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研究生:曾建超
研究生(外文):Tseng,Chien-Chao
論文名稱:表面修飾鈣/鋁之磁鐵礦以應用於吸附水中磷酸鹽
論文名稱(外文):Application of magnetite modified with calcium and aluminum to adsorb phosphate in aqueous solution
指導教授:邱求三
指導教授(外文):Chiou, Chyow-San
口試委員:.陳華偉洪桂彬
口試日期:2012-07-04
學位類別:碩士
校院名稱:國立宜蘭大學
系所名稱:綠色科技學程碩士在職專班
學門:工程學門
學類:綜合工程學類
論文種類:學術論文
論文出版年:2012
畢業學年度:100
語文別:中文
論文頁數:98
中文關鍵詞:磁性顆粒硝酸鋁硝酸鈣吸附磷酸鹽
外文關鍵詞:SiO2
相關次數:
  • 被引用被引用:2
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  • 下載下載:15
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磷酸鹽是工業上常用的原料之一,常因大量使用而造成生態環境的危害,而吸附技術是一種簡單且高效率去除磷酸鹽的方法之一。吸附劑以磁性顆粒作為材料,只需在外加磁場下就能輕易的回收再利用,在實際應用上頗為可行。本實驗為避免磁性顆粒在水溶液中因水解而遭受破壞,先將磁性顆粒(Fe3O4)表面以矽酸鈉對其做SiO2 層包覆(SiO2/Fe3O4),以達到保護磁性顆粒的目的, 再添加硝酸鈣與硝酸鋁對SiO2 層進行表面修飾(Ca-Al/SiO2/Fe3O4)。進而利用FT-IR、XRD、VSM 及BET 對所合成的磁性吸附劑作材質分析,並對水溶液中的磷酸鹽進行吸附實驗,實驗中分別對水溶液pH 值及磷酸鹽濃度等參數進行探討,並進行等溫吸附實驗、動力吸附及脫附實驗。經由pH 效應的探討發現,最佳吸附條件的pH 値為6.0。而在等溫實驗中發現,Ca-Al/SiO2/Fe3O4 對磷酸鹽的吸附行為均符合Langmuir 和Freundlich 等溫吸附模式,而其對磷酸鹽最大吸附量(qm)及吸附反應的自由能分別為35.12 mg g–1 和 -21.17 kJ mol–1 。在動力吸附實驗求得Ca-Al/SiO2/Fe3O4 吸附的活化能為8.95 kJ mol–1,且其吸附行為較符合擬二階模式為動力吸附模式。在脫附實驗條件探討發現,利用0.05 M 的NaOH 水溶液即可有效使Ca-Al/SiO2/Fe3O4 達到脫附磷酸鹽的目的。由實驗結果得知,磁性吸附劑可作為一種有效的水處理方法。
Phosphate is one of the industrial raw materials, often cause ecological harm to the environment due to the extensive use, and adsorption is a simple and potential method of removal phosphate.A magnetic adsorbent manufactured from magnetite (Fe3O4) can be easily recycled under an external magnetic field. In this research, the surface of magnetite modified with calcium﹑aluminum and silica (Ca-Al/SiO2/Fe3O4) was used to adsorb phosphate in an aqueous solution in a batch system.The optimum solution pH for phosphate adsorption by Ca-Al/SiO2/Fe3O4 was found to be 6.0. The phosphate adsorption behavior by Ca-Al/SiO2/Fe3O4 was in good agreement both with the Langmuir and Freundlich adsorption isotherm, and the maximum adsorption capacity ( m q ) and Gibbs free energy of phosphate was 35.12 mg g–1 and -21.17 kJ mol–1, respectively. A pseudo-second-order model could best describe the adsorption kinetics, and the derived activation energy was 8.95 kJ mol–1. The optimum condition to desorb phosphate from Ca-Al/SiO2/Fe3O4 is provided by a solution with 0.05 M NaOH. Magnetic adsorbent is a potential material of water treatment method.
