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研究生： 鍾文浩
Chung, Wen-Hao
論文名稱： 氧化石墨烯量子點應用於鈣鈦礦太陽能電池之研究
Application of Graphene Oxide Quantum Dots on Perovskite Solar Cell
指導教授： 鄧熙聖
Teng, Hsi-Sheng
學位類別： 碩士
Master
系所名稱： 工學院 - 化學工程學系
Department of Chemical Engineering
論文出版年： 2015
畢業學年度： 103
語文別： 中文
論文頁數： 91
中文關鍵詞： 氧化石墨烯量子點 、鈣鈦礦太陽能電池
外文關鍵詞： Graphene Oxide Quantum Dots, Mixed Halide Perovskite Solar Cells
相關次數： 點閱：74  下載：1 
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    • 本篇首先以研究氯混摻對於鈣鈦礦太陽能電池之影響，進而了解鈣鈦礦之物理與電性。憑藉組裝固態鈣鈦礦太陽能電池之經驗，目標為將氧化石墨烯量子點取代鈣鈦礦作為吸收層應用於太陽能電池。
    本篇將甲基胺氯混入甲基胺碘／異丙醇之溶液，並利用兩步連續沉積法將此混合溶液旋轉塗佈於碘化鉛上反應，經由100℃鍛燒兩小時後形成氯混摻之鈣鈦礦太陽能電池。
    研究分析方面，本篇藉由XRD繞射分析與SEM分析探討鈣鈦礦之結晶組成與表面形態的變化；以紫外-可見光吸收光譜與量子效率量測系統分析鈣鈦礦於特定入射光波長下之吸收與光電流關係；分別利用I-V特性曲線、IMPS與IMVS以了解鈣鈦礦之電池特性、電子傳遞時間及電子生存時間。
    經由XRD繞射分析發現，氯的混摻並不會改變鈣鈦礦的結晶組成；而從SEM中可看出，氯的混摻能使鈣鈦礦表面形態更為緻密，減少漏電途徑，同時使鈣鈦礦具有更大的結晶粒徑，有效地提升電子傳遞速率。
    由紫外-可見光吸收光譜得知，氯的混摻對於鈣鈦礦吸收強度與吸收曲線特徵並無影響，其Onset Wavelength位置約於800 nm ( 能隙約為1.55 eV )；吸收峰位於藍光區與量子效率量測之光電流趨勢吻合。
    根據I-V測試，藉由氯的混摻可將光電流由11.6 mA/cm2提升至17.1 mA/cm2，為轉換效率由6.53 %提升至10.4 %之主因。由紫外-可見光吸收光譜與IMPS結果可說明，光電流的提升主要於源於更短的電子傳遞時間而非吸光量的改變。同時，由IMPS之結果可發現鈣鈦礦擔載於二氧化鈦時，電子具有兩種傳遞模式：其一，電子經由鈣鈦礦導帶被工作電極收集後傳出外電路；其二，電子經由鈣鈦礦導帶注入到二氧化鈦導帶後，傳遞至工作電極再導向外電路。另外，由IMVS分析結果可知，氯的混摻得以延長電子生存時間與SEM之結果相符。然而，由IMVS分析我們無法找到可對應兩種電子傳遞模式的電子再結合模式。
    最後，本篇嘗試將氧化石墨烯量子點應用於混合異質接面型鈣鈦礦太陽能電池結構，並藉由混入PCPDTBT高分子幫助電子電洞對分離與傳導，同時補足氧化石墨烯量子點的低紅光吸收。由I-V特性曲線可看出其暗電流於高電位差處並無下降趨勢，表示有其它行為產生正電流。進一步經由正向掃描的開關光I-V測試，其結果顯示氧化石墨烯量子點太陽能電池內部於0.49伏特下有PN性質的轉換，而引發此種轉換之原因仍有待更深入地探討。

    In this report, we present the planar heterojunction prerovskite solar cell based on the modified sequential deposition method. We emphasized that the chloride doping in precursor is crucial to the morphology of perovskite. By means of the experience, an attempt was then made on graphene oxide quantum dots (GOQDs), which is more environment- friendly and better humidity-tolerance. With chloride doping, over 50% promotion of power conversion efficiency (PCE) was achieved due to higher photocurrent. Accord- ing to the SEM, IMPS and IMVS results, the advanced parameters was mainly influenced by the better perovskite crystallinity, leading to shorter electron transit time (τd ) and longer electron life time (τn ). Besides, GOQDs mixed with fullerene and Poly[2,6-(4,4-bis-(2-ethyl-hexyl)-4H-cyclopenta[2,1-b;3,4-b′]dithio-phene)-alt-4,7(2,1,3-benzothiadiazole)] (PCPDTBT) was functioned as interlayer in solar cells. Eventually, 0.25 mA/cm2 photocurrent was attained, accompanying an interesting P-N property exchange pending further discussion.

