本研究成功研發出 CuS@g-C3N4 與 CuxSe@g-C3N4 複合材料並作為背電極應 用於量子點敏化太陽能電池(Quantum Dot Sensitized Solar Cells, QDSSCs)，其中 作為背電極材料的 CuS@g-C3N4 與 CuxSe@g-C3N4 具有出色的導電性、電催化活 性以及比表面積，使 QDSSCs 有著傑出的效能。在實驗中選用具良好導電性與高 化學穩定性的氧化銅(Copper oxide, CuO)作為背電極材料，接著加入石墨氮化碳 材料(Graphic Carbon Nitride, g-C3N4)提升比表面積與增加更多的電子傳輸通道， 最後以陰離子置換法將硫(Sulfur)與硒(Selenium)元素添加至背電極中，賦予其優 異電催化的效果，製備出 CuS@g-C3N4 與 CuxSe@g-C3N4 複合材料背電極，其光 電轉換效率值(Power Conversion Efficiency, PCE)由原條件之 CuO 背電極的 7.94% 分別提升至 9.71%與 9.41%。
本篇研究中也會進行背電極材料的組成與整體形貌之鑑定。起初先以 XPS 與 FTIR 證明 g-C3N4 與三-三嗪基(Tris-triazine-based)的組成結構有相符之鍵結; 接著利用 XRD、SEM、HR-TEM 與 Mapping，來佐證添加 g-C3N4 與陰離子交換 反應而產生之形貌與元素組成的改變。此外研究中也針對不同背電極材料進行電 化學的檢測，包含 EIS、Tafel 和 CV，其中 CuS@g-C3N4 與 CuxSe@g-C3N4 都有 優異的電催化表現，表示添加 g-C3N4 與陰離子交換反應能有利於電子的傳遞與 背電極的催化，以此提升 QDSSCs 的整體效能;最後實驗也進行了 QDSSCs 的 穩定性測試，CuxSe@g-C3N4 表現了最良好的穩定性，QDSSCs 製備後存放 300 小時仍有原始效率的 60%。

In the present study, a morphology-controlled CuS@g-C3N4 and CuxSe@g-C3N4 composites were successfully developed using a facile nanocomposite engineering approach and subsequently used as electrocatalysts for quantum dot-sensitized solar cells (QDSSCs). First, hierarchically assembled copper oxide (CuO) nanostructures are synthesized using microwave-assisted synthesis. These CuO are then embedded within graphitic carbon nitride material (CuO@g-C3N4) to improve the specific surface area and increase electron transport channels. Subsequently, sulfur and selenium have been incorporated into the counter electrode via an anion exchange strategy, making composite electrocatalysts (CuS@g-C3N4 and CuxSe@g-C3N4) with enhanced electrocatalytic activity. When employed as a counter electrode (CE) in QDSSCs, both the CuS@g-C3N4 (9.41%) and CuxSe@g-C3N4 (9.71%) composites outperform the CuO (7.94%), in terms of power conversion efficiencies (PCE). Notably, both the CuS@g-C3N4 and CuxSe@g-C3N4 have shown remarkable electrochemical and device stability in polysulfide redox couple electrolytes.
In conclusion, we have used a two-stage method to develop efficient and stable CuS@g-C3N4 and CuxSe@g-C3N4 electrocatalysts. The 3D carbon network in these catalysts is porous and has improved surface properties, making it electrically conductive and useful. These electrocatalysts have demonstrated that these CEs photovoltaic performance and surface morphologies are composition-dependent. At first, XPS and FTIR were used to prove that g-C3N4 and tris-triazine-based had the same bonding structure; then XRD, SEM, HR-TEM, and Mapping were used to prove the addition of g-C3N4 changes in morphology and elemental composition resulting from anion exchange reactions. In addition, the electrochemical detection of various counter electrode materials was carried out using EIS, Tafel, and CV analysis. Accordingly, CuS@g-C3N4 and CuxSe@g-C3N4 exhibited excellent electrocatalytic performance, indicating that the addition of g-C3N4 and anion exchange reaction energy is beneficial to the transfer of electrons and the catalysis of the counter electrode, thereby improving the overall performance of QDSSCs. In terms of stability, CuxSe@g- C3N4 was found to be the most stable electrocatalyst retaining its 60% of original efficiency after 300 hours of storage.

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