隨著時代的發展，石化能源的持續消耗以及環境汙染問題日益嚴重，導致能源危機的問題長期以來一直受到重視；因此，如何有效率地利用再生能源變成全世界討論的一個重要議題。在眾多再生能源中，穩定且龐大的太陽能是最受到矚目的永續替代能源，具備高轉換效率、低成本且無排放等優點的光伏電池成為所有的再生能源技術中最有潛力的一項技術。因此，本論文主軸將著重於開發高效能且高穩定性之電極材料應用於量子點敏化太陽能電池及敏化光充電儲能元件中來提升太陽能取代傳統石化能源的可行性。
擁有高消光係數的量子點被廣泛應用於敏化太陽電池中的光敏化層且具有高達44%的理論光電轉換效率，因此吸引學者們將其視為極具潛力的研究領域。然而，開發高效率的量子點敏化太陽能電池須具備高電催化活性的對電極才能有效還原電解液中的氧化還原對並進一步提供量子點再生的功能。因此，本論文的第4章中將利用氧化還原沉積薄膜技術用於製備雙金屬鈷錳硫化物對電極應用於量子點敏化太陽能電池；首先，利用過錳酸鉀作為表面錨定氧化劑與溶液中的醋酸鈷產生表面氧化還原反應進而於導電玻璃表面上形成鈷錳氧化物，此沉積技術不受限於基材材質及其表面粗糙度，具備成本低、可低溫操作、易於大面積製作且元素均勻度高等優勢。錳與鈷能產生協同效應進而增加其雙金屬氧化物的導電性並產生額外缺陷來提供更多的活性位點，基於上述導入錳於氧化鈷的優勢，本研究將進一步透過硫化將鈷錳氧化物轉化為鈷錳硫化物來提升其電催化能力。經由最適化控制鈷錳前驅物的比例進而探討不同雙金屬比例下鈷錳硫化物於多硫氧化還原對的還原能力，其結果顯示最適化的鈷錳硫化物(5:1)對電極在100 mW/cm2光照強度下，其元件效能可達到5.88±0.19%。此外，經過長圈數循環伏安法測試(50圈)，鈷錳硫化物電極所組成的元件之光電流保留率(90%)相較於傳統硫化銅電極(30%)展現出更好的穩定性。本章節研究提供一種簡易製程的雙金屬鈷錳硫化物薄膜對電極應用於實現高效能與高穩定性之量子點敏化太陽能電池。
另一方面，為了克服太陽能電池具有間歇性供電的先天問題，許多研究團隊開始嘗試將太陽能電池與儲能元件兩種元件結合進而發展出全新型態的光驅動充電儲能系統。然而，元件串聯電阻所造成的能量損耗以及複雜的線路設計使得此種系統在實務應用上的限制與挑戰。有鑑於此，發展兼具光電轉化能力與儲能效果的雙功能光驅動充電儲能元件是極具有潛力的研究。因此本論文的第5章設計一種新穎兩極式結構之敏化光充電離子電容器，提出利用兼具電催化能力與儲能效果的奈米碳管雙功能電極來實現光驅動充電儲能元件能兼具染料敏化太陽能電池(創能)與離子電容器(儲能)的功能。在敏化光充電離子電容器中，光陽極由染料敏化層與三氧化鎢儲能層(負極)所組成，另一端電極則使用奈米碳管作為兼具電催化能力與儲存電荷(正極)的雙功能電極。具有高比表面積且良好導電性的奈米碳管備廣泛應用於染料敏化太陽能電池的對電極電催化層以及超級電容器的儲能層。本研究結果顯示最適化奈米碳管雙功能電極能使敏化光充電離子電容器之光伏效能達到2.38%且具有2.57 uAh/cm2的儲能效果。在5分鐘的光驅動充電中，使用奈米碳管雙功能電極的元件可提供穩定的光伏電壓(0.70 V)，在閉光操作下仍可維持0.45 V的開路電壓，顯示奈米碳管比傳統白金更適合應用於敏化光充電離子電容器。在實際應用方面，本研究使用4顆元件串聯可提供高達1.80V左右的光電壓來驅動單一LED並可於室內弱光下提供穩定電壓輸出持續驅動LED燈。本章所提出的新式敏化光充電離子電容器可於戶外強光下直接作為太陽能電池將太陽能轉成電能應用於電子元件或儲存於元件的儲能層中；在室內弱光下則可利用儲能層驅動電子元件並透過染敏電池於弱光下的高轉換效率來持續維持充電。綜合上述敏化光充電離子電容器的優點，未來將可整合雙功能光驅動充電儲能元件於穿戴式電子元件中實現永續光驅動穿戴式元件的願景。

The continous increase of energy demand and the fossil fuel dependence has caused severe environmental pollution problems. Thus, the effective and efficient use of renewable energy become so much important worldwide. Solar energy is the most attractive sustainable alternative energy nowadays. At such, photovoltaic cells with high efficiency, low cost, and zero emission have become the most potential technology among all renewable energy technologies. Therefore, this research will focus on developing high stability and efficiency electrode materials for quantum dot-sensitized solar cells (QDSSCs) and sensitized photorechargeable ion capacitors (SPICs) to improve the feasibility of replacing traditional fossil fuels with solar energy.
