臺灣博碩士論文加值系統

全球能源消耗的增加和對化石能源的依賴導致了環境中大量二氧化碳引起的氣候變化。太陽能電池已成為最有希望的化石燃料替代品，因為太陽能是未來可再生和可持續能源技術中最安全、最清潔且最豐富的能源之一。鈣鈦礦太陽能電池(Perovskite Solar Cell, PSC)在過去十年中發展迅速，為了提升太陽能轉換效率，製備新穎電洞傳輸層材料(Hole transporting material, HTM)被視為依最有效的方式。於本論文中，合成了兩個系列的電洞傳輸層(Hole transporting layer, HTL)有機小分子材料，即 CC 和 SN 系列。在這些新型 HTL中，以亞甲基芴作為核心基團，在支鏈上導入具有電子豐盈特性之三苯胺和其他各種化學物質(三氟甲基、二苯胺、咔唑和吩噻嗪）。這些電洞傳輸材料將與NiOx配對，作為反式鈣鈦礦太陽能電池中的雙層空穴傳輸層。有機小分子HTL有望鈍化NiOx界面上的缺陷並提高器件的性能。
研究中除研究並比較不同有機小分子導入後其形貌、能級、電荷轉移電阻、元件效率及穩定性等特性。而反式元件之構型包含 ITO/NiOx/CC或SN系列/Perovskite/PC61BM/BCP/Ag。如前所述，NiOx是無機 HTL，CC和SN系列是有機HTL，鈣鈦礦是光吸收層，PC61BM和BCP分別是電子傳輸層和電動阻擋層。於CC系列中，以NiOx/CC-3雙層的結構因改善了能級排列、薄膜形態、結晶度和電洞傳輸特性，從而實現了高質量的鈣鈦礦層和界面接觸行為。因此，這種反式電池顯著提高了開路電壓(open-circuit voltage, VOC)、短路電流密度(short-circuit density, JSC)、填充因子(fill factor, FF)和光電轉換效率(power conversion efficiency, PCE)值，最高可達21.66 mA cm-2、1.105 V、79.33 %和19.813%。此外，NiOx/CC-3元件具有可忽略不計的遲滯效應和長期穩定性，在氬氣下保持超過 90%的原始效率，在40天後在環境大氣中仍保持超過80%的效率。
而於SN系列中，迄今亦已完成了3個樣品的合成與基本熱性質、光與電化學性質。相信藉由引入更長共軛結構的亞甲基芴結構，同時搭配不同推電子基結構可以對於其光電性質有所差異，並期望得到更高的光電轉換效率。

The rising global energy consumption and the dependence on fossil energy led to climate change caused by significant amounts of CO2 in the environment. Solar cells have emerged as the most promising substitute for fossil fuels since solar energy is the safest, cleanest, and one of the most abundant energy sources for future renewable and sustainable energy technology. Perovskite solar cells (PSCs) have advanced fast during the last decade. This work synthesized two series of hole transport layers (HTLs), namely CC and SN series. On these novel HTLs, dibenzofulvene segment was employed as the core, with additional triphenylamine and various chemicals on the branches (trifluoromethyl groups, diphenylamine, carbazole, and phenothiazine). These hole transport materials will be paired with NiOx as a bilayer hole transport layer in inverted perovskite solar cells. The small organic molecule HTLs are expected to passivate the defect on the NiOx interface and boost the device's performance.
Morphology, energy level, charge transfer resistance, and device stability were compared and studied. The device architecture contained ITO/NiOx/CC or SN series/Perovskite/PC61BM/BCP/Ag. As mentioned, NiOx is the inorganic HTL, CC and SN series are the organic HTLs, perovskite is the light absorption layer, PC61BM and BCP are the electron transport layer and hole blocking layer, respectively. For CC series, the NiOx/CC-3 bilayer-based architecture improves energy level alignment, film morphology, crystallinity, and hole transportation, allowing for a high-quality perovskite layer and interfacial contact behavior. As a result, this inverted cell significantly improves open-circuit voltage (VOC), short current density (JSC), fill factor (FF), and power conversion efficiency (PCE) values up to 21.66 mA cm-2, 1.105 V, 79.33%, and 19.813%, respectively. Remarkedly, the NiOx/CC-3 device has negligible hysteresis and long-term stability, retaining over 90% of its original efficiencies under argon and over 80% in the ambient atmosphere after 40 days.
In the SN series, three samples were synthesized accordingly, basic thermal properties, optical and electrochemical properties have been completed. It is believed that by introducing a methylene fluorene structure with a longer conjugated structure and matching different electron-pushing group structures simultaneously, the photoelectric properties can differ, and higher photoelectric conversion efficiency is expected to be obtained.

