臺灣博碩士論文加值系統

本論文將探討本實驗室所設計出的兩種新型的低能隙共軛高分子，並將其應用於高分子薄膜太陽能元件。我們比較不同主結構的共軛高分子，分別是苯並噻二唑以及苯並硒二唑衍生物作為基礎之低能隙聚合物。在苯並噻二唑衍生物之共軛聚合物的設計中，我們以缺電子單元benzothiadiazole (BTD)單體來增強共軛高分子之光學吸收能力，推電子單元為3,3-difluoro-2,2-bithiophene-5,5-diyl)bis(trimethyl-stannane)(DFBT-bisSn)以提升高分子鏈之平面性，並利用將長碳鏈導入thiophene中，而導入長碳鏈之目的是使溶解度提升，藉由導入不同碳鏈長度，提供足夠共軛側鏈排列堆疊，並期許高分子鏈之排列趨向平面。共軛高分子苯並噻二唑衍生物本身表現出良好的電洞遷移率，PBDOD-TF的電洞遷移率為(2.72±0.1.21)x10-4；PBDOD-TF的電洞遷移率為(2.24±0.38)x10-4。在實驗中我們同時研究了烷基鏈對本體異質結構型態和光伏性能的影響。在本體異質結構聚合物的高分子薄膜太陽能元件中，我們以共軛高分子作為電子予體；以PC61BM作為電子受體做為太陽能電池的發電主動層。此太陽能元件依結構順序為ITO/ ZnO/ conjugated polymer:PCBM/ V2O5/ Ag。在此元件製程中，雖然共軛高分子本身具有良好的電洞遷移率，但是透過穿透式顯微鏡我們可以看到該共軛高分子與富勒烯衍生物混摻過後的薄膜的表面型態具有相當大的domain size，造成了電子予體與電子受體無法有效利用彼此的界面面積進而傳遞電子與電洞，因此製成太陽能電池元件後，以PBDOD-TF:PC61BM作為主動層的最佳元件短路電流為5.89 mA/cm2，光電轉換效率為2.63%；PBDOT-TF:PC61BM作為主動層的最佳元件短路電流為2.87 mA/cm2，光電轉換效率為1.39%
在論文的第二部分中，共軛聚合物包含電子缺乏區的苯並二噻吩4,7-di(thiophen-2-yl)benzo[c][1,2,5]sele odiazole (DTBSe)的單元，二氟雙噻吩(3,3-difluoro-2,2-bithiophene)則是作為電子供體單元，並且以乙烯基三噻吩vinyl-terthiophene (VTT)及兩個2-辛基十二烷基鏈(2-octyldodecyl chains)作為側鏈來提升溶解度。共軛高分子PDTBSeVTT-2TF在UV光譜中，表現出300-800nm的寬吸收和1.57eV的窄光學帶隙，其HOMO為-5.57eV。我們以苯並硒二唑衍生物作為基礎的共軛高分子，與富勒烯衍生物(PC71BM)混摻的製程溶液分別在50℃和65℃的兩個不同溫度下混溶。在65℃下的共混溶液表現出最佳的光電轉換效率，其PCE為5.03％，Jsc為10.99 mA/cm2。在50℃下的共混物溶液所製得的太陽能元件之PCE為4.63％， Jsc為10.15 mA/cm2。 PCE的提升可能是由於聚合物鏈的熱運動增加使PDTBSeVTT-2TF簇分解成單分子和小聚集體，促進共軛高分子和PC71BM之間形成奈米級域，進而增加D/A界面和光電流。

