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研究生:沈育仁
研究生(外文):Yu-Jen Shen
論文名稱:CdS量子點敏化劑及高分子/奈米粒子複合膠態電解質在染料敏化太陽能電池應用之研究
論文名稱(外文):Applications of CdS Quantum-Dot Sensitizer and Hybrid Polymer/Nanoparticle Gel-State Electrolyte on Dye-Sensitized Solar Cells
指導教授:李玉郎
指導教授(外文):Yuh-Lang Lee
學位類別:博士
校院名稱:國立成功大學
系所名稱:化學工程學系碩博士班
學門:工程學門
學類:化學工程學類
論文種類:學術論文
論文出版年:2008
畢業學年度:96
語文別:中文
論文頁數:194
中文關鍵詞:奈米碳管表面改質CdSLB 沈積技術PVDF-HFP石墨染料敏化太陽電池量子點
外文關鍵詞:Dye-Sensitized Solar CellCdSQuantum dotsurface modificationLangmuir-Blodgett techniquegraphite and carbon nanotube
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  • 被引用被引用:5
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本研究以微乳化系統合成CdS量子點,並利用十二碳硫醇(dodecanethiol)及琥珀酸硫醇(Mercaptosuccinic acid,MSA)分子進行量子點表面改質,分別製作疏水性量子點粒子(C12-CdS)與含羧酸基的親水性量子點(MSA-CdS),其中利用CTAB物理吸附於MSA-CdS可提高量子點的移動性,可利用LB沈積技術精確控制層數來製備多層的CdS量子點薄膜。此外,在TiO2組裝CdS量子點的太陽電池研究中,利用3-硫醇基矽丙烷(3-Mercaptopropyl trimethoxysilane,MPTMS)及3-胺基甲基二乙氧基矽丙烷(3-Aminopropylmethyl diethoxysilane,APMDS)對TiO2表面改質使TiO2具有硫醇基(-SH)與胺基(-NH2),可與CdS反應提高CdS 量子點的吸附量,但易造成TiO2電極孔洞阻塞。而利用MSA-CdS直接利用羧基在未改質TiO2表面吸附形成單層且高覆蓋率結構,可避免阻塞TiO¬2孔洞與抑制暗電流發生。由IPCE效率分析顯示,於400nm光波長下以MSA-CdS直接吸附於未改質TiO2效率約20 %,而MPTMS與APMDS改質的TiO2吸附CdS則分別為13%及6%。在光電轉換總效率分析上MSA-CdS吸附於未改質TiO2效率可達0.30%,而CdS吸附於MPTMS與APMDS改質的TiO2¬則約為0.19%
另一方面,本研究亦利用PVDF-HFP高分子分別混摻TiO2、奈米碳管及石墨等無機奈米粒子製作膠態電解質,並組裝應用於太陽電池中,探討無機奈米粒子對電池轉換效率影響。實驗結果發現奈米粒子可降低高分子結晶度與減低離子移動活化能而提升導電度。由電化學阻抗分析發現,高分子混摻TiO2可改善膠態電解質與TiO2電極間的接著,但亦會導致白金電極界面電荷轉移電阻增加與漏電情形發生,而混摻奈米碳管與石墨粒子可抑制電子與電洞再結合發生,可提升光電流。在太陽電池光電轉效率分析中,PVDF-HFP未添加奈米粒子製備之電解質所測得的電池效率約為4.69%,而PVDF-HFP混摻0.5% TiO2奈米粒子效率可提升至5.19%;而混摻0.3%奈米碳管時為5.92%;而混摻0.2%石墨奈米粒子可將效率提升至6.04%,接近液態太陽電池的效率值。
In this study, Cadmium sulfide (CdS) quantum dots (QDs) were prepared by microemulsion process and surface modified by dodecanethiol or mercaptosuccinic acid (MSA) to render a surface with hydrophobic alkyl chains (C12-CdS) or hydrophilic carboxylic acid groups (MSA-CdS), respectively. For the MSA-CdS QDs, the surface was hydrophobized through physical adsorption of cetyltrimethyl ammonium bromide (CTAB) which improved the stability and mobility of the QDs at the air/water interface. The CTAB-MSA-CdS QDs could be used to prepare multilayer of CdS QD films using Langmuir-Blodgett (LB) technique. Moreover, the CdS was assembled onto TiO2 mesoporous surface for dye-sensitized solar cells (DSSCs) application. TiO2 was surface modified by 3-mercaptopropyl trimethoxysilane (MPTMS) or 3-aminopropyl-methyl diethoxysilane (APMDS), respectively, to prepare a thiol or amino terminated surface for binding with the CdS. The interaction of CdS to the thiol and amino groups leads to a higher adsorption amount of CdS. However, the fast adsorption rate leads to blocking of mesopores, resulting a poor performance of the cell. On the bare TiO2 film, CdS QDs have a lower adsorption rate and incorporated amount of CdS were obtained, but a better-covered QDs monolayer was resulted. The incident photon-to-current conversion efficiency (IPCE) obtained at 400 nm for the CdS-sensitized TiO2 electrode were about 20%, 13% and 6%for the bare-TiO2, MPTMS-TiO2 and APMDS-TiO2, respectively. The total energy conversion efficiency were 0.30% for bare TiO2, 0.19% for MPTMS-TiO2 and APMDS-TiO2.
