SiO2@AIZS奈米殼層結構合成及其光催化產氫研究

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姓名

吳承洋(Cheng-Yang Wu) 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

SiO2@AIZS奈米殼層結構合成及其光催化產氫研究
(Photocatalytic hydrogen production based on SiO2@AIZS core-shell particles)

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摘要(中)

利用表面電漿共振效應提升光觸媒的活性是近年來熱門的議題，我們過去的研究成功利用金銀奈米粒子的表面電漿共振效應提升ZnIn2S4的光催化產氫效率48,49，因AgInS2-ZnS (AIZS) 固態溶液具有可調控能隙的特性，所以本研究使用AIZS作為包覆二氧化矽外殼的金銀奈米粒子(GSNS@SiO2)的材料，但是GSNS@SiO2合成不易，因此我們主要先以二氧化矽作為AIZS的包覆對象。
我們使用直接加熱法在有機溶劑環境下將AIZS包覆在二氧化矽表面，改變溫度及組成兩個重要的合成參數來探討其對包覆結果的影響。此外，為了提升SiO2@AIZS在有機溶劑下合成之親水性，我們使用表面離子基交換對光觸媒表面進行改質，結果顯示親水性有顯著地提升，且產氫效率也大幅上升。最後將合成法套用在GSNS@SiO2上，然而因GSNS@SiO2容易形成聚集的特性，以及二氧化矽與GSNS@SiO2顆粒大小的差異，使包覆的效果不如預期。應用表面電漿共振效應提升AIZS的產氫效率雖然仍未完善，但對於合成殼層結構(GSNS@dielectric@photocatalyst)有了進一步的了解。

摘要(英)

Enhancing photocatalytic activities by surface plasmon resonance effect has been a popular issue in recent years. In our past research, we successfully apply surface plasmon resonance from gold-silver nanoparticles (GSNS NPs) to promote photocatalytic hydrogen production efficiency of ZnIn2S4. Due to a tunable band gap of AgInS2-ZnS (AIZS), AIZS solid solutions are used as the coating material to cover silica-coated gold-silver nanoparticles (GSNS@SiO2). Because of difficult synthesis of GSNS@SiO2, silica serves as the main coating target of AIZS.
We used heating up method to coat AIZS onto silica surface in organic solvents, while two important parameters, temperature and composition, were varied to discuss its effect to coating results. Furthermore, in order to increase hydrophilicity of SiO2@AIZS synthesized in organics, we applied surface ligand exchange to do modification on its surface. Results of modification showed not only hydrophilicity obviously improved but hydrogen production efficiency increased substantially. Finally, synthesis method was carried out on GSNS@SiO2. However, due to easier aggregation of GSNS@SiO2 and difference of particle size between SiO2 and GSNS@SiO2, consequence of coating on GSNS@SiO2 was not as expected. Although it took time to study enhancing AIZS efficiency by surface plasmon resonance, our facile procedure paved the way to synthesize core-shell structure GSNS@dielectric@photocatalyst.

關鍵字(中)

★ 固態溶液
★ 殼層結構
★ 光觸媒產氫

關鍵字(英)

★ Solid solutions
★ Core-shell
★ Photocatalytic hydrogen production

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 4
第二章文獻回顧 5
2-1 光觸媒分解水產氫 5
2-2 光觸媒材料 8
2-3 二氧化矽奈米粒子合成與表面改質 12
2-4 (AgIn)xZn2(1-x)S2光觸媒 15
2-5 光觸媒表面離子基交換 22
2-6 表面電漿共振效應 26
2-7 GSNS@SiO2@ZnIn2S4 28
第三章實驗方法及步驟 30
3-1 實驗藥品 30
3-2 分析與實驗儀器 34
3-3 實驗步驟 37
3-3-1 溶膠-凝膠法製備二氧化矽粉體及MPS表面改質 37
3-3-2 定組成SiO2@AIZS合成溫度最佳化 37
3-3-3 定溫下SiO2@(AgIn)xZn2(1-x)S2元素比例最佳化 38
3-3-4 光觸媒粉體溶液產氫速率量測 39
3-3-5 SiO2@AIZS表面離子基交換 42
3-3-6 奈米殼層結構合成 42
第四章結果與討論 46
4-1 AIZS包覆於MPS改質的二氧化矽 46
4-2 AIZS包覆在二氧化矽前後比較 51
4-2-1 外觀形貌比較 51
4-2-2 結晶性比較 52
4-2-3 產氫效率比較 53
4-3 在不同溫度下合成SiO2@AIZS 54
4-3-1 SiO2@AIZS成分分析 54
4-3-2 表面均質性 55
4-3-3 結晶性 57
4-3-4 產氫效率 58
4-4 以不同比例合成SiO2@(AgIn)xZn2(1-x)S2 60
4-4-1 表面均質性 60
4-4-2 結晶性 61
4-4-3 光學性質分析 64
4-4-4 產氫效率 66
4-5 SiO2@AIZS表面離子基交換 72
4-6 GSNS@SiO2@AIZS套用SiO2@AIZS合成 77
4-6-1 GSNS@SiO2@AIZS 成分分析 77
4-6-2 形貌分析 79
4-6-3 結晶度 80
4-6-4 產氫效率 82
第五章結論與未來展望 83
附錄 85
奈米殼層結構(GSNS, GSNS@SiO2, GSNS@SnO2, GSNS=Ag@Au)的合成 85
SnO2 二氧化錫奈米粒子合成 85
銀奈米粒子合成 86
Gold-silver nanoshells, GSNS金銀奈米粒子合成 87
GSNS@SiO2二氧化矽外殼金銀奈米粒子合成 89
GSNS@SnO2二氧化錫金銀奈米粒子合成 90
GSNS、GSNS@SiO2、GSNS@SnO2的UV-Vis比較 91
參考文獻 92

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指導教授

李岱洲(Tai-Chou Lee)

審核日期

2019-8-16

推文