This thesis mainly studies the photovoltaic behaviors of two different types of new low bandgap conjugated polymers. We compare conjugated polymers of different structures which based on Benzothiadiazole or Benzoselenodiazole derive low bandgap polymers. In the first conjugated polymer, an electron-deficient unit benzothiadiazole (BTD) monomer is added to enhance the optical absorption capability of the conjugated polymer, and the electron donor unit is 3,3-difluoro-2,2-bithiophene-5,5-diyl)bis(trimethyl-stannane)(DFBT-bisSn) to enhance the planarity of the polymer chain and to introduce long carbon chains into the thiophene, while the purpose of introducing long carbon chains is to increase solubility. By introducing different carbon chain lengths, enough conjugated side chains are arranged and stacked, and the arrangement of polymer chains tends to be flat. Polymer abbreviated as PBDOD-TF and PBDOT-TF, respectively and the effect alkyl chain on the bulk-heterojunction morphology and photovoltaic performance were investigated. The hole mobility µh of PBDOD-TF ((2.72±0.1.21)x10-4) and PBDOT-TF ((2.24±0.38)x10-4) are in the same order of magnitude with slightly higher values when compared to PBDOT-TF. Through the transmission microscope, we can see that the surface morphology of the film blended with the conjugated polymer and the fullerene derivative has a considerable domain size, which causes the electron donor and the electron acceptor to be unable to effectively utilize each other interface to transfer electrons and holes. Polymer solar cells were fabricated by using [6,6]-phenyl-C61-butyric acid methyl ester (PC61BM) as the acceptor with the inverted device configuration of ITO/ ZnO/ Polymers:PC61BM/ V2O5/ Ag. The solar device based on T2F-PBDTBT-OD/PC60BM blend showed power conversion efficiency (PCE) of 2.63% with a Voc of 0.84 ±0.01V, and Jsc of 4.9±0.54 mA/cm2. In contrast, the T2F-PBDTBT-OT device exhibited a lower PCE of 1.39% and Jsc of 2.41±0.18 mA/cm2 with slightly higher Voc of 0.88 ±0.01V.
In the second part, we synthesized novel two-dimensional conjugated polymer PDTBSeVTT-2TF based on 3,3-difluoro-2,2-bithiophene (2TF) as donor unit and 4,7-di(thiophen-2-yl)benzo[c][1,2,5]selenodiazole (DTBSe) as acceptor unit bearing vinyl-terthiophene (VTT) conjugated side chains along with two 2-octyldodecyl chains and the effect of processing temperature on bulk-heterojunction morphology and photovoltaic performance were investigated. The copolymer PDTBSeVTT-2TF exhibited broad absorption from 300-800 nm and a narrow optical bandgap of 1.57 eV with a deep HOMO of -5.57 eV. Polymer solar cells (PSCs) was fabricated by using [6,6]-phenyl-C71-butyric acid methyl ester (PC71BM) as acceptor and PDTBSeVTT-2TF as donor with an inverted device configuration of ITO/ ZnO/ PDTBSeVTT-2TF:PC71BM/ V2O5/ Ag. The PDTBSeVTT-2TF:PC71BM blend solution were processed at two different temperature 50 °C and 65 °C, respectively. The blend solution processed from the 65°C device exhibited enhanced PCE of 5.03% with a Jsc of 10.99 mA/cm-2 compared with the blend solution processed at 50 °C, which had a PCE of 4.63 % with a Jsc of 10.15 mA/cm-2. This enhancement of PCE is probably due to the increased thermal motion of polymer chains dissociates the PDTBSeVTT-2TF clusters into into single molecules and small aggregates that facilitate the miscibility between the polymer and PC71BM to form nano-scale domains, thus increases the D/A interface and photocurrent.

摘要 i
ABSTRACT iii
致謝 vi
目錄 vii
圖目錄 x
表目錄 xiv
第一章 緒論 1
1.1 前言 1
1.2 太陽光能介紹 2
1.3 太陽能電池歷史 4
1.4 太陽能電池的種類 4
1.5 高分子太陽能電池的工作原理 9
1.6 太陽能電池之特性參數 11
1.6.1 光電轉換效率 11
1.6.2 外部量子效率 13
1.6.3 等效電路模型 14
1.7理想太陽能電池與實際太陽能電池分析 16
1.7.1 理想太陽能電池 16
1.7.2 實際太陽能電池分析 17
第二章 有機高分子薄膜太陽能電池歷史文獻回顧 19
2.1 高分子太陽能電池之結構發展 19
2.1.1 單層結構 20
2.1.2 p-n雙層異質接面結構 21
2.1.3 混摻異質接面結構 24
2.1.4 有序異質接面結構 24
2.1.5 反置混摻異質接面結構 25
2.1.6 反置有序混摻異質接面結構 28
2.1.7 混摻異質接面加入夾層結構 29
2.1.8 疊加式混摻異質接面結構 30
2.2 混摻異質接面之形態控制 31
2.2.1 退火處理 31
2.2.2 溶劑退火效應 33
2.2.3 添加劑效應 33
2.3 共軛高分子 35
第三章 以苯并噻二唑衍生物作為基礎之低能隙聚合物及其太陽能電池之光電特性表現 40
3.1 前言與研究目的 40
3.2 共軛高分子的合成 41
3.2.1 共軛高分子結構 41
3.2.2 共軛高分子性質 42
3.3 結果與討論 43
3.3.1 共軛高分子之電洞遷移率 43
3.3.2 太陽能元件光伏特性分析與比較 44
3.3.3 元件製程最佳化之異質界面型態分析 54
3.3.4 共軛高分子/PC61MB元件之載子遷移率 55
3.5 結論 58
第四章 以苯并硒二唑衍生物作為基礎之低能隙聚合物及其太陽能電池之光電特性表現 59
4.1 前言與研究目的 59
4.2 共軛高分子的合成 62
4.3結果與討論 63
4.3.1 共軛高分子的物理性質 63
4.3.2 共軛高分子之X光繞射圖譜分析 65
4.3.3 太陽能元件光伏特性 66
4.3.4 異質界面型態分析 69
4.3.5 共軛高分子/ PC71MB元件之載子遷移率 71
4.4 結論 73
第五章 實驗方法 74
5.1 太陽能電池之製備流程與方法 74
5.2 實驗儀器量測方法與量測樣品製備 76
第六章 總結與未來展望 79
參考文獻 80

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