臺灣博碩士論文加值系統

本研究在可見光的照射下，以二氧化鈦/鈦箔作為光觸媒，於含有三價鐵離子的溶液中降解鄰苯二甲酸二酯(DEHP)，並使用批次反應器進行操作，探討DEHP與三價鐵離子的濃度、溶液pH值、光照強度和溫度等實驗操作變因對DEHP光降解速率之影響。此外，藉由比表面積分析 (BET)、X-光繞射 (XRD)、場發射掃描式電子顯微鏡 (FESEM)、紫外-可見漫反射光譜 (UV-vis DRS)、X射線光電子能譜和界達電位，分析光觸媒的特性。
研究結果表明，當DEHP濃度為10 mg/L時，具有最佳的光降解性能。並根據二氧化鈦的零電荷點 pH 值、三價鐵離子的物種分佈和鄰苯二甲酸的解離常數，光降解效率在溶液pH 3.9時為最高。 此外，在低光強度下，DEHP的光降解速率隨著光強度的增加而顯著提升；而在高光強度下，光降解速率的增加則趨近平緩。同時，於溶液中添加二價鐵離子能促使Fe(II) 氧化為Fe(III)，以利於進行DEHP的光降解程序；而在共存離子的實驗當中，氯離子則會顯著抑制DEHP 的光降解效能。透過本實驗的動力學研究表明，DEHP 的光降解過程符合 Langmuir-Hinshelwood 動力學模型，並且速率決定步驟為表面反應。

Photodegradation of DEHP by TiO2/Ti foil in aqueous solution in the presence of Fe(III) Ions were conducted at UV-LED illumination. The effect of DEHP and Fe(III) ions concentration, solution pH, light intensity, and temperature were evaluated in a batch reactor. Brunauer-Emmet-Teller surface area measurement (BET), X-ray diffraction (XRD), field emission scanning electron microscope (FESEM), UV-vis diffuse reflectance spectra (UV-vis DRS), X-ray photoelectron spectroscopy, and zeta potential were used to examine the characteristics of the photocatalyst.
The result demonstrated that 10 mg/L of DEHP and Fe(III) ions exhibited higher photodegradation performance. Due to the pHzpc of TiO2, species distribution of Fe(III) ions, and the pKa of phthalic acid, the photodegradation rate showed better performance at pH 3.9. Additionally, the photodegradation rate of DEHP increased significantly at low light intensity, however the increase of the photodegradation rate tended to remain constant at high light intensity. The reaction didn’t seem to be dependent with the arising temperatures. Meanwhile, the addition of Fe(II) ions only slightly induces the DEHP photodegradation from the oxidation of Fe(II) to Fe(II) ions and the chloride ions significantly inhibited the DEHP photodegradation from the co-existing ions experiment. The kinetic analysis in this study revealed that DEHP photodegradation follows the Langmuir-Hinshelwood kinetic model and the rate-determining step is the surface reaction.

中文摘要 V
Abstract VI
Acknowledgments VII
Table of Content VIII
List of Figure XI
List of Tables XVI
List of Symbol XVIII
Chapter 1 Introduction 1
1.1 Background 1
1.2 Objectives and Scopes 3
Chapter 2 Literature Review 1
2.1 Photolysis and Photocatalysis 1
2.1.1 Basic Properties of TiO2 1
2.1.2 Basic Properties of DEHP 3
2.1.3 Fundamentals of Photocatalytic Reaction and Mechanism 4
2.2 Photocatalytic Degradation of DEHP in Aqueous Solution 8
2.2.1 DEHP Removal Process 8
2.2.2 DEHP Photodegradation in Presence of Oxidizing Agents 12
2.2.3 Reaction Mechanism of DEHP Photodegeadation 14
2.3 Operating Factors Affecting Photocatalytic Redox Reactions 18
2.3.1 Initial Concentration of Fe(III) Ions 18
2.3.2 Initial Concentration of Organic Compound 19
2.3.3 Solution pH 19
2.3.4 Light Intensity 22
2.3.5 Temperature 23
2.3.6 Co-existing Ions 24
Chapter 3 Materials and Experiments 26
3.1 Materials 26
3.2 Experimental Instruments and Apparatus 26
3.2.1 Experimental Apparatus 27
3.2.2 Experimental Instruments 30
3.3 Experimental Procedures 31
3.3.1 Experimental Framework 32
3.3.2 Preparation of Photocatalyst 34
3.3.3 Background Experiments 34
3.3.4 Photooxidation of DEHP under UV-LED Illumination 47
Chapter 4 Results and Discussion 48
4.1 Characterization of TiO2-Ti Foil 48
4.2 Photodegradation of DEHP in Presence of Fe(III) Ions under Continuous Illumination 58
4.2.1 Effect of Initial Concentration of Fe(III) Ions 60
4.2.2 Effect of Initial Concentration of DEHP 68
4.2.3 Effect of Solution pH 73
4.2.4 Effect of Light Intensity 80
4.2.5 Effect of Temperature 87
4.2.6 Effect of Radical Inhibitors 93
4.2.7 Effect of Co-existing Ions 96
4.2.8 Characterization of of TiO2/Ti Foil after Reaction 101
4.3 Proposed Mechanism and Kinetic Analysis 107
4.3.1 Proposed Mechanism and Kinetic Models 107
4.3.2 Kinetic Analysis 119
Chapter 5 Conclusions and Recommendations 128
Reference 132

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