臺灣博碩士論文加值系統

本論文以物理吸附的方法來對多層奈米碳管進行表面改質，並將其分散在二氧化鈦薄膜中，作為染料敏化太陽能電池的光電極。在表面改質劑的選擇上，分別為陰離子型的十二烷基苯磺酸鈉(SDBS)及分子量為9350、20800、70000的聚苯乙烯磺酸鈉(NaPSS)，而非離子型表面改質劑則使用兩性三嵌段共聚物(PEG-PPG-PEG)，分別為P123、F68及F108。碳管的表面吸附製程如下，首先於水溶液中將表面改質劑與多層奈米碳管以超音波震盪法進行分散及表面吸附，且將多餘的改質劑利用過濾的方法去除，乾燥後取得表面處理過後的奈米碳管。由UV-vis光譜測定、表面電位分析及粒徑的量測發現，陰離子型表面吸附的碳管在水中之再分散能力比非離子型表面吸附碳管來得好。原因在於陰離子型改質劑具有苯環結構，可與碳管表面進行π-π堆疊。此外，磺酸根離子(SO3-)提供的靜電排斥分散能力比PEG-PPG-PEG的分散力來得大。之後將陰離子型表面吸附碳管分散在二氧化鈦薄膜中，由XRD的結果證實碳管的存在可幫助二氧化鈦結晶形成更多銳態礦相(anatase)，並且使穿透度上升。在染料敏化太陽能電池的元件方面，加入0.03wt%陰離子型表面吸附碳管於二氧化鈦能使短路電流值(Jsc)提升約10~12%。光電流的提升使元件具有較高的光電轉換效率、較佳的電子收集效率及較多的電量，原因來自於碳管能提供良好的導電性、二氧化鈦有較多的anatase相及光穿透度的上升，效率最佳的表現為NaPSS(70000)-MWCNT於添加量為0.03wt%時，短路電流及效率分別為20.68mA/cm2及8.42%。另外，為了進一步提升效率，光電極的外層採用大粒徑的二氧化鈦光散射薄膜，得到最佳短路電流及效率分別為21.44mA/cm2及8.84%。

In this thesis, multi-walled carbon nanotubes(MWCNTs) physisorbing anionic and nonionic dispersing agent for surface modification were dispersed in TiO2 thin film utilizing as a photoelectrode for dye-sensitized solar cells (DSSCs). Anionic dispersing agents such as sodium dodecylbenzenesulfonate(SDBS) and poly (sodium4-styrenesulfonate) (NaPSS) with molecular weight of 9350, 20800 and 70000 were used to disperse MWCNTs. We also chose amphiphilic triblocks of PEG-PPG-PEG as nonionic surface modifying agents, such as P123、F68、and F108. The procedure for surface treatment MWCNTs is as following. Surface modifying agents and MWCNTs were dispersed and adsorbed in water by sonication. After fully adsorption, the solution was filtrated to remove the extra dispersing agents. After drying, the surface-modified MWCNTs were obtained. From the results of UV-vis spectroscopy, zeta potential and dynamic light scattering measurements, anionic surface modifying agents have better dispersing power than nonionic surface modifying agents because anionic agents have benzene ring to physisorb onto CNTs via π-π stacking. Furthermore, the electrostatic repulsion from the SO3- groups leads to the charge stabilization of MWCNTs compared to the nonionic agents. Then we dispersed anion-physisorbed MWCNTs onto the TiO2 system. From the XRD results, we found that TiO2 can crystallize into more anatase structures in the presence of MWCNTs. The resulting materials also had higher light transmittance. For the performance of DSSCs with MWCNT-TiO2 photoelectrode, the addition of 0.03wt% CNT to the TiO2 film could enhance the Jsc of DSSC from 18.65mA/cm2 to 19.26 mA/cm2. And the increase of Jsc resulted in higher power conversion efficiency and better charge collection efficiency because of good conductivity of MWCNTs, more anatase TiO2 crystal structures and higher light transmittance of the MWCNT-TiO2 films. The best Jsc and power conversion efficiency of 20.68mA/cm2 and 8.42% were achieved with MWCNT(70000) dispersing in TiO2. In addition, in order to enhance the light harvesting efficiency, the larger size of TiO2 scattering layer was deposited on the outer layer of MWCNT-TiO2 thin films. After addition of the scattering layer, the Jsc and power conversion efficiency were both increased to 21.44mA/cm2 and 8.84%.

