本研究主要著重在固態染料敏化太陽電池的系統建立和應用，並使用新型高吸光苝錯合物作為染料製作高效率電池。固態染料敏化太陽電池(Solid-state Dye-sensitized Solar Cells)，簡稱s-DSSC，有別於一般染敏太陽電池採用的液態電解液，而改以固態電洞傳輸材料(Hole Transporting Material, HTM)作為氧化還原對，s-DSSC的優點包含可避免電解液洩漏及封裝問題、單片式設計可減少電池體積占比以及較短製程時間，然而其效率仍舊低於液態DSSC，歸因於HTM製作過程中於TiO2介孔層內存在孔隙滲透率及固含量多寡問題，導致電池在開路偏壓下(照光狀態)測得電子擴散長度縮短至~2μm，因此須將介孔層厚度減至2μm，但卻減少染料吸附量而導致吸光效率不足，目前可行策略之一為使用具有高消光係數有機染料。
這是我們首次嘗試開發s-DSSC並建構完整製作系統，在第四章中主要針對電池中各項組成材料進行優化處理，隨後基於上述優化技術，在第五章中我們介紹一系列不同推-拉電子能力(D-π-A)的苝錯合物作為染料，並分別搭配碘電解液(I-/I3-)及Spiro-OMeTAD製作液態和固態染敏電池。其中，具有多重推-拉電子(D-A-π-A)的苝染料GJ-BP，除了具有高消光係數(在541nm波長處為35400 M-1 cm-1）及延伸至700nm光譜，使其在液態及固態染敏電池中的平均效率分別達到6.0%及4.6%之外，針對抑制電子-氧化電解質再結合及其他影響效率的因素，透過電化學阻抗分析及電子密度空間分布計算，顯示GJ-BP具有優異的再結合阻抗、電子壽命及電荷收集效率，與常見的釕金屬染料相比更適用於s-DSSC。最後在第六章中，著眼於s-DSSC的實用性，設計出一種嵌入s-DSSC和指叉對稱式二氧化錳電容的光電裝置，透過電路設計整合於同一基材，裝置搭配高吸光Y123染料(530nm為48000 M-1 cm-1) 測得在AM1.5G太陽光下具有0.91V的VOC值和3.80%的轉換效率；而在室內光T5燈(6000lux)下，因其光源輻射範圍與染料吸光光譜具有高匹配性而可提升至10.52 %；在電容部分，以簡易電沉積製作並經優化後的MnO2電容，在充放電測試中測得其平均電容值約為13.2 mF cm-2，與s-DSSC整合後裝置分別在太陽光及T5室內光環境下進行充放電測試並探討其充放電效率。

In this study, we investigated high photovoltaic performance of perylene derivatives as dyes used in optimized solid-state dye-sensitized solar cells (s-DSSC). s-DSSC was attractive for its ignorable leakage problem by employing the hole-transporting material (HTM) instead of conventional liquid electrolyte. Generally, the light harvest capability of a s-DSSC was lower than its liquid-electrolyte counterpart because the mesoporous TiO2 film of a s-DSSC was thinner than that of a liquid-type DSSC in order to allow satisfactory penetration of HTM. To solve this problem, one of the viable tactic was the use of dyes with high extinction coefficient and broad spectral response, targeting to enable high ligh harvesting capability within a thin film.
It was our first time to fabricate the s-DSSC and to build its optimization system. Therefore, in chapter 4 we used progressive optimization toward each component in s-DSSC. Based on aforementioned optimized techniques, in chapter 5 we introduced a series of D-π-A designed perylene derivatives as dyes used in I-/I3--based liquid-DSSC and spiro-OMeTAD-based s-DSSC respectively. In particular, the D-A-π-A designed perylene dye called GJ-BP featured better extinction coefficenct (ε of 35400 M-1 cm-1 at wavelength of 541nm) and exceptional spectral broadening to 700nm wavelength, leading to the conversion efficiencies of 6.0% and 4.6% in liquid- and solid-DSSC respectively. In addition, other factors that influenced the efficiency such as recombination occurring at TiO2-electrolyte interface were elucidated by using electrochemical impedance spectroscopy and spatial distributed calculation. The results showed that GJ-BP-sensitized s-DSSC has enhanced charge recombination resistance, electron lifetime, and charge collection efficiency in comparison with Ruthenium dye-sensitized s-DSSC. In chapter 6, it was concerned with s-DSSC in practical application. We attempted to design an on-chip photocapacitor embedding with a s-DSSC and a MnO2-based symmetric interdigitated supercapacitor. By modulating electrical circuit design, the integrating platform with energy generation and storage was successfully established. The preliminary results showed that s-DSSC sensitized with Y123 dye (48000 M-1 cm-1 at 530nm) obtained the open-circuit voltage (VOC) of 0.91V and efficiency of 3.80% under one sun condition and 10.52 % under 6000-lux indoor T5-lamp environment, respectively. The capacitance of MnO2-based supercapacitor was measured about 13.2 mFcm-2 by charge-discharge test. Subsequently the charging efficiency of the integrated device under solar and indoor light condition was further investigated.

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