Quantum dots with high extinction coefficient are frequently employed in the photosensitizing layer of QDSSCs, drawing researchers' interest as a prospective research subjects. However, developing high-efficiency QDSSCs requires counter electrodes (CEs) with high electrocatalytic activity to reduce the redox couple and further regenerating quantum-dot in the polysulfide electrolyte. Herein, Chapter 4 will describe the facile redox deposition fabricated the Cobalt Manganese sulfide (CMS) as CEs for QDSSCs. In brief, the potassium permanganate act as the surface anchoring oxidant that reacts with the cobalt acetate via surface redox reaction and then deposits the cobalt manganese oxyhydroxide (CMOH) on the substrate. Co and Mn can synergistically increase the conductivity of the CMOH and create defects to provide more active sites. Taking the advantages of abovementioned, the CMOH is then sulfurized to improve its electrocatalytic activity. By controlling the precursor ratio of Co and Mn, the CMS could be adjusted to manipulate the electrocatalytic activity for Sn2- reduction. As a result, the QDSSCs with an optimized CMS (5:1) CEs exhibit a high η of 5.88± 0.19% under 100 mW/cm2 irradiation. Furthermore, after 50th scanning cycles of cyclic voltammetry, the photocurrent retention rate of the QDSSCs composed of the CMS CE (90%) showed better than that of CuS CE (30%) in the stability test. This chapter revealed the simple redox deposition of CMS thin film, which possessed superior reduction activity to Sn2- at the CE/electrolyte interface.
On the other hand, to overcome the inherent problem of intermittent power supply of solar cells, many researchers have tried to combine solar cells and energy storage devices to develop a new type of solar-driven charging storage system. However, the energy loss caused by the series resistance of the components and the complicated circuit design made a limitation and challenge in practical application. Because of this, the dual-function solar-driven charging storage device with photo-conversion capability and energy storage ability has been an attractive topic lately. In Chapter 5, a novel dual-electrode of SPICs is designed by introducing a bifunctional carbon nanotubes (CNTs) electrode with electrocatalytic and energy storage ability for realizing solar-driven charging storage device. In SPICs, the photoanode is composed of a dye-sensitized layer of N719/TiO2 and a energy storage layer of WO3. The other bifunctional electrode utilizes CNTs with electrocatalytic ability and ion storage capability. CNTs with high specific surface area and good electrical conductivity are widely used in the electrocatalytic layer of dye-sensitized solar cells and the energy storage layer of supercapacitors. As a result, the optimized bifunctional CNTs electrode can achieve a photovoltaic efficiency of 2.38% and an energy storage effect of 2.57 uAh/cm2 for SPICs. During 5 minutes of photocharging, the SPIC with bifunctional CNTs electrodes can provide a stable photovoltage (0.70 V) and maintain at 0.45 V under closed light, showing that CNTs are more suitable for use in SPICs, compare with traditional Pt. Furthermore, connected with four series SPICs provide a photovoltage of up to 1.80V to drive a single LED and continuously drive LED lights under indoor light by the stable voltage output. Combining the advantages of the SPICs, the vision of sustainable solar-driven devices can be realized by integrating dual-functional SPICs into wearable electronic devices in the future.

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