臺灣博碩士論文加值系統

四環素 (TC)、布洛芬 (IBP) 和 Cr(VI) 對於疾病控制和工業生產等人類活動至關重要。 然而，由於其有毒處置，它們是對環境、生態系統和人類健康造成威脅的潛在因素。 因此，他們在出院前需要適當的處理技術。 眾所周知，光催化是一種低成本、有效去除這些污染物的氧化過程，其中光催化劑是促進光催化反應的主要試劑。 如今，石墨碳氮化物（g-C3N4）作為一種具有許多優點和廣泛應用前景的材料，已廣泛應用於光催化活性，特別是在光催化去除污染物方面。 更有趣的是，許多修飾策略已被應用於合成新型和先進的 g-C3N4 基異質結光催化劑，以增強光催化性能。 此外，許多基於 g-C3N4 的光催化劑和其他氧化劑（例如 PMS）之間的組合可以優化光催化過程以消除污染物。 因此，本研究的主要目的是（1）合成1D/2D/3D g-C3N4光催化劑並與其他材料複合形成新型g-C3N4基異質結光催化劑，（2）研究這些製備的光催化劑在光催化劑中的光催化性能。可見光下TC、IBP的氧化和Cr(VI)的還原，(3)了解EDTA和PMS對光催化活性的影響，(4)研究光催化性能的影響因素，(5)研究光催化性能的可能機制光催化過程、污染物轉化途徑和光催化劑的穩定性。

Tetracycline (TC), Ibuprofen (IBP), and Cr(VI) have been essential to human activities like disease control and industrial production. However, they are potential factors that cause threats to the environment, ecological systems, and human health due to their toxic disposals. Hence, they are needed appropriate treatment technologies before being discharged. It is well-known that photocatalysis is a low-cost, effective oxidation process for removing these pollutants, in which photocatalyst is the primary agent to promote photocatalytic reactions. Nowadays, graphitic carbonitride (g-C3N4), a promising material with many advantages and versatile applications, has been widely used in photocatalytic activities, especially in the photocatalytic removal of contaminants. More interestingly, many modification strategies have been applied to synthesize novel and advanced g-C3N4-based heterojunction photocatalysts for enhancing photocatalytic performance. Besides, many present combinations between g-C3N4-based photocatalysts and other oxidation agents, such as PMS, optimize photocatalytic processes for pollutant elimination. Therefore, the main aims of this study are (1) synthesizing 1D/2D/3D g-C3N4 photocatalysts and compositing with other materials to form new g-C3N4-based heterojunction photocatalysts, (2) investigating the photocatalytic performance of these prepared photocatalysts in the oxidation of TC, IBP and reduction of Cr(VI) under visible light, (3) understanding effect of EDTA and PMS on photocatalytic activities, (4) investigating affective factors on the photocatalytic performance, and (5) investigating the possible mechanism of photocatalytic processes, pathways of pollutant conversion and stability of photocatalysts.

