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研究生: 李亭儀
Lee, Ting-Yi
論文名稱: 溴化銫鉛鈣鈦礦奈米晶體與還原氧化石墨烯複合材料進行高效率光催化二氧化碳還原反應之探討
CsPbBr3 Nanocrystals/Reduced Graphene Oxide Composite for Efficient Photocatalytic CO2 Reduction Reaction
指導教授: 陳家俊
Chen, Chia-Chun
口試委員: 陳家俊
Chen, Chia-Chun
陳俊維
Chen, Chun-Wei
王迪彥
Wang, Di-Yan
郭聰榮
Kau, Tsung-Rong
李紹先
Li, Shao-Sian
口試日期: 2021/07/30
學位類別: 碩士
Master
系所名稱: 化學系
Department of Chemistry
論文出版年: 2021
畢業學年度: 109
語文別: 中文
論文頁數: 62
中文關鍵詞: 光催化二氧化碳還原溴化銫鉛鈣鈦礦奈米晶體輔助型催化劑還原氧化石墨烯複合材料
英文關鍵詞: Photocatalytic reduction of carbon dioxide, Cesium bromide lead perovskite nanocrystals, Co-catalyst, Reduced graphene oxide, Composite
研究方法: 實驗設計法比較研究觀察研究敘事分析
DOI URL: http://doi.org/10.6345/NTNU202101028
論文種類: 學術論文
相關次數: 點閱:145下載:0
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  • 減少二氧化碳是目前全球暖化的首要目標,許多科學家嘗試使用光催化的方式將二氧化碳還原成碳氫能源,達到永續生活;尋找效果好與穩定的材料做二氧化碳光催化還原是重要的環節。鈣鈦礦有優異的光電性質,除了在太陽能電池與光電二極體…等展現優異的效果,近幾年,科學家將鈣鈦礦應用於二氧化碳還原,並研究出鈣鈦礦在催化方面的活性位點,根據使用不同的金屬,有許多不錯的結果,探討如何能讓產量增加也是一大重點。
    本篇論文先探討以氣相-固相的反應條件,純CsPbBr3進行光催化二氧化碳還原以AM1.5G的LED仿太陽光進行6小時的照射,發現純的電子反應速率為20.664,為了達到更好的產率,本篇論文也探討將純CsPbBr3與不同的材料做異質結複合材料進行相同條件的光催化反應,探討異質結複合材料是否能有更突出的效果,其中分別使用了輔助型催化劑.能加強鈣鈦礦電洞傳輸與加強電子傳輸的材料。實驗得出,使用輔助型催化劑加上CsPbBr3可加強二氧化碳還原的效果,其中使用CsPbBr3/RGO的鈣鈦礦複合材料,有最高的電子反應效率361.04,相較於純CsPbBr3而言,多了17.47倍;使用CsPbBr3/SnS2的鈣鈦礦複合材料,其電子反應效率也高達120.59,與純CsPbBr3相比,將近多了4倍的產率。由以上的反應結果,根據不同材料的能隙位置,探討出能隙的位置會影響電子電洞的分離與轉換的效率,產生不同的加強效果。以上結論,不僅能總結如何增強二氧化碳的還原效果,更能夠使用於其他適合的鈣鈦礦材料去進行異質結結構的光催化二氧化碳還原。

    Reducing CO2 is currently the primary goal of global warming. Many scientists tried to use photocatalysis to reduce CO2 into hydrocarbon energy to achieve sustainable life. Finding effective and stable materials for photocatalytic CO2 reduction is an important link. Perovskite has excellent photoelectric properties. In addition to exhibiting excellent effects in solar cells and photodiodes, etc., in recent years, scientists have applied perovskite to the reduction of CO2 and studied the catalytic activity of perovskite According to the use of different metals, there are many good results, and it is also a key point to explore how to increase production.
    This paper first discusses the reaction conditions of gas-solid phase, pure CsPbBr3 for photocatalytic CO2 reduction, and AM1.5G LED imitating sunlight for 6 hours. It is found that the pure electron reaction rate is 20.664, in order to achieve better, this paper also discusses the photocatalytic reaction of pure CsPbBr3 with different materials as heterojunction composite materials under the same conditions, and discusses whether the heterojunction composite materials can have more prominent effects, and co-catalysts are used respectively. A material can not only strengthen the separation of perovskite electrics and electric holes but also strengthen the transfer
    of electrons. Experiments have shown that the use of CsPbBr3 /co-catalysts composite can enhance the effect of carbon dioxide reduction. Among them, the perovskite composite material using CsPbBr3/RGO has the highest electronic reaction efficiency of 361.04, which is 17.47 times higher than that of pure CsPbBr3. The CsPbBr3/SnS2 perovskite composite has an electronic reaction efficiency as high as 120.59, which is nearly 4 times higher than that of pure CsPbBr3. From the above reaction results, according to the position of the energy gap of different materials, it is explored that the position of the energy gap will affect the efficiency of the separation and conversion of electron holes, resulting in different strengthening effects. The above conclusions can not only summarize how to enhance the reduction effect of CO2, but also can be used in other suitable perovskite materials to perform photocatalytic CO2 reduction of heterojunction structure.

