MIL-68-NH2@ZnIn2S4中空管狀結構光觸媒之光催化產氫研究

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范聿瑄(Yu-Hsuan Fan) 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

MIL-68-NH2@ZnIn2S4中空管狀結構光觸媒之光催化產氫研究
(Hollow Tubular Structured MIL-68-NH2@ZnIn2S4 for Photocatalyst Hydrogen Production)

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至系統瀏覽論文 (2025-8-14以後開放)

摘要(中)

能源議題近年來倍受關注，尤其環保及能源逐年匱乏經常是該議題中最具挑戰的項目，因此發展再生能源成為能源短缺和永續發展最好的解方，能源載體（energy carrier）之一的氫能為一種潔淨能源，可以取代傳統化石燃料且對環境汙染極低，是非常具有潛力的能源。過渡金屬硫化物為現今光催化進行水分解產氫的領域中效能較好的觸媒之一，但其光生載流子快速複合使產氫效率下降是目前面臨的一大挑戰，因此在本研究中，我們嘗試改質過渡金屬硫化物，以提高其光催化效率。
本研究藉由簡易的低溫溶劑熱法合成由有機金屬骨架（MOF）MIL-68-NH2與過渡金屬硫化物ZnIn2S4（ZIS）組成的異質結構複合物，進一步提升ZIS光催化產氫的性能。MIL-68-NH2具有高比表面積和獨特的管狀結構，因此，引入MIL-68-NH2增加的比表面積可以捕獲更多光子，此外，在MIL-68-NH2@ZnIn2S4複合物形成的同時，MIL-68-NH2形成中空結構，進一步提高活性位點的數量，而MIL-68-NH2吸收光波長範圍落在近紅外光處，ZnIn2S4與其複合後可有效地擴展光吸收範圍。為了減少材料成本，本研究於實驗中並無額外加入貴金屬（如：鉑、金等）作為共觸媒來提高產氫效率，並在室溫下以100mW/cm2的光強度照射進行反應，其中MIL10020@ZIS為最佳比例之複合物，以光觸媒總重計算得到之最高產氫效率為1901µmol/g/h。

摘要(英)

Recently, increasing attention has been paid to energy issues, especially in relation to environmental protection and energy scarcity, which are the most challenging aspects of the future. Therefore, the development of renewable energy has become the best solution for addressing energy shortages and promoting sustainable development. Hydrogen energy is one type of renewable and clean energies carrier, whose representative reaction is light-driven water splitting for hydrogen evolution. It can replace fossil fuels without causing environmental pollution. Hence, it’s important to develop efficient photocatalysts that can be used in hydrogen energy. Transition metal sulfides are among the most efficient photocatalysts in the field of photocatalytic hydrogen evolution, but their hydrogen evolution efficiency is hindered by the rapid recombination of photogenerated charge carriers, presenting a major challenge. Therefore, in this study, we attempted to modify transition metal sulfides to improve their photocatalytic efficiency.
We synthesized a heterostructured composite consisting of the organic metal-organic framework (MOF) MIL-68-NH2 and the transition metal sulfide ZnIn2S4 (ZIS) by a simple oil bath method to further enhance the photocatalytic hydrogen evolution performance of ZIS. MIL-68-NH2 possesses a high surface area and a unique tubular structure. Therefore, the introduction of MIL-68-NH2 not only increases the surface area of the photocatalyst for light absorption but also exposes more active sites for reaction. In addition, during the formation of the MIL-68-NH2@ZnIn2S4 composite, MIL-68-NH2 forms a hollow structure, further increasing the number of active sites. Moreover, the heterostructure composite effectively expands the light absorption range.
In order to keep the cost down, t this study didn’t add any additional precious metals, e.g., Pt and Au as co-catalyst in the reaction. The highest hydrogen evolution rate of the optimal ratio sample MIL10020@ZIS reaches up to 1901 µmol/g/h under 100 mW/cm2 of visible light intensity at room temperature.

關鍵字(中)

★ ZnIn2S4
★ MIL-68-NH2
★ 光觸媒產氫
★ 異質結構

關鍵字(英)

★ ZnIn2S4
★ MIL-68-NH2
★ photocatalyst hydrogen evolution
★ heterostructure

論文目次

摘要 i
Abstract ii
誌謝 iv
目錄 v
圖目錄 ix
表目錄 xiii
第1章緒論 1
1-1 前言 1
1-2 研究動機 3
第2章文獻回顧 5
2-1 光觸媒裂解水產氫 5
2-2 光觸媒材料 7
2-3 ZnIn2S4光觸媒 11
2-4 改善光觸媒產氫效率的方式 13
2-4-1 能帶調節 13
2-4-2 元素摻雜 16
2-4-3 擔載共觸媒（co-catalyst loading） 17
2-4-4 建立異質結構 18
2-4-5 缺陷（vacancy）工程 21
2-5 金屬有機骨架 22
第3章實驗方法及步驟 24
3-1 實驗藥品 24
3-2 分析與實驗儀器 25
3-3 實驗步驟 27
3-3-1 製備不同合成溫度之MIL-68-NH2 27
3-3-2 油浴法製備不同硫前驅物（TAA）比例之ZnIn2S4 27
3-3-3 油浴法製備MIL-68-NH2與ZnIn2S4之複合物 28
3-3-4 粉體光觸媒產氫量測 29
3-3-5 產氫檢量線量測 32
第4章結果與討論 34
4-1 前導 34
4-2 不同溫度下製備之MIL-68-NH2 35
4-2-1 MIL-68-NH2形貌分析 (SEM) 35
4-2-2 傅立葉轉換紅外線光譜分析 36
4-2-3 X光繞射分析 37
4-2-4 X-ray光電子能譜儀 38
4-2-5 紫外光-可見光光譜分析 41
4-2-6 螢光光譜分析 43
4-3 不同前驅物比例下合成之ZnIn2S4 44
4-3-1 ZIS形貌分析 (HR-STEM) 44
4-3-2 X光繞射分析 46
4-3-3 X-ray光電子能譜儀 48
4-3-4 紫外光-可見光光譜分析 51
4-3-5 螢光光譜分析 52
4-3-6 產氫效率 53
4-4 不同溫度下製備之MIL-68-NH2與ZIS組成之異質結構 54
4-4-1 MN@ZIS形貌分析 55
4-4-2 X光繞射分析 58
4-4-3 紫外光-可見光光譜分析 60
4-4-4 螢光光譜分析 62
4-4-5 產氫效率 63
第5章結論與未來展望 67
第6章附錄 69
6-1 合成ZnIn2S4之前驅物探討 69
6-2 H2BDC-NH2添加量對MIL-68-NH2光吸收範圍之影響 70
6-3 MIL-68-NH2之產氫效率 71
參考文獻 72

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指導教授

李岱洲(Tai-Chou Lee)

審核日期

2023-8-15

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