ABSTRACT
ACKNOWLEDGEMENTS
TABLE OF CONTENTS
LIST OF TABLES
LIST OF FIGURES
CHAPTER 1-INTRODUCTION 1
1.1 The statement of research 1
1.2 Research objectives 4
1.3 Scopes 5
1.4 Dissertation structure 5
CHAPTER 2- LITERATURE REVIEW 7
2.1 Graphitic carbon nitride (g-C3N4) 7
2.1.1 Structure, characteristics, advantages and disadvantages, synthesis, and applications 7
2.1.1.1 Structure 7
2.1.1.2 Properties 10
2.1.1.3 Advantages and disadvantages 17
2.1.1.4 Synthesis 19
2.1.2 Modification of g-C3N4 21
2.1.2.1 Band-gap engineering 22
2.1.2.2 Heterojunction construction 25
2.1.2.3 Dimensionality tuning 26
2.1.3 Application of g-C3N4 27
2.2 Tetracycline 31
2.2.1 Sources, fate, and toxicity of tetracycline (TC) 31
2.2.1.1 Sources of pollution and fate of tetracycline (TC) in the aqueous environment 31
2.2.1.2 Toxicity of tetracycline 32
2.2.2 Technologies of TC removal 33
2.2.2.1 Adsorption 33
2.2.2.2 Photocatalysis and photochemistry 34
2.2.2.3 Electrochemical method 35
2.3 Ibuprofen (IBP) 36
2.3.1 Sources, occurrence, and toxicity of Ibuprofen 36
2.3.1.1 Sources and occurrence 36
2.3.1.2 Toxicity 37
2.3.2 Technologies for IBP degradation 38
2.4 Hexavalent Chromium (Cr(VI)) 39
2.4.1 Sources, fate, and toxicity of chromium (Cr) in the water environment 39
2.4.1.1 Sources of chromium (Cr) in the environment 39
2.4.1.2 Main forms of chromium in the aqueous environment 40
2.4.1.3 Toxicity of chromium 42
2.4.2 Technologies of Cr(VI) removal 43
2.4.2.1 Adsorption 43
2.4.2.2 Membrane technology 44
2.4.2.3 Photocatalysis 45
2.5 Photocatalysis 45
2.5.1 Definitions of photocatalysis 45
2.5.2 Photocatalysis mechanism using g-C3N4-based catalysts 46
CHAPTER 3 – METHODOLOGY 52
3.1 Research overview 52
3.2 Research contents 56
3.3 Photocatalytic lab-scale reactor model and experiment 57
3.4 Chemicals and analysis methods 58
3.4.1 Chemicals 58
3.4.2 Analysis methods 58
3.4.2.1 Characterization of catalysts 58
3.4.2.2 Analysis methods of pollutants 60
3.4.2.3 Toxicity estimation of IBP and byproducts 61
3.4.2.4 Mass spectroscopy analysis of TC and IBP byproducts 61
3.5 Processing data and calculations 62
3.5.1 Characterization of catalysts 62
3.5.2 Photocatalytic performance 63
CHAPTER 4- A Z-SCHEME NiCo2O4/S CODOPED 1D g-C3N4 HETEROJUNCTION FOR SOLAR-LIGHT-SENSITIVE PHOTOCATALYTIC DEGRADATION OF ANTIBIOTICS IN AQUEOUS SOLUTIONS EXEMPLIFIED BY TETRACYCLINE 65
4.1 Introduction 66
4.2 Materials and methods 67
4.2.1 Synthesis of NiCo2O4@SCN 67
4.2.2 Photocatalytic activities 69
4.3 Characterization of photocatalysts 69
4.4 Photocatalytic decomposition of TC 78
4.5 Effect of catalyst dosage on TC degradation 81
4.6 Effect of pH on TC degradation 82
4.7 Effect of initial TC concentration on TC degradation 86
4.8 Investigation of temperature on TC degradation 87
4.9 Stability, reusability, and applicability of NiCo-S@CN 88
4.10 Determining main reactive oxidation species and possible photocatalytic mechanism 90
4.11 Evaluation of tetracycline and toxicity and mineralization 94
4.12 Conclusion 97
CHAPTER 5- IN-SITU IMMOBILIZATION OF Ag/AgCl ON SULFURIZED g-C3N4 NANOSHEET FOR ENHANCING VISIBLE-LIGHT-DRIVEN PHOTOCATALYSIS TOWARD SIMULTANEOUS OXIDATION OF TETRACYCLINE AND REDUCTION OF Cr(VI) IN WATER 99
5.1 Introduction 100
5.2 Materials and methods 102
5.2.1. Synthesis of S@CN 102
5.2.2. synthesis of silver/silver chloride and S-codoped g-C3N4 (Ag/AgCl-S@CN) 103
5.2.3 Photocatalytic activities 103
5.3 Results and discussions 104
5.3.1 Morphology and structural examination 104
5.3.2 Optical and electrochemical properties 120
5.3.3 Simultaneously TC oxidation and Cr(VI) reduction in photocatalytic systems 115
5.3.4. Enhancement of photocatalytic reaction with EDTA in the TC and Cr(VI) copresence 116
5.3.5. Reusability and stability and of photocatalyst 119
5.3.6 Impact of initial pH 119
5.3.7 Impacts of different antibiotics 122
5.3.8 Separately photocatalytic decomposition of TC and removal of Cr(VI) 124
5.3.9 Possible photocatalytic mechanism 124
5.3.10 Tetracycline degradation pathway 129
5.4 Conclusions 131
CHAPTER 6- PEROXYMONOSULFATE-ASSISTED VISIBLE LIGHT-SENSITIVE 0D/3D Z-SCHEME NiCo2O4@G-C3N4 PHOTOCATALYST FOR EFFECTIVE DEGRADATION OF IBUPROFEN IN WATER 133
6.1 Introduction 133
6.2 Materials and methods 136
6.2.1 Preparation of hollow porous microsphere g-C3N4 136
6.2.2. Preparation of NiCo¬2O4 doped hollow porous microsphere g-C3N4 (NiCo2O4@CN) 136
6.2.3 Photocatalytic performance 137
6.3 Results and discussions 138
6.3.1 Characterization of catalysts 138
6.3.1.1 Morphology and structural analysis 138
6.3.1.2 Optical and electrochemical properties 144
6.3.2 Catalytic degradation tests 149
6.3.3 Effects of operation parameters 152
6.3.3.1 Effect of catalyst, IBP, and PMS dosage 152
6.3.3.2 Effect of initial pH 153
6.3.3.3 Effect of temperature 154
6.3.4 Stability and recyclability of photocatalyst 156
6.3.5 Effect of surface water matrixes on IBP degradation 157
6.3.6 Possible mechanism of IBP photocatalytic oxidation in the NiCo@CN/PMS/Vis system 158
6.3.7 Degradation pathway of IBP and toxicity evaluation 163
6.4 Conclusions 165
CHAPTER 7- CONCLUSIONS AND RECOMMENDATIONS 167
7.1 Conclusions 167
7.2 Recommendations 172

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