Table of Content
摘要 i
Abstract iii
Acknowledgement v
List of Tables ix
List of Figures x
Chapter 1 Introduction 1
1-1 Background 1
Chapter 2 Literature Review and Research Motivation 5
2-1 Types of Solar Cells 5
2-2 Perovskite Solar Cells 7
2-3 Hole Transporting Materials of Inverted Perovskite Solar Cells 10
2-3-1 Type of SM-HTMs for Inverted Perovskite Solar Cells 12
2-4 Double-layer HTMs for Inverted Perovskite Solar Cells 18
2-5 Research Motivations 19
Chapter 3 Experiment Methodology 21
3-1 Experimental Flow Chart 21
3-2 Instruments 23
3-3 Experimental Chemicals 24
3-4 Organic solvents 25
3-5 Synthesis of HTMs 26
3-5-1 Synthesis Process of F-01 (N,N-diphenyl-4-(trifluoromethyl)aniline) (Figure 3-2) 28
3-5-2 Synthesis of Process of F-02 (4-(phenyl(4-(trifluoromethyl) phenyl) amino) benzaldehyde (Figure 3-3) 29
3-5-3 Synthesis Process of F-03 (4-((2,7-dibromo-9H-fluoren-9-ylidene)methyl)-N-phenyl-N-(4-(trifluoromethyl)phenyl)aniline) (Figure 3-4) 30
3-5-4 Synthesis Process of CC-1 (Figure 3-5) 31
3-5-5 Synthesis Process of TPA-DBF (Figure 3-6) 33
3-5-6 Synthesis Process of CC-2 (Figure 3-7) 34
3-5-7 Synthesis Process of CC-3 (Figure 3-8) 36
3-5-8 Synthesis Process of SL-01 (Figure 3-9) 38
3-5-9 Synthesis Process of SL-02 (Figure 3-10) 39
3-5-10 Synthesis Process of SL-03 (Figure 3-11) 40
3-5-11 Synthesis Process of SL-04 (Figure 3-12) 41
3-5-12 Synthesis Process of SN-1 (Figure 3-13) 42
3-5-13 Synthesis Process of SN-2 (Figure 3-14) 44
3-5-14 Synthesis Process of SN-3 (Figure 3-15) 46
Chapter 4 Results and Discussion 48
4-1 CC Series Synthesis and Identifications 48
4-1-1 Synthesis and Identification of CC-1 48
4-1-2 Synthesis and Identification of CC-2 52
4-1-3 Synthesis and Identification of CC-3 55
4-2 SN Series Synthesis and Identifications 58
4-2-1 Synthesis and Identification of SN-1 58
4-2-2 Synthesis and Identification of SN-2 62
4-2-3 Synthetic and Identification of SN-3 66
4-3 Photochemical Property Analysis 70
4-3-1 Part-1 71
4-3-2 Part-2 74
4-4 Electrochemical Analysis 77
4-4-1 Part-1 77
4-4-2 Part-2 80
4-5 Theoretical Approach 82
4-5-1 Part-1 82
4-6 Thermal Properties Test 85
4-6-1 Part-1 85
4-6-2 Part-2 88
4-7 Inverted Solar Cells Fabrication 90
4-7-1 Part-1 90
Chapter 5 Conclusions 111
Chapter 6 References 112

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