在本研究當中，以水熱法為主要製程方式，首先探討一維氧化鋅奈米線在不同添加物(如：聚乙烯亞胺與氨水)下的成長機制，並藉由螢光光譜與X光吸收光譜界定出缺陷與鋅、氧原子的相關性。之後，相較於傳統批次成長方式，開發連續式反應製程來製備氧化鋅奈米線以進一步控制奈米線品質。製程改善結果顯示：採連續式反應製程所製備的氧化鋅奈米線，在成長時可有效維持反應化學物濃度，提升氧化鋅奈米線材料的結晶性。隨後，利用連續式反應製程系統製備之高結晶性氧化鋅奈米線做為染料敏化型太陽能電池之光陽極並進行相關性能的探討。由研究結果發現：藉由增長長度雖可提高染料吸附量，但長度同時也影響收集效率。若電子擴散係數無法進一步提升，則單純提高奈米線長度將使得整體效率不增反減。此外，當添加氨水於反應系統中來製備氧化鋅奈米線時，除表面缺陷有效下降外，藉由拉曼光譜分析中也發現氮原子可有效進入結構中。此氮摻雜氧化鋅奈米線可使電子擴散係數大幅提升至1.2x10-2 cm2 s-1。利用此電子擴散係數提升之概念將奈米線長度提升至55 μm時，效率可進一步提升至3.92%。然而相較於奈米顆粒為基礎的光陽極系統，高傳輸速率的奈米線系統仍受限於較低的染料吸附面積。因此，在有效長度概念的前提下，於製備好具高電子傳輸性質的氧化鋅奈米線表面進行氧化鋅奈米粒子的磊晶被覆，以做為複合式的氧化鋅光陽極。以此ZnO奈米線/奈米粒子複合結構所製備的光陽極應用於染料敏化型太陽能電池中，在長度13.5 μm的光陽極中，其平均效率可達5.25 %。當長度提升至26.2 μm時，ZnO複合光陽極之最高效率可達7.53 %。最後，針對已吸附染料之複合光陽極進行表面修飾。利用4-叔丁基啶去除多餘的染料以及利用水分子之氫鍵接附於染料為完全鍵結懸鍵上，改善電子傳遞阻力，平均長度13.5 μm之複合式氧化鋅光陽極染料敏化型太陽能電池的效率可由5.25 %分別有效提升至5.71 %﹑6.30 %﹑6.59 %。

In this study, the growth mechanism of ZnO nanowire arrays (ZnO-NWAs) via chemical solution method under different additives, such as: polyethylenimine (PEI) and ammonia (NH3), has been investigated. By using photoluminescence spectroscopy (PL) and X-ray absorption spectroscopy (XAS), the relation between PL emissions, interstitial zinc defects (Zni) interstitial oxygen defects (Oi) has been investigated. To further improve the quality of ZnO-NWAs, unlike the conventional batch process, a facile continuous flow injection (CFI) process has been conducted to synthesize high-quality ZnO-NAWs. According to the study, the concentration of zinc precursor can be maintained at a constant level in CFI process to provide a steady-state growth environment. High quality and long length ZnO-NWAs can be obtained from CFI process to be the photoanode of ZnO based dye-sensitized solar cells (DSSCs). From the results, the increment of length of ZnO-NWAs could effectively improve the dye absorption amount; however, it also influenced the electron collection efficiency (ηCC). To effectively increase the power conversion efficiency (PCE) of DSSCs with long ZnO-NWAs, the diffusion coefficient (Dn) need to improve simultaneously. In this study, NH3 was added into the chemical solution process and it could effectively reduce the surface defects and increase the diffusion coefficient achieved 1.2x10-2 cm2s-1, which was investigated by Raman spectroscopy and electrochemical impedance spectroscopy (EIS) techniques. ZnO-NWAs with length of 55 μm was synthesized via NH3-assised CFI process to use as photoanode of DSSCs and the PCE achieved 3.92 %. To improve the performance of ZnO-based DSSCs furthermore, a low temperature chemical bath deposition (CBD) was employed to decorate ZnO nanoparticles (ZnO-NPs) on the surfaces of ZnO-NWAs photoanodes for increasing dye loading amount. The PCE of ZnO-NWAs/NPs composite DSSC could achieve 5.25 % under the thickness of 13.5 μm. When the thickness of ZnO-NWAs/NPs composite photoanode increased to 26.2 %, the PCE could achieve 7.53 %, which is the highest value in this study. Finally, we also studied the influence of photoanode surface treatment on the performance of DSSCs. In this study, 4-tert-butylpyridine (t-BP) and water vapor were employed as surface modifier. According to the results, the excess dye molecules could be removed by t-BP treatment to avoid the multilayer adsorption and the carrier transport/transfer properties could effectively be improved by water vapor. The PCE could enhanced from 5.25 % to 6.59% via t-BP and water vapor treatment under the photoanode thickness of 13.5 μm.

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