臺灣博碩士論文加值系統

本研究嘗試以製程簡易且成本便宜之碳材料製作對電極催化層，應用於[Cu(II/I)(dmby)2]TFSI2/1錯合物電解質之染料敏化太陽能電池（Dye-Sensitized Solar Cell，DSSC）。使用包含鉛筆塗層、蒸鍍石墨基材、石墨烯與多壁式奈米碳管等碳材，探討催化層特性對於光電轉換效率之關鍵影響參數，同時比較不同光照強度下，催化層之阻抗特性對於整體光電轉換效率影響之差異。
本研究以拉曼光譜儀分析不同碳材料的結構，以掃描式電子顯微鏡（SEM）觀察催化層於FTO導電玻璃的覆蓋與分佈情形，以電化學阻抗分析（EIS）分析催化層之異質傳輸阻抗與介面間之串聯電阻，結合其組成DSSC之光伏參數，進行統整性比較。歸納結果發現，在低光時，催化層擁有較高的串聯電阻(RS)與較低的異質傳輸阻抗(RCT)較為理想，因為在低光下的漏電與再結合行為嚴重，對光伏數據有很大的負面影響，若催化層有較高的RS，則可以防止電荷回流至對電極，有助於提升電池性能，另方面RCT直接關係到催化效率，當RCT越低則電荷傳輸效率越佳。本研究測試之材料中，多壁式奈米碳管由於其高比表面積與微結構具有高比例的懸鍵(dangling bond)，而dangling bond又是與電解質鍵結並傳遞電子的關鍵結構，因此奈米碳管系列樣品具有較多的催化位址，其RCT值也是所有樣品中最低，在本研究測試之碳材料中具有最佳催化效率，在200 Lux光強下的光電轉換效率可達20.2 %，高於傳統Pt對電極催化層（16.6 %）。然而在光通量提高時，電子再結合作用與漏電的負面影響比例逐漸降低，此時RCT成為主導電池的光伏數據表現的關鍵因素。

Copper-complex redox couple is known as efficient electro-transfer mediator that exhibit low driving force for dye regeneration. Even though [Cu(II/I)(dmby)2]TFSI2/1 complex coupling with Y123 dye demonstrates a highest theoretical photovoltage over 1.0 V in liquid-electrolyte based DSSCs, the rapid electron self-exchange rate of copper-complexes requires a higher efficient catalytic counter-electrode. In this work, two carbon-based materials, graphite and multi-wall carbon nanotubes (MWCNTs), were respectively used as catalyst layer onto the FTO glass serving as counter-electrode and their electro-catalytic activities were carefully examined. The charge transfer resistance (RCT) at the electrolyte/electrode interface and the serial resistance (RS) of counter-electrode were investigated by Electrochemical Impedance Spectroscopy (EIS). The results showed that MWCNTs exhibits a lowest RCT, that allow a highest electron transfer rate, in comparison with the other carbon materials used in the present work. Briefly, the DSSC composed of MWCNTs as catalytic counter electrode demonstrated a high photovoltage up to 0.8 V and an overall high PCE at 20.2% under dim light condition (200 Lux).

中文摘要 I
Abstract II
誌謝 XV
目錄 XVII
圖目錄 XX
表目錄 XXV
第一章、 緒論 1
第二章、 文獻回顧與理論基礎 3
2.1.1染料敏化太陽能電池工作原理 3
2.1.2染料敏化太陽能電池結構 5
2.2銅系統電解液與對電極催化層 18
2.3染料敏化太陽能電池室內應用 25
2.4研究動機與目的 27
第三章、 實驗步驟與方法 28
3.1實驗藥品 28
3.2實驗流程 30
3.2.1工作電極製備 30
3.2.2對電極製備 31
3.2.3染料敏化太陽能電池封裝 33
3.3工作電極分析 36
3.3.1紫外可見光分光光譜儀(UV-Visible Spectrophotometer) 36
3.4對電極催化層性質分析 37
3.4.1掃描式電子顯微鏡(Scanning Electron Microscope, SEM) 37
3.4.2拉曼光譜分析儀(Raman Spectroscopy) 37
3.4.3循環伏安法量測(Cyclic Voltammetry, CV) 39
3.5染料敏化太陽能電池元件檢測儀器 40
3.5.1室內光源模擬器 40
3.5.2太陽光模擬器 43
3.5.3入射單色光子-電子轉換效率(IPCE) 44
3.5.4電化學交流阻抗頻譜分析(EIS) 45
第四章、 結果與討論 51
4.1銅系統電解液DSSC性能表現 51
4.1.1銅錯合物電解質 51
4.1.2 [Cu(II/I)(dmby)2]TFSI2/1錯合物對染料選擇性 54
4.1.3 Pt對電極催化層 59
4.2鉛筆塗層對電極催化層 61
4.2.1對電極催化層性質分析 61
4.2.2以鉛筆塗層組成DSSC之光伏參數 63
4.2.3催化層之阻抗分析 64
4.3蒸鍍石墨基質材料對電極催化層 70
4.3.1對電極催化層性質分析 70
4.3.2室內光(200 Lux)DSSC光伏性能表現 72
4.3.3催化層之阻抗分析 73
4.4石墨烯對電極催化層 76
4.4.1對電極催化層性質分析 76
4.4.2室內光(200 Lux)DSSC光伏性能表現 78
4.4.3催化層之阻抗分析 79
4.5奈米碳管對電極催化層 82
4.5.1對電極催化層性質分析 82
4.5.2室內光(200 Lux)DSSC光伏性能表現 85
4.5.3催化層之阻抗分析 86
4.6 PEDOT對電極催化層 90
4.6.1對電極催化層性質分析 91
4.6.2室內光(200 Lux)DSSC光伏性能表現 91
4.6.3催化層之阻抗分析 92
4.7 DSSC光伏性能表現綜合討論 96
4.7.1低光光強遞增之DSSC光伏性能表現 96
4.7.2高光強遞增之DSSC光伏性能表現 100
4.7.3 DSSC效能穩定性測試 105
第五章、 結論 108
參考文獻 111

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