On the other hand, the PVDF-HFP was blending with nanofillers (TiO2, carbon nanotube and graphite) to prepare polymer gel electrolyte (PGE) for DSSC application. Graphite nanoparticle was proved to be a more efficiency filler, than TiO2 and carbon nanotube, in enhancing the charge conductivity of the PGE, decreasing the activation energy for charge transport, and inhibit the charge recombination at the TiO2/electrolyte interface. The energy conversion efficiency of a DSSC fabricated using a PGE containing 0.25 wt% of graphite can be increased from 4.69% (without filler) to 6.04%, close to that of a liquid system obtained in this work.
摘要 I
Abstract III
謝誌 V
總目錄 VII
表目錄 XII
圖目錄 XIV
第一章 緒論 1
1-1 前言 1
1-2 太陽能電池發展現況 2
1-3 研究目的與動機 6
第二章 文獻回顧 8
2-1 半導體奈米材料與量子點 8
2-2 量子點的特性 9
2-2-1 量子侷限效應 10
2-2-2 衝擊離子化效應與歐傑再結合效應 13
2-2-3 迷你傳送帶效應 14
2-3 量子點的合成 16
2-3-1 液體溶膠法 16
2-3-2 微乳化法 17
2-4 CdS量子點薄膜的製備與組裝 20
2-4-1 奈米粒子薄膜的製備與組裝 20
2-4-2 LB沈積技術製備CdS奈米粒子薄膜 22
2-5 染料敏化太陽電池 24
2-5-1 DSSC之工作原理 25
2-5-2 DSSC組件介紹 26
2-5-3 DSSC之沿革及發展現況 31
2-5-4 半導體量子點粒子在DSSC的應用 33
2-5-5 膠態與固態電解質 34
第三章 實驗技術與原理 38
3-1 實驗藥品 38
3-2 實驗流程 40
3-3 CdS量子點的合成與表面改質 41
3-3-1 CdS量子點的合成 41
3-3-2 CdS量子點的表面改質 42
3-4 LB沈積技術(Langmuir Blodgett Technology) 43
3-4-1 單分子層的等溫線行為 44
3-4-2 CdS量子點粒子層鬆弛曲線分析 47
3-4-3 CdS量子點粒子層遲滯曲線分析 48
3-4-4 Langmuir-Blodgett(LB)粒子膜 49
3-5 布魯斯特角顯微鏡(Brewster angle microscope,BAM) 52
3-6 原子力顯微鏡(Atomic Force Microscope,AFM) 56
3-7 紫外光-可見光吸收光譜(UV-Vis spectroscopy) 59
3-8 CdS量子點敏化太陽電池 61
3-8-1 透明導電玻璃基板的清洗 62
3-8-2 TiO2膠體溶液的製備 63
3-8-3 TiO2光電極的製備 63
3-8-4 TiO2光電極上光敏化劑(N719或CdS量子點)的吸附組裝 64
3-8-5 I-/I3-碘系統液態電解液配製 65
3-8-6 膠態電解質的製備 65
3-8-7 電池組裝程序 66
3-9 太陽電池光電效率分析 68
3-9-1 光電轉換效率分析 70
3-9-2 入射光電轉換效率(Incident Photon to Charge Carrier Efficiency,IPCE)分析 74
3-10 電解質電性分析 76
3-10-1 循環伏安測試(cyclic voltammogram,CV) 76
3-10-2 導電度分析 78
3-11 DSSC電化學阻抗分析(Electrochemical Impedance Spectroscopy,EIS) 82
第四章 實驗結果與討論 85
( I ) CdS無機量子點合成與其在DSSC敏化劑的應用 85
4-1 CdS量子點的合成、表面改質與量子點特性分析 85
4-1-1 CdS量子點的合成 85
4-1-2 CdS量子點的表面改質 88
4-2 CdS量子點的等溫線分析 93
4-3 CdS量子點的布魯斯特角顯微鏡(BAM)影像分析 98
4-4 CdS量子點粒子膜鬆弛曲線分析 103
4-5 CdS量子點粒子膜遲滯曲線分析 105
4-6 CdS量子點粒子薄膜表面型態分析 107
4-7 CdS量子點粒子LB多層膜的製備 112
4-8 CdS量子點在TiO2薄膜上的組裝分析 115
4-8-1 CdS量子點在TiO2上的吸附動力學與UV-Vis吸收度分析 117
4-8-2 CdS量子點吸附於不同官能性玻璃表面上的表面型態分析 120
4-9 CdS量子點敏化太陽電池光點轉換效率分析 124
4-9-1 入射光電轉換效率(IPCE)分析 124
4-9-2 太陽電池光電效率分析與暗電流分析 126

( II ) PVDF-HFP膠態高分子電解質在太陽電池上的應用 131
4-10 PVDF-HFP膠態高分子電解質性質分析 131
4-10-1 DSC結晶度分析 132
4-10-2 高分子電解質表面型態分析 135
4-11 膠態電解質之光電轉換效率分析 139
4-12 極限擴散電流分析 147
4-13 導電度分析 151
4-13-1 奈米粒子對高分子導電度之影響 151
4-13-2 高分子電解質活化能之探討 155
4-14 交流阻抗分析 157
4-14-1 模擬太陽光照射下太陽電池之交流阻抗分析 157
4-14-2 黑暗中太陽電池之交流阻抗分析 165
第五章 結論與未來展望 172
( I ) CdS無機量子點合成與其在DSSC敏化劑的應用 172
( II ) PVDF-HFP膠態高分子電解質在太陽電池上的應用 173
第六章 參考文獻 174
附錄一 多層Langmuir-Blodgett分子膜之沈積型式 190
作者簡介 192
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