UiO-66-NH2@ZnIn2S4光觸媒光催化產氫之研究

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姓名

盧奕汝(Yi-Ru Lu) 查詢紙本館藏

畢業系所

化學工程與材料工程學系

論文名稱

UiO-66-NH2@ZnIn2S4光觸媒光催化產氫之研究
(Solar Hydrogen Production using UiO-66- NH2@ZnIn2S4 Photocatalyst)

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至系統瀏覽論文 (2027-9-23以後開放)

摘要(中)

地球上的能源越來越缺乏，加上環保意識的不斷提高，再生能源將是取之不盡且乾淨的能源，其中太陽能是一備受關注的再生能源。在眾多轉換再生能源的方法中，我們選用光催化反應的方式將太陽能轉換為化學形式儲存起來，且該製程的污染物和能耗相對較低，因此開發提高光催化反應之光觸媒極其重要。
通過簡便的溶劑熱法合成UiO-66-NH2@N-ZnIn2S4-S (UN-Xy@N-ZIS-S)異質結構，在光催化產氫反應中產生優異的性能，本研究利用氮摻雜與過量硫代乙醯胺，以及引入金屬有機骨架UiO-66-NH2，可以將形貌從2D奈米片轉變為2D奈米片構成之繡花球狀，同時過量的硫代乙醯胺能夠驅動ZnIn2S4與UiO-66-NH2更緊密接觸，使其均勻度提升從而減短電子與質子之間的反應距離，其中UiO-66-NH2的引入除了MOF本身多孔性結構外，異質結構的構成可以讓載流子移動順利，而能隙值從2.19 eV (ZnIn2S4)變寬至2.6 eV (UN-12030@N-ZIS-S)，進一步降低電子-電洞再結合的狀況，變寬的能隙值會因為N的存在捕捉電洞，促進產氫效率的提升。為了減少反應成本，過程中沒有添加Pt，而本研究在常溫下使用光強度100 mW / cm2，光觸媒為UN-12030@N-ZIS-S進行反應，得到最佳產氫效率為2592 μmol/g/h。

摘要(英)

Due to the lack of energy on the earth and people’s awareness of environmental protection was enhanced. We have to find other alternative energy. While renewable energy will be inexhaustible and clean, among which solar energy is a renewable energy that has received much attention. We use the photocatalytic reaction to convert solar energy into chemical form for storage. The pollutants and energy consumption of this process are relatively low. Thus, it is extremely important to develop photocatalysts to improve photocatalytic reactions. In this study, N-doping and excess TAA, as well as the introduction of metal-organic framework UiO-66-NH2, can transform the morphology from 2D nanosheets to flowerlike nanospheres composed of 2D nanosheets. At the
same time, excess TAA can drive ZIS and UiO-66-NH2 in intimate contact, which improves the uniform of the composite and shortens the reaction distance between electrons and protons. In addition to the porous structure
of the MOF, the introduction of UiO-66-NH2 can boost the carriers to move, and the band gap change from 2.19 eV (ZnIn2S4) to 2.6 eV (UN-12030@NZIS-S). Further reducing the recombination of electrons and holes. The broad energy gap will trap holes due to the presence of N and promote hydrogen production efficiency. In order to reduce the reaction cost, no Pt was added to the reaction. The sample of UN-12030@N-ZIS-S has the best hydrogen production efficiency about 2592 μmol/g/h under 100 mW/cm2 of light
intensity at room temperature.

關鍵字(中)

★ 光觸媒產氫
★ 異質結構

關鍵字(英)

★ photocatalyst hydrogen production
★ heterostructure

論文目次

摘要 i
Abstract ii
致謝 iii
目錄 iv
圖目錄 viii
表目錄 xiii
第一章緒論 1
1-1 前言 1
1-2 光觸媒產氫 3
1-3 研究動機 5
第二章文獻回顧 6
2-1 產氫方法 6
2-2 光觸媒粉末分解水產氫 7
2-3 光觸媒材料 12
2-4 影響光觸媒產氫重要因素 16
2-4-1 能隙值 16
2-4-2 犧牲試劑 22
2-4-3粉末顆粒表面與大小 23
2-4-4光強度 24
2-4-5溫度 25
2-5 ZnIn2S4 光觸媒 26
2-6 金屬有機骨架 30
2-7 異質結構之光觸媒結構研究 31
第三章實驗方法及步驟 33
3-1 實驗藥品 33
3-2 分析與實驗儀器 37
3-3 實驗步驟 39
3-3-1 溶劑熱法(純DMF)製備金屬有機骨架 (UiO-66-NH2) 39
3-3-2 溶劑熱法在不同溫度下製備金屬有機骨架 (UiO-66-NH2-X) 39
3-3-3 水熱法製備不同硫代乙醯胺含量(TAA)的純ZnIn2S4 40
3-3-4 溶劑熱法製備N dopped ZnIn2S4 41
3-3-5 溶劑熱法合成UN-Xy@N-ZIS-S 41
3-3-6 粉體光觸媒產氫量測 42
第四章實驗結果與討論 45
4-1 前導 45
4-2 不同溫度與溶劑製備UiO-66-NH2 45
4-2-1 UN粒徑及形貌分析 (HR-STEM) 47
4-2-2 傅立葉轉換紅外線光譜分析 51
4-2-3 X光繞射分析 52
4-2-3 紫外光-可見光光譜分析 54
4-2-4 螢光光譜分析 55
4-2-5 產氫效率 56
4-3 過量TAA與N doping製備ZnIn2S4 58
4-3-1 不同ZIS之形貌分析 (HR-STEM) 58
4-3-2 X光繞射分析 61
4-3-3 X-ray 光電子能譜儀 63
4-3-4 紫外光-可見光光譜分析 66
4-3-4 螢光光譜分析 67
4-3-5 產氫效率 68
4-4 異質結構UiO-66-NH2與N-ZIS-S結合效應 69
4-4-1 UiO-66-NH2-Xy@N-ZIS-S形貌分析 (HR-STEM) 69
4-4-2 X光繞射分析 76
4-4-3 紫外光-可見光光譜分析 77
4-4-4 螢光光譜分析 79
4-4-5 傅立葉轉換紅外線光譜分析 80
4-4-6 產氫效率 82
第五章結論與未來展望 85
附錄 87
參考資料 90

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指導教授

李岱洲(Tai-Chou Lee)

審核日期

2022-9-23

推文