臺灣博碩士論文加值系統

光催化法可有效處理水中汙染物，並廣泛運用在廢水處理，但有著不易回收的問題，因此，本研究主要製備具有磁性並且在可見光下可以有效去除在水中有機物質(例如: 甲基橙Methyl orange, MO)之光觸媒，使其轉變較無害的CO2以及H2O等無二次汙染的產物，並以磁性來回收再利用光觸媒。本實驗透過溶膠凝膠法及溶劑熱法製備出八面體、中空球體及十二面體氧化亞銅，並將氧化亞銅附載於高電子遷移率的還原氧化石墨烯(Reduce grapheme oxide, rGO)上，利用rGO電子遷移率高的特性，解決氧化亞銅吸收可見光激發的電子容易電子電洞再聚合的問題，結果顯示，以添加1% rGO於氧化亞銅之光觸媒具最好降解活性。此外，在合成不同氧化亞銅晶相的實驗中，由HR-TEM可觀察到，八面體、中空球體以及十二面體氧化亞銅分別具有(111)、(110)&(111)以及(110)結晶面，因(110)結晶面表面具有較多銅原子可與污染物反應使其光催化效果會優於(111)結晶面相之氧化亞銅。進一步添加磁性核殼材料(Fe3O4@SiO2)作為磁性基質用於回收觸媒，形成具有高飽和磁化量(11.79 emu/g)及光催化活性的光觸媒，並以TEM證明磁性粒子有附著於石墨烯上。負載具有磁性十二面體氧化亞銅於還原氧化石墨烯上之觸媒於兩小時內，在可見光照射下降解效率可達將近98%，並經過多次循環後仍保有85.17%。

Photocatalysis can be effectively applied in removing the pollutants in the water, and it has the significant problem that need to be solved. As a result, this research mainly focused on synthesizing magnetic photocatalysts which can effectively remove organic pollutants in the water under visible light. The organic pollutants (Methyl orange, MO) can be transformed into CO2¬ and H2O, etc. The used photocatalysts can be recycled by magnetic process.
The octahedron, hollow sphere, and dodecahedron Cu-2O/graphene were synthesized via sol-gel and solvothermal methods. Then dope Cu2O onto high electron conductivity of graphene oxide (rGO) to reduce recombination electrons and electron holes. As a result, it has the most effective degradation efficiency when combine with 1% graphene oxide. Besides, the results demonstrate that Cu2O dodecahedra with exposed {110} facets with more dagling “Cu” atoms possesses higher activity than those with hollow sphere {110} & {111} facets and Octahedral {111} facets.
We synthesized magnetic core-shell materials (Fe3O4@SiO2), follow by adding Cu2O and graphene oxide that can produce high saturation magnetization and photocatalysis performance of magnetic photocatalysts. Magnetic photocatalysts, dodecahedron Cu¬2O/rGO have removal efficiency of 98% MO in two hours under visible light, after several cycles still retains 85.17%.

目錄
中文摘要 I
ABSTRACT III
誌謝 V
目錄 VII
表目錄 XIII
圖目錄 XVI
第一章 緒論 21
1-1 前言 21
1-2 研究動機 21
1-3 研究目的 22
第二章 相關知識與文獻回顧 23
2-1石墨烯簡介 23
2-1-1石墨烯基本性質 23
2-1-2石墨烯製備與檢測方法 27
2-2 光觸媒簡介 35
2-2-1光觸媒發展歷史 35
2-2-2光觸媒材料 37
2-2-3高級氧化程序 38
2-2-4光觸媒催化機制 41
2-2-5氧化亞銅基本性質: 44
2-3影響光觸媒效率之因素 51
2-3-1觸媒濃度效應 51
2-3-2汙染物濃度效應 54
2-3-3 pH值效應 55
2-3-4 催化劑 56
2-4 磁性分離技術 57
2-4-1鐵氧磁體特性 57
2-4-2磁性觸媒應用 61
第三章 實驗方法與步驟 63
3-1 實驗藥品 63
3-2 實驗器材 65
3-3 分析儀器 66
3-4 實驗流程以及操作變因 74
3-5 製備氧化石墨烯(GRAPHENE OXIDE) 75
3-4 製備超順磁性核殼材料 77
3-4-1 製備四氧化三鐵 77
3-4-2製備具核殼結構四氧化三鐵 (Fe3O4@SiO2) 78
3-5 製備具光催化活性之不同晶型氧化亞銅/還原氧化石墨烯 79
3-5-1 製備八面體氧化亞銅/還原氧化石墨烯 79
3-5-2製備中空球體氧化亞銅/還原氧化石墨烯 81
3-5-3製備十二面體氧化亞銅/還原氧化石墨烯 83
3-6製備具磁性及光催化活性之氧化亞銅/還原氧化石墨烯 85
3-7光觸媒於可見光下降解汙染物 86
第四章 結果與討論 87
4-1 探討不同比例氧化亞銅/還原氧化石墨烯其物性及光催化性質 87
4-1-1 XRD分析 87
4-1-2 TEM 分析 91
4-1-3 SEM分析 92
4-1-4 Uv-Vis吸收光譜分析 94
4-1-5 PL分析 97
4-1-6 XPS 分析 99
4-1-7吸附實驗 104
4-1-8 可見光降解實驗 105
4-1-9 反應速率常數 107
4-2探討不同晶型氧化亞銅物理性質及光催化效率比較 109
4-2-1 XRD分析 110
4-2-2 TEM分析 112
4-2-3 SEM分析 115
4-2-4 Uv-Vis吸收光譜分析 117
4-2-5 XPS 分析 119
4-2-6 吸附實驗 121
4-2-7 可見光降解實驗 122
4-2-8 反應速率常數 124
4-3 磁性光觸媒(CU2O/RGO- FE3O4@SIO2) 126
4-3-1 TEM分析 127
4-3-2 SEM分析 131
4-3-3 SQUID分析 134
4-3-4 XRD分析 137
4-3-5 Uv-Vis吸收光譜分析 139
4-3-5 PL分析 141
4-3-6 XPS分析 142
4-3-7 吸附實驗 147
4-3-8 可見光降解實驗 148
4-3-9 反應速率常數 149
4-4探討各種變因對於可見光降解效果 152
4-4-1 觸媒濃度效應 152
4-4-2 pH值效應 156
4-4-3 觸媒穩定性實驗 160
第五章 結論 162
參考文獻 165
附錄 172
自傳 173

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