    中文摘要........ I 英文延伸摘要......III 誌謝.........IX 目錄.........X 表目錄.........XIV 圖目錄.........XV 第一章 緒論..........................1 1-1 前言............................1 1-2 半導體簡介.........................3 1-3 光伏效應...........................6 1-4 太陽能電池簡介.........................8 1-4-1 矽晶太陽能電池.......................9 1-4-2 化合物半導體太陽能電池 (薄膜太陽能電池)................10 1-4-3 染料敏化太陽能電池.......................11 1-4-4 有機半導體太陽能電池 .....................12 1-5 氧化石墨烯量子點簡介.......................13 1-6 研究動機與目的........................15 第二章 文獻回顧與理論說明......................16 2-1 固態鈣鈦礦太陽能電池結構與工作原理...................16 2-1-1 全固態染料敏化型( solid-state Dye Sensitized Solar Cell )..........16 2-1-2 中孔支架型 ( Meso-Superstructured Solar Cell )............18 2-1-3 平板薄膜型 ( Planar Thin Film Perovskite Solar Cell )...........20 2-1-4 免電洞傳輸層型 ( Hole-Conductor-Free Perovskite Solar Cell )........21 2-1-5 混合異質接面型 ( Bulk Hetero-junction Solar Cell )............22 2-1-6 薄膜中孔複合型 ( Meso-Planar Hybrid Perovskite Solar Cell ).........23 2-2 緻密層與傳遞層( COMPACT LAYER AND MAIN LAYER )..............24 2-3 鈣鈦礦( PEROVSKITE ).....................25 2-3-1 鈣鈦礦結構與組成......................25 2-3-2 鈣鈦礦沉積製程........................26 2-4 電洞傳輸層( HOLE TRANSPORT MATERIAL )................30 2-5 相對電極( COUNTER ELECTRODE )..................31 第三章 實驗方法與儀器原理介紹....................32 3-1 實驗藥品.........................32 3-2 實驗儀器設備.........................34 3-3 組裝固態鈣鈦礦太陽能電池.....................35 3-3-1 FTO導電玻璃基板......................35 3-3-2 二氧化鈦緻密層.......................36 3-3-3 二氧化鈦中孔層.......................36 3-3-4 鈣鈦礦吸收層.......................36 3-3-5 電洞傳輸層........................39 3-3-6 相對電極........................39 3-4 組裝氧化石墨烯量子點太陽能電池..................40 3-4-1 ITO導電玻璃基板.......................40 3-4-2 電洞傳輸層........................41 3-4-3 氧化石墨烯量子點與高分子複合吸收層.................41 3-4-4 電子傳輸層........................43 3-4-5 工作電極........................43 3-5 儀器原理與測量方法.......................44 3-5-1 I-V特性曲線的測試......................44 3-5-2 IMPS與IMVS之原理與測量.....................46 3-5-3 XRD繞射分析.......................49 3-5-4 紫外-可見光分光光度計 ( UV-Vis Spectrophotometer )...........51 3-5-5 掃描式電子顯微鏡 ( Scanning Electron Microscope, SEM ).........53 3-5-6 量子效率量測系統 ( Incident Monochromatic Photon-to-electron Conversion Efficiency, IPCE ).54 第四章 結果與討論 .......................55 4-1 氯混摻對甲基胺鉛碘鈣鈦礦太陽能電池之影響 ...............55 4-1-1 前言..........................55 4-1-2 XRD繞射分析.......................56 4-1-3 紫外-可見光吸收光譜分析.....................59 4-1-4 SEM分析.........................60 4-1-5 光電轉換效率.......................63 4-1-6 IMPS分析........................69 4-1-7 IMVS分析........................73 4-2 氧化石墨烯量子點應用於鈣鈦礦太陽能電池................76 4-2-1 前言..........................76 4-2-2 紫外-可見光吸收光譜分析.....................78 4-2-3 光電轉換效率.......................80 第五章 結論與建議........................83 5-1 結論 ...........................83 5-2 建議 ...........................84 第六章 參考文獻........................85

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