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研究生： 張婷維
Ting-Wei Chang
論文名稱： 以異質結構背電極開發高效穩定性之量子點敏化太陽能電池
Efficient and stable quantum dots-sensitized solar cells through heterostructured counter electrodes
指導教授： 張家耀
Jia-Yaw Chang
口試委員: 江佳穎
Chia-Ying Chiang
林正嵐
Cheng-Lan Lin
學位類別： 碩士
Master
系所名稱： 工程學院 - 化學工程系
Department of Chemical Engineering
論文出版年： 2021
畢業學年度： 109
語文別： 中文
論文頁數： 128
中文關鍵詞： 量子點敏化太陽能電池 、背電極 、量子點
外文關鍵詞： Quantum dots-sensitized solar cell, Counter electrode, Quantum dots
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  •  上一筆

    • 本研究使用二步合成法，其中包含了網印法與液滴塗佈法。PART I為網印法，先使用微波輔助合成法，合成CuS奈米材料，藉由網印法搭配高溫燒結，得到CuxS背電極。此製程優勢在於透過微波輔助法可以快速合成材料且精確調控材料晶型，並藉由網印法控制薄膜厚度，同時，使用高溫燒結能提高材料的結晶性，以及能使材料更穩固的貼附於導電玻璃上。透過SEM材料分析得知經微波輔助合成法得到類棒狀結構的CuS奈米材料，經網印高溫燒結後得到網狀結構的CuxS。另外，CuxS 背電極經由XRD結構分析得知，CuxS由CuS與Cu2S所構成。由電池量測穩定性分析也證實相較於傳統化學浴沉積法能有效提高電池的壽命。除此之外，此方法也可以製作出PbxS、NixS與CoxS背電極，經元件測試得知，CuxS背電極為最高光電轉換效率7.24 %，其他背電極的光電轉換效率分別為PbxS的5.20 %、NixS的1.94 %及CoxS的3.12 %。
    PART II為液滴塗佈法，將Se前驅物披覆在CuxS背電極上，藉由不同材料Ksp的差異，形成CuxS@CuxSe異質結構。當Se前驅物加入20 L於CuxS背電極時，具有最高光電轉換效率8.02 %，其中以FF值上升最多由49.6 %上升至54.5 %。因此，藉由電化學分析證實在CuxS外殼形成CuxSe結構，有利於電子的傳遞與背電極的催化，同時，此結構有助於Se2-解離至多硫化物電解液中，形成多硒硫化物電解液，利於清除量子點價帶上的電洞。透過電池量測穩定性分析證實，藉由CuxS@CuxSe結構，量測至120 hrs仍有原光電轉換效率的一半。

     

    In this paper, we adopted a two-step synthesis method that involves screen printing and drop coating techniques to improve the traditional process. In Part I, we introduced the basics of screen printing. The CuS electroatalyst was first synthesized using a microwave-assisted synthesis, followed by screen printing and annealing to obtain the CuxS counter electrode (CE). Screen printing were found to be useful in adjusting film thickness, and making the material more stable on FTO glass substrate, respectively. According to SEM and XRD results, the combination of CuS and Cu2S produced CuxS CE with net-like morphology. The stability analysis of power conversion efficiency (PCE) data suggests that this approach can greatly extend cell lifetime when compared to chemical bath deposition. Furthermore, this method can produce CEs from PbxS, NixS and CoxS. Device measurements show that, in comparison with other counter electrodes, the maximum PCE value of 7.24 % was shown by CuxS CE.
    In Part II, a CuxS@CuxSe heterostructure CE was fabricated utilizing the drop-casting technique, in which Se precursor was incorporated on the CuxS CE. The maximum PCE of 8.02 % was obtained when only 20 L Se precursor were added to CuxS CE. The CE's electrodynamic behavior was investigated using electrochemical impedance spectroscopy (EIS), Tafel, and cyclic voltammetry (CV). Thus, CuxSe shell-like structure was formed on the CuxS particles, helping to enhance electron transfer rate and boost high catalytic activity. This structure also disassociates Se2-, which is useful in the fabrication of polyselenosulfide electrolyte to scavenge photo-generated holes. The stability result after 120 hrs reveals that the PCE value drops to half of its initial value due to the CuxS@CuxSe structure.

    摘要 I Abstract II 總目錄 III 圖目錄 VI 表目錄 XI 一、緒論 1 1.1 前言 1 1.2 太陽能電池發展 2 1.2.1 第一代---矽晶太陽能電池 3 1.2.2 第二代---薄膜太陽能電池 4 1.2.3 第三代---敏化太陽能電池 4 1.3 研究動機 6 二、文獻回顧 7 2.1 量子點 7 2.1.1 量子侷限效應 Quantum confinement effect 7 2.1.2 多重激子效應 Multiple exciton generation 10 2.1.3 迷你傳導帶效應 Minibands effect 12 2.2 量子點敏化太陽能電池 (Quantum dots of sensitized solar cell , QDSSC) 13 2.2.1 基本原理 13 2.2.2 元件介紹 15 2.2.3 背電極製備方法 33 2.2.4 離子交換法與其應用 37 三、實驗步驟 50 3.1 實驗藥品 50 3.2 實驗儀器 53 3.3 實驗流程簡介 55 3.4 導電玻璃清洗 56 3.5 光電極薄膜基板製備 57 3.5.1 TiCl4前處理 57 3.5.2網印法網印TiO2薄膜 57 3.6 量子點敏化劑製備 58 3.6.1 Cu-In-S前驅物母液製備 58 3.6.2 Cu-In-S量子點合成 58 3.6.3量子點敏化劑配製 59 3.7 ZnS鈍化層 59 3.7.1前驅物溶液配製 59 3.7.2 ZnS鈍化層沉積 59 3.8 電解液之配製 60 3.9 背電極製備 60 3.9.1 CuS奈米材料合成 60 3.9.2 CuxS背電極製備 60 3.9.3 CuxS@CuxSe背電極製備 61 3.10 電池元件封裝 61 四、結果與討論 62 4.1電池元件之結構分析 63 4.1.1光電極之結構分析 63 4.1.2背電極之結構分析 65 4.2 PART I‐不同製程之背電極穩定度比較與不同金屬硫化物之比較 74 4.2.1光電轉換效率分析之基本原理 74 4.2.2不同製程之背電極穩定度 76 4.2.3不同金屬硫化物背電極光電轉換效率之分析 79 4.3 PART II‐CuxS@CuxSe異質結構背電極 81 4.3.1背電極光電轉換效率分析 81 4.3.2穩定度之比較 83 4.4背電極之電化學分析 86 4.4.1電化學阻抗分析(Electrochemical impedance spectroscopy, EIS) 86 4.4.2 Tafel量測分析 90 4.4.3循環伏安法量測分析(Cyclic voltammetry, CV) 93 4.5背電極對光電轉換效率各值(JSC、VOC、FF)之影響 96 五、結論與未來展望 99 參考文獻 100

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