PSC) 5
1-2-1. 鈣鈦礦太陽能電池的架構 5
1-2-2. 反式鈣鈦礦太陽能電池的工作原理 6
1-2-3. 鈣鈦礦太陽能電池的光電轉換效率 7
1-3、錫鈣鈦礦太陽能電池之研究歷程 10
1-3-1. 第一個以MASnI3作為吸收層的錫鈣鈦礦太陽能電池研究 10
1-3-2. 第一個以CsSnI3作為吸收層的錫鈣鈦礦太陽能電池研究 12
1-3-3. 第一個以FASnI3作為吸收層並以SnF2作為添加劑的錫鈣鈦礦太陽能電池研究 14
1-3-4. 第一個將EDAI2與GAI應用於FASnI3膜作為吸收層的錫鈣鈦礦太陽能電池研究 16
1-3-5. 現今錫鈣鈦礦太陽能電池的最高光電轉換效率之文獻 19
1-4、體異質介面鈣鈦礦太陽能電池之研究歷程 22
1-4-1. 第一個反式體異質介面鈣鈦礦太陽能電池的研究 22
1-4-2. 第一個反式體異質介面混鉛錫鈣鈦礦太陽能電池的研究 24
1-4-3. 第一個反式體異質介面錫鈣鈦礦太陽能電池的研究 27
1-5、製備錫鈣鈦礦膜的方法 30
1-5-1. 以一步合成法製備錫鈣鈦礦膜 30
1-5-2. 以兩步合成法製備錫鈣鈦礦膜 31
1-5-3. 以一步反溶劑法製備錫鈣鈦礦膜 32
1-6、減少錫鈣鈦礦前驅液與膜中SN4+的方法 33
1-6-1. 添加錫粉使FASnI3前驅溶液中的Sn4+還原成Sn2+ 33
1-6-2. 利用喹啉化合物中的N及O原子與FASnI3膜中的Sn2+配位形成錯合物抑制Sn2+氧化成Sn4+ 37
1-6-3. 在酸性環境下FASnI3前驅溶液中的Sn2+不易氧化成Sn4+ 41
1-7、增加錫鈣鈦礦膜結晶顆粒大小的方法 43
1-7-1. 添加N2H5Cl藉由氯離子延緩錫鈣鈦礦膜的結晶速度製備顆粒大且無孔洞的錫鈣鈦礦膜 43
1-7-2. 添加PHCl利用PH+使錫鈣鈦礦的晶體結構膨脹而舒張製備結晶度高的錫鈣鈦礦膜 45
1-7-3. 調整FAI與MABr之比例將錫鈣鈦礦前驅溶液的組成改為MA0.25FA0.75SnI2.75Br0.25所製備之膜有高的結晶度 49
1-8、實驗動機 51
第二章、實驗方法 53
2-1、實驗藥品與儀器 53
2-1-1. 藥品 53
2-1-2. 儀器設備 54
2-2、反式錫鈣鈦礦太陽能電池組裝步驟 55
2-2-1. 藥品配製 55
2-2-2. 元件組裝步驟 57
2-3、儀器原理及樣品製備 61
2-3-1. 太陽光模擬器的原理及光電轉換效率、暗電流與遲滯現象的量測(Solar Simulator, Enlitech SS-F5) 61
2-3-2. 空間電荷限制電流的原理及量測(Space Charge-Limited Current, SCLC) 62
2-3-3. 太陽能電池外部量子效率量測系統(Incident Photon to Current Conversion Efficiency (IPCE), QE-S3011) 64
2-3-4. X-ray繞射光譜儀(X-Ray Diffractometer, BRUKER D8 Discover) 65
2-3-5. 紫外光/可見光/近紅外光吸收光譜儀(Ultraviolet–visible-NIR spectroscopy, HITACHI U-4100) 66
2-3-6. 光致螢光光譜儀(Photoluminescence Spectrometer, Uni think UniRAM) 67
2-3-7. 場發射掃描式電子顯微鏡(Field Emission Scanning Electron Microscope, NOVA NanoSEM-230) 67
2-3-8. XPS光電子能譜儀(X-ray photoelectron spectroscopy, Thermo VG-Scientific/Sigma Probe) 68
2-3-9. UPS紫外光電子能譜儀(Ultraviolet photoelectron spectroscopy, Thermo VG-Scientific/Sigma Probe) 69
2-3-10. 接觸角量測儀(Contact angle, Grandhand Ctag01) 69
2-3-11. 傅立葉轉換紅外光光譜儀(Fourier transform infrared spectrometer, Jasco 4100) 70
