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研究生:左紘屹
研究生(外文):Hong-Yi Zuo
論文名稱:具多芳香胺取代紫質之合成及其在鈣鈦礦太陽能電池的應用
論文名稱(外文):Synthesis of Multiple Arylamine-Substituted Porphyrins and Their Applications in Perovskite Solar Cells
指導教授:葉鎮宇
指導教授(外文):Chen-Yu Yeh
口試委員:張啟光陳錦地
口試委員(外文):Chi-Kwong ChangChin-Ti Chen
口試日期:2018-01-08
學位類別:碩士
校院名稱:國立中興大學
系所名稱:化學系所
學門:自然科學學門
學類:化學學類
論文種類:學術論文
論文出版年:2018
畢業學年度:106
語文別:中文
論文頁數:145
中文關鍵詞:紫質鈣鈦礦太陽能電池
外文關鍵詞:PorphyrinPerovskite solar cell
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本篇論文主要的研究方向為合成π共軛擴張特性之紫質電洞傳輸材料(Hole-transporting materials, HTMs),並應用在高效率之鈣鈦礦太陽能電池(Perovskite solar cells, PSCs)。所研究的HTM材料分為具雙炔基架橋紫質(Diethynyl-bridged porphyrin)與熔合紫質(Fused porphyrin)兩類。在具雙炔基架橋紫質的研究中,分別於紫質的meso-5,15位置以乙炔基做為架橋,並於另一端修飾不同的推、拉電子基而得HTM材料HY1–HY3,材料合成的策略主要是應用鈀催化之Sonogashira coupling來進行碳-碳鍵之偶合。本論文同時也探討不同的取代基對於紫質材料的吸光範圍、電化學表現及光電性質之影響。
在太陽能電池應用測試中,於TiO2或SnO2半導體表面以spin-coating方式塗佈Cs0.05[(FA0.83MA0.17)PbI0.83Br0.17]0.95 triple-cation perovskite為吸光敏化層,以新開發之HY1–HY3為電洞傳輸層、並蒸鍍上金做為對電極而製成鈣鈦礦太陽能電池元件。結果顯示在SnO2為基板下,HY3元件具有極佳的光電轉換效率(PCE)、開環電壓(VOC)及短路電流(JSC),分別為PCE = 13.37 %;VOC = 1.04 V;JSC = 20.07 mA cm-2,與同條件下Spiro-OMeTAD元件相當接近(PCE = 14.53 %;VOC = 0.98 V;JSC = 20.74 mA cm-2)。然而當以TiO2為基板時,元件HY1-HY3之PCE介於14.46-14.95%之間,略低於Spiro-OMeTAD之17.77%。值得一提的是,在dopant-free的條件下,雖然元件HY1-HY3測得的效率不高,分別為SnO2基板之5.82-7.62%與TiO2基板之10.90-13.10%,但SnO2基板之HY3元件VOC高達1.08 V。或許在更換元件材料、測試的參數等條件後,該分子於光電表現上有機會更進一步的突破。
This thesis mainly focuses on the design and synthesis of extended π-conjugated porphyrins as hole-transporting materials (HTMs) for the application on Perovskite solar cells (PSCs). The materials to be studied in this thesis can be categorized into diethynyl porphyrins and fused porphyrins. In the former cases, different donor and acceptor groups were attached to terminal positions of 5,15-diethynyl substituted porphyrin using series of palladium-catalyzed Sonogashira coupling reactions. These were further studied the influence of donor/acceptor groups on corresponding photophysical, electrochemical properties and device performances.
In the photovoltaic investigations, the triple-cation perovskite containing Cs0.05[(FA0.83MA0.17)PbI0.83Br0.17]0.95 were spin-coated on TiO2 or SnO2 semiconductors as photosensitizing layer, HY1-HY3 in this thesis as hole-transporting layer and vacuum deposited Au layer as counter electrode. As a result, the HY3-based device shows impressive performance on power conversion efficiency (PCE), open-circuit voltage (VOC) and short-circuit current (JSC) when using SnO2 substrate (PCE = 13.37 %, VOC = 1.04 V, JSC = 20.07 mA cm-2), which is comparative to Spiro-OMeTAD under similar condition (PCE = 14.53 %, VOC = 0.98 V, JSC = 20.74 mA cm-2). However, when TiO2 is used as substrate, devices HY1-HY3 have PCE ranging between 14.46% and 14.95%, which is slightly lower that that of Spiro-OMeTAD (17.77%). It is worth noting that without the using of dopants, devices HY1-HY3 have mediate measured PCEs (SnO2: 5.82-7.62%; TiO2: 10.90-13.10%). Nevertheless, the dopant-free SnO2-based device using HY3 as HTM has outperforming VOC of 1.08 V. Perhaps suitable optimization on materials and conditions involved, the HY3 device will show even higher performance.
第一章 緒論
1-1 前言 1
1-2 太陽能電池簡介 2
1-3 鈣鈦礦太陽能電池(Perovskite solar cell, PSCs)8
1-4 太陽能電池的性能量測 14
1-5 紫質簡介 17
1-6 紫質吸收光譜理論 20
1-7 研究動機 22
第二章 紫質染料合成
2-1 應用於雙炔基紫質的推電基合成 25
2-2 應用於雙炔基紫質的拉電子基合成 26
2-3 具推拉電子基的雙炔基紫質合成 29
2-4 應用於熔合紫質的推電子基之合成 34
2-5 雙邊熔合紫質的合成 35
2-6 四邊熔合紫質的合成 40
第三章 結果與討論
3-1 具推拉電子基的雙炔紫質染料 43
3-2 UV-vis and Photoluminescence (PL) spectra 44
3-3 電化學性質 47
3-4 Photovoltaic Characterization 52
第四章 結論 57
第五章 未來展望 58
第六章 實驗藥品、儀器 60
第七章 合成步驟 64
第八章 參考資料 93
附錄 97
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