摘要...............................................................................................I
Abstract ........................................................................................ II
目錄............................................................................................. III
圖目錄............................................................................................VII
表目錄............................................................................................ IX
第一章 緒論........................................................................................ 1
1.1 研究背景..................................................................................... 1
1.1.1 磁性顆粒簡介............................................................................. 1
1.1.2 磁性顆粒合成............................................................................. 2
1.1.3 磁性載體技術............................................................................. 3
1.1.4 磁性載體技術應用.......................................................................... 3
1.1.5 含磷酸鹽廢水............................................................................. 3
1.2 研究目標..................................................................................... 4
第二章 文獻回顧..................................................................................... 6
2.1 Fe3O4 簡介................................................................................... 6
2.1.1 氧化鐵.................................................................................. 6
2.1.2 磁性載體Fe3O4............................................................................ 9
2.1.3 磁學性質................................................................................ 12
2.1.3.1 磁性材料分類...................................................................... 12
2.1.3.2 磁區與磁滯曲線.................................................................... 14
2.1.3.3 磁性與粒徑關聯.................................................................... 16
2.2 SiO2/Fe3O4 顆粒.............................................................................. 19
2.2.1 膠體粒子生成機制.......................................................................... 19
2.2.1.1 均質成核(homogeneous nucleation)與表面成長(surface growth)理論...................... 19
2.2.1.2 膠體穩定與凝聚..................................................................... 20
2.2.2 SiO2 特性介紹............................................................................ 23
2.2.3 SiO2 包覆Fe3O4.......................................................................... 29
2.3 Al/SiO2/Fe3O4 顆粒........................................................................... 32
2.3.1 硝酸鋁改質SiO2/Fe3O4 顆粒................................................................. 32
2.4 粒子表面修飾.................................................................................. 34
2.4.1 粒子的表面修飾........................................................................... 34
2.5 磷酸鹽的介紹.................................................................................. 38
2.5.1 磷酸鹽的介紹............................................................................. 38
2.5.2 磷酸鹽的來源特性.......................................................................... 38
2.5.3 磷酸鹽的應用.............................................................................. 39
2.5.4 工業上處理磷酸鹽的方法..................................................................... 40
2.5.4.1 沉澱法去除水中磷酸鹽................................................................ 40
2.5.4.2 多段式流體化床..................................................................... 41
2.5.4.3 生物除磷..........................................................................42
2.5.4.4 吸附法應用於處理磷酸鹽..............................................................43
2.6 吸附理論...................................................................................... 44
2.6.1 等溫吸附理論............................................................................. 44
2.6.2 熱力學研究................................................................................ 46
2.6.3 吸附動力學................................................................................ 46
2.6.4 影響吸附因子............................................................................... 48
第三章 材料與方法...................................................................................... 50
3.1 實驗藥品與儀器................................................................................... 50
3.1.1 實驗藥品................................................................................... 50
3.1.2 儀器...................................................................................... 51
3.2 特性分析....................................................................................... 52
3.2.1 XRD 分析................................................................................. 52
3.2.2 FT-IR 分析............................................................................... 52
3.2.3 BET 比表面積分析.......................................................................... 53
3.2.4 震動樣品磁度儀分析(Vibrating Sample Magnetometer, VSM)..................................... 54
3.3 合成方法....................................................................................... 54
3.3.1 SiO2 包覆Fe3O4............................................................................ 54
3.3.2 鈣/鋁改質SiO2/Fe3O4 ....................................................................... 55
3.4 吸附實驗........................................................................................ 56
3.4.1 等溫吸附實驗................................................................................ 56
3.4.2 動力吸附實驗................................................................................ 57
3.4.3 脫附實驗.................................................................................... 57
3.4.4 重複實驗.................................................................................... 58
第四章 結果與討論....................................................................................... 59
4.1 合成吸附劑之討論.................................................................................. 59
4.1.1 FT-IR 分析.................................................................................. 59
4.1.2 XRD 分析.................................................................................... 60
4.1.3 BET 分析.................................................................................... 61
4.1.4 VSM 分析.................................................................................... 62
4.2 等溫吸附實驗...................................................................................... 63
4.2.1 pH 值影響................................................................................... 63
4.2.2 空白吸附實驗................................................................................. 66
4.2.3 等溫吸附實驗................................................................................. 66
4.2.4 動力吸附實驗................................................................................. 70
4.2.5 脫附實驗..................................................................................... 74
4.2.6 重覆實驗..................................................................................... 75
第五章 結論............................................................................................. 77
5.1 結論............................................................................................. 77
參考文獻................................................................................................ 79
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