2-3-12. 酸鹼度測定計(pH meter, Jenco 6173) 71
2-3-13. 動態光散射儀(Dynamic light scattering, Microtrac nanotrac wave) 71
第三章、結果與討論 73
3-1、篩選適合用於錫鈣鈦礦膜中的離子性富勒烯衍生物 73
3-1-1. 添加不同離子性富勒烯衍生物至錫鈣鈦礦前驅溶液製備成膜所組裝之元件的光伏表現 73
3-1-2. 添加不同濃度的6-Br至錫鈣鈦礦前驅溶液製備成膜所組裝之元件的光伏表現 75
3-2、篩選0.01-6-BR@FA0.98EDA0.01SNI3膜的最佳製備條件 77
3-2-1. 不同濃度之0.01-6-Br@FA0.98EDA0.01SnI3前驅溶液製備成膜所組裝之元件的光伏表現 77
3-2-2. 以不同SnI2:有機鹵化物比例的0.01-6-Br@FA0.98EDA0.01SnI3前驅溶液製備成膜所組裝之元件的光伏表現 78
3-2-3. 以不同加熱方式製備0.01-6-Br@FA0.98EDA0.01SnI3膜所組裝之元件的光伏表現 80
3-2-4. 在添加6-Br下是否添加EDAI2於錫鈣鈦礦前驅溶液製備成膜對所組裝元件的光伏表現之影響 81
3-2-5. 在添加6-Br下是否添加SnF2於錫鈣鈦礦前驅溶液製備成膜對所組裝元件的光伏表現之影響 83
3-2-6. 在添加6-Br下是否添加錫粉於錫鈣鈦礦前驅溶液製備成膜對所組裝元件的光伏表現之影響 85
3-2-7. 在6-Br@FA0.98EDA0.01SnI3膜上有無沉積C60膜作為電子傳遞層對所組裝之元件的光伏表現之影響 87
3-2-8. 以6-Br是否能取代錫粉作為FA0.98EDA0.01SnI3前驅溶液的添加劑製備高效率的錫鈣鈦礦膜 88
3-3、添加不同離子性富勒烯衍生物之錫鈣鈦礦膜所組裝之最高效率元件的IPCE表現 90
3-4、添加不同離子性富勒烯衍生物之錫鈣鈦礦膜所組裝之最高效率元件的遲滯現象 91
3-5、添加不同離子性富勒烯衍生物之錫鈣鈦礦膜的SEM表面形貌、EDS MAPPING及剖面圖 93
3-6、有無添加6-BR之錫鈣鈦礦膜的AFM表面形貌及相位影像 100
3-7、 6-BR、6-BR@SNI2及6-BR@SNF2之FTIR穿透光譜 101
3-8、添加不同離子性富勒烯衍生物之錫鈣鈦礦膜的XRD繞射圖 103
3-9、添加不同量的6-BR之錫鈣鈦礦膜的XRD繞射圖 106
3-10、添加不同離子性富勒烯衍生物之錫鈣鈦礦膜的UV-VIS吸收光譜 108
3-11、添加不同量的6-BR之錫鈣鈦礦膜的UV-VIS吸收光譜 109
3-12、添加不同離子性富勒烯衍生物之錫鈣鈦礦膜的前置軌域能階 111
3-13、添加不同離子性富勒烯衍生物之錫鈣鈦礦膜的PL及TRPL光譜 116
3-14、添加不同量的6-BR之錫鈣鈦礦膜的PL光譜 125
3-15、添加不同離子性富勒烯衍生物之錫鈣鈦礦膜的XPS能譜圖 126
3-16、添加離子性富勒烯衍生物對錫鈣鈦礦膜親疏水性的影響 129
3-17、添加離子性富勒烯衍生物所配製之錫鈣鈦礦前驅溶液對PEDOT:PSS膜的相容性 130
3-18、添加離子性富勒烯衍生物對錫鈣鈦礦太陽能電池元件長時間穩定性的影響 131
3-19、添加離子性富勒烯衍生物對錫鈣鈦礦太陽能電池元件之穩態電流密度及效率輸出的影響 133
3-20、添加離子性富勒烯衍生物對錫鈣鈦礦太陽能電池元件之暗電流的影響 134
3-21、添加離子性富勒烯衍生物對錫鈣鈦礦太陽能電池元件之空間電荷限制電流的影響 135
第四章、結論 140
參考文獻 141
附錄 148
附錄1. 添加不同溴化物之錫鈣鈦礦膜所組裝之元件的光伏表現 148
附錄2. C60、PCBM與6-X (X = CL, BR ,I)在DMSO中的平均粒徑及平均粒徑分佈 150
附錄3. 添加離子性富勒烯衍生物對錫鈣鈦礦太陽能電池元件各項光伏參數之長時間穩定性的影響 151

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指導教授

吳春桂(Chun-Guey Wu)

審核日期

2021-8-30

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