近年來鈣鈦礦太陽能電池快速的發展，其經由認證的光電轉換效率從原先3.8％已經大幅提升到25.2％，除了效率的提升以外，鈣鈦礦太陽能電池本身優良的光電性質以及能使用低成本溶液製程製作的優勢，被認為具有商業化的潛力。然而目前高效率鈣鈦礦太陽能電池的研究大多數著眼在小型元件中(約為0.1cm2)，大面積製作的鈣鈦礦太陽能模組表現落後於小型元件甚多，故元件放大製程的開發亦開始被重視。開發放大製程過程中會遇到的問題包括設備需求、鍍膜方法品質以及環境的要求。其中無孔洞且均勻的阻隔層被視為改善大面積鈣鈦礦太陽能電池的關鍵因素之一。
本實驗室擁有以電沉積方法製備二氧化鈦阻隔層之技術，其所需的設備以及製程相較於其他大面積沉積技術簡單，而該方法可通過改變電極系統參數控制二氧化鈦薄膜的形貌和厚度。此外本實驗室過去也成功開發水性硝酸鉛前驅物製程，改善以往被廣泛應用在碘化鉛前驅物系統的有毒溶劑二甲基甲醯胺，將製備鈣鈦礦薄膜過程趨向環保。然而上述兩種技術尚未在真正大面積鈣鈦礦太陽能模組的平台試驗，而這正是本研究的目標。
首先利用薄膜太陽能模組中常見的單片互聯P1＆P2＆P3劃線技術製備鈣鈦礦太陽能模組，開發出可在模組上量測單一電池以及串聯模組的結構。接著比較電沉積法與常見旋轉塗佈法阻隔層在模組中的表現，最後將水性硝酸鉛製程應用於鈣鈦礦太陽能模組並對其進行優化，提供相對於碘化鉛前驅物製程對人體以及環境較友善的鈣鈦礦太陽能模組製程技術。

Recently, significant progress of organometallic halide perovskite solar cell (PSC) has been achieved, boosting the power conversion efficiency (PCE) to 25.2%. Based on this rapid development, PSCs are regarded as a potential candidate for the commercial application. However, most high PCE of PSCs are recorded in tiny areas, typically around 0.1cm2 or less. The PCEs of large-area perovskite solar cells and modules still lag behind those of small area devices. The quality requirement of the films in large-area PSC is much more severe than that in small area devices. For example, a pinhole-less and uniform blocking layer (BL) is regarded as one of the key factors to improve the PCE of large-area PSC.
We previously developed the bottom-up deposition method to prepare TiO2 BL by electrodeposition technology and the low-toxicity Pb(NO3)2/water system to fabricate perovskite thin film. Electrodeposition method provides controllability for the morphology and thickness of resultant TiO2 films by simply manipulating deposition parameters. Low-toxicity Pb(NO3)2/water system compared to the PbI2/DMF system is an environmentally friendly fabrication of PSCs. However, these two technologies have still not been extensively investigated on perovskite solar modules (PSM).
In this report, we tried our efforts in developing monolithic PSM. In particular, the interconnect structure, P1&P2&P3 scribe, was established. Moreover, based on our unique pattern design of PSMs, the PCE of single cell and series module can be individually measured. Subsequently, we compared PSMs equipped with electrodeposited and spin-coated TiO2 BL. Uniformity, thickness, and PCE are compared and discussed. Finally, we fabricated PSM by using low-toxicity Pb(NO3)2/water system and optimized characteristics of perovskite thin film boosting the device performance. Our approach is compatible with up-scalable deposition techniques and we pave the way for eco-friendly fabrication of efficient PSM.

摘要 I
目錄 V
表目錄 VIII
圖目錄 X
第一章 緒論 1
1-1 前言 1
第二章 文獻回顧 7
2-1 鈣鈦礦太陽能電池簡介 7
2-1-1 鈣鈦礦結構的發現 7
2-1-2 鈣鈦礦太陽能電池起源與發展 8
2-1-3 鈣鈦礦太陽能電池結構與工作原理 11
2-1-4 有機無機混合含鉛鈣鈦礦簡介[21] 14
2-2 鈣鈦礦太陽能模組(Perovskite solar module, PSM) 19
2-2-1 鈣鈦礦太陽能模組的發展現況 19
2-2-2 鈣鈦礦太陽模組單片互聯技術和劃線技術(scribing technique) 24
2-2-3 鈣鈦礦太陽能模組大面積沉積技術 26
2-2-3-1. 旋轉塗佈法(Spin Coating) 26
2-2-3-2噴霧式塗佈(Spray Coating) 28
2-2-3-3噴墨印刷法(Inkjet Printing) 32
2-2-3-4 狹縫式塗佈法(Slot Die Coating) 34
2-4-4-5 刮刀式塗佈法(Blade Coating) 35
2-4-4-6 氣相沉積技術(Vapor Phase Deposition ,VPD) 40
2-3 水性硝酸鉛前驅物製程與電沉積二氧化鈦技術 44
2-3-1水性硝酸鉛前驅物製程 44
2-3-2 電沉積二氧化鈦技術 47
2-4 研究目的與動機 52
第三章 實驗方法與儀器分析 53
3-1 實驗藥品與材料 53
3-1-1 藥品與材料 53
3-1-2 藥品製備與配製 55
3-2 實驗儀器 56
3-2-1 實驗儀器與分析相關設備 56
3-2-2 設備與分析儀器簡介 57
3-3 實驗方法 67
3-3-1 模組P1劃線以及FTO導電玻璃前處理流程 67
3-3-2 TiO2阻隔層製備流程 67
3-3-3 TiO2多孔層製備流程 68
3-3-4 兩步法鈣鈦礦層製備流程 68
3-3-5 模組P2劃線以及電洞傳輸層製備流程 69
3-3-6 模組P3劃線以及背電極製備流程 70
第四章 實驗結果與討論 72
4-1 鈣鈦礦太陽能模組(PSM)系統建立 72
4-1-1 PSM上單顆電池及多顆電池串聯量測平台 72
4-1-2 雷射劃線參數調控 75
4-1-3 P1以及P3劃線 76
4-1-4 P2劃線 77
4-2 鈣鈦礦太陽能模組(PSM)與小型電池(PSC)之比較 84
4-2-1 PSM串聯機制以及PSC之比較 84
4-2-2 PSM量測異常問題 92
4-3 電沉積二氧化鈦阻隔層鈣鈦礦太陽能模組系統 96
4-3-1 電沉積二氧化鈦阻隔層性質分析 96
4-3-2 電沉積二氧化鈦阻隔層鈣鈦礦太陽能模組討論 100
4-3-3 電沉積與旋轉塗佈二氧化鈦阻隔層鈣鈦礦太陽能模組之比較 102
4-4 水性硝酸鉛前驅物鈣鈦礦太陽能模組 103
4-4-1 鈣鈦礦太陽能模組中碘化鉛兩步連續旋塗法之困境 103
4-4-2 水性硝酸鉛與傳統碘化鉛兩步浸泡法鈣鈦礦太陽能模組比較 105
4-4-3 水性硝酸鉛系統鈣鈦礦太陽能模組優化 110
第五章 結論 120
第六章 未來工作 122
參考文獻 123

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