第一章 緒論 1
1-1 前言 1
1-2 染料敏化太陽能電池的發展 2
1-3 染料敏化太陽能電池產業未來研發方向 4
1-4 文獻回顧與探討 4
1-4.1 染料敏化太陽能電池簡介與工作原理 4
1-4.1.1 染料敏化太陽能電池的工作原理.........................................4
1-4.1.2 透明導電基板.........................................................................7
1-4.1.3 染料.........................................................................................8
1-4.1.4 工作電極 ...............................................................................10
1-4.1.5 電解質....................................................................................14
1-4.1.6對電極.....................................................................................16
1-4.2 染料敏化太陽能電池的量測技術與輸出特性 17
1-4.2.1 太陽光譜與光源模擬器........................................................17
1-4.2.2 光電流-電壓特徵曲線.......................................................... 19
1-4.2.3 交流阻抗分析........................................................................20
1-4.2.4 IMPS與IMVS之量測...........................................................22
1-4.2.5 電壓下降與電量收集法........................................................24
1-4.3 奈米碳管簡介 25
1-4.4 奈米碳管的表面修飾法 27
1-4.5奈米碳管於染料敏化太陽能電池工作電極的應用 30
1-5 研究目的 32
第二章 實驗設備與方法 36
2-1 藥品器材 36
2-2 儀器設備 37
2-3 不同分子量NaPSS的製備 38
2-4 表面處理奈米碳管之製作 39
2-5 物理表面改質奈米碳管的性質測試與試片製備 39
2-5.1 TGA 之測試 39
2-5.2 TEM試片製備 39
2-5.3 紫外光/可見光吸收光譜儀樣品的製備 39
2-5.4 粒徑分析 40
2-5.5 表面電位分析 40
2-6 太陽能電池的製作 40
2-6.1 染料溶液的製備 40
2-6.2 液態電解質的製備 40
2-6.3 多層奈米碳管-二氧化鈦複合鍍液的製備 40
2-6.4 光散射二氧化鈦鍍液的製備 41
2-6.5 多層奈米碳管-二氧化鈦工作電極的製備 41
2-6.6 白金對電極的製備 42
2-6.7 元件組合 43
2-7 多層奈米碳管-二氧化鈦的性質測試與試片製備 44
2-7.1 XRD試片製備 44
2-7.2 TEM試片製備 44
2-7.3 紫外光/可見光光譜儀樣品的製備 44
2-7.4 SEM試片製備 44
2-8 太陽能電池的光電化學測試 45
2-8.1 光電流-電壓特徵曲線 45
2-8.2 交流阻抗分析 45
2-8.3 IMVS與IMPS之量測 46
2-8.4 電壓衰退及電量分析實驗之量測 46
第三章 結果與討論 47
3-1 物理表面改質奈米碳管的性質鑑定 47
3-1.1 物理表面改質奈米碳管的分散外觀 47
3-1.2 物理表面改質奈米碳管的TEM鑑定 49
3-1.3 物理表面改質奈米碳管的TGA鑑定 53
3-1.4 物理表面改質奈米碳管的紫外光/可見光吸收鑑定 58
3-1.5 物理表面改質奈米碳管的表面電位分析 60
3-1.6 物理表面改質奈米碳管的粒徑分析 62
3-1.7 綜合討論 65
3-2 陰離子表面改質多層奈米碳管/二氧化鈦複材之鑑定 66
3-2.1 多層奈米碳管/二氧化鈦粉末X光繞射分析 66
3-2.2 多層奈米碳管/二氧化鈦粉末的TEM鑑定 72
3-2.3 多層奈米碳管/二氧化鈦薄膜的穿透度分析 74
3-2.4 多層奈米碳管/二氧化鈦薄膜的SEM分析 77
3-3 陰離子型表面改質多層奈米碳管/二氧化鈦工作電極應用於DSSC的元件表現 80
3-3.1 MWCNT/TiO2 工作電極的元件表現 80
3-3.1.1 光電轉換效率 80
3-3.1.2交流阻抗分析 86
3-3.1.3 IMPS/IMVS分析 96
3-3.1.4 電壓衰退及電量分析 101
3-3.1.5 綜合討論 106
3-3.2 MWCNT/TiO2工作電極引入光散射層的元件表現 107
3-3.2.1 光電轉換效率......................................................................108
3-3.2.2 交流阻抗分析......................................................................126
3-3.2.3 IMPS/IMVS分析.................................................................137
3-3.2.4 電壓衰退及電量分析..........................................................142
3-3.2.5綜合討論 ..............................................................................149
3-4 非離子型表面改質多層奈米碳管/二氧化鈦工作電極應用於DSSC的元件表現 148
3-4.1 MWCNT/TiO2及MWCNT/TiO2工作電極引入光散射層的元件表現......................................................................................................................148
3-4.1.1 光電轉換效率......................................................................148
3-4.1.2 綜合討論..............................................................................149
第四章 結論 154
第五章 參考文獻 156
附錄 167

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