    中文摘要 i Abstract ii 目次Table of Contents iii 表次 List of Tables vi 圖次List of Figures vii 第一章 緒論 1 1-1 前言 1 1-2 光催化 2 1-3 光催化劑 3 1-4 光催化的應用 3 1-5 光催化二氧化碳還原反應 7 1-6 光電催化二氧化碳還原反應 7 第二章 文獻回顧與動機 8 2-1 鈣鈦礦材料介紹 8 2-1-1 基本結構與光學性質 8 2-1-2 無機鹵素銫鉛鈣鈦礦奈米晶體 9 2-1-3 鈣鈦礦的應用 10 2-2 鈣鈦礦使用於光催化水分解反應 11 2-3 鈣鈦礦使用於光催化二氧化碳還原反應 12 2-4 鈣鈦礦進行光催化二氧化碳還原反應結構探討 13 2-5 研究動機 14 2-6 CsPbBr3鈣鈦礦複合材料 15 第三章 儀器設備 17 3-1 粉末X光繞射儀(Powder X-ray Diffraction) 17 3-2 紫外光-可見光-近紅外光光譜儀(UV-Visble-Near IR Spectrophotometer) 18 3-3 光致發光光譜儀(Photoluminescence Spectroscopy) 19 3-4 移動式顯微拉曼光譜儀(Mobile Raman Microscope) 20 3-5 穿透式電子顯微鏡(Transmission Electron Microscopy , TEM) 21 3-6 掃描電子顯微鏡(Scanning Electron Microscope , SEM) 22 3-7 氣相層析質譜儀(Gas chromatography–mass spectrometry) 23 第四章 實驗藥品與步驟 26 4-1 實驗藥品 26 4-2 實驗步驟 28 4-2-1 合成CsPbBr3鈣鈦礦之前驅物 28 4-2-2 合成CsPbBr3鈣鈦礦奈米晶體 28 4-2-3 合成氧化石墨烯(Graphine Oxide,GO) 29 4-2-4 合成還原氧化石墨烯(reduced graphine oxide,RGO) 29 4-2-5 製備Spiro-OMeTAD(Spiro)溶液 29 4-2-6 合成二維鈣鈦礦氧化物(Ca2Nb3O10 , CNO) 29 4-2-7 合成二硫化錫奈米片狀晶體(SnS2 Nanosheets) 30 4-2-8 製備CsPbBr3鈣鈦礦薄膜與CsPbBr3鈣鈦礦複合材料薄膜 30 4-3 光催化二氧化碳還原實驗架構 32 第五章 結果與討論 33 5-1 CsPbBr3鈣鈦礦奈米晶體 33 5-1-1 結構分析 33 5-1-2 光學性質 34 5-2 不同基底材料的性質結構探討 35 5-2-1 結構分析 35 5-2-2 光學性質 37 5-3 CsPbBr3鈣鈦礦做光催化二氧化碳還原結果 39 5-3-1 定性分析 39 5-3-2 定量分析 41 5-4 使用不同材料做光催化二氧化碳還原結果 42 5-5 CsPbBr3加上不同材料做複合材料進行光催化二氧化碳還原結果 44 5-6 使用輔助型催化劑與CsPbBr3複合材料差異結果 45 5-6-1 CsPbBr3/RGO複合材料 45 5-6-2 CsPbBr3/SnS2複合材料 47 5-6-3 光催化二氧化碳還原反應增強結果探討 49 5-7 時間與產率探討 50 5-8 穩定度測試 51 5-9 與使用其他鈣鈦礦作為催化劑進行光催化二氧化碳還原結果 52 第六章 結論與未來展望 54 參考文獻References 55 附件 Appendix 61 附件一 61 附件二 62

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