石墨化氮化碳(g-C3N4)複合材料用於可見光催化降解污染物的開發

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研究生：	阮孟容 Nguyen, Manh-Dung
論文名稱：	石墨化氮化碳(g-C3N4)複合材料用於可見光催化降解污染物的開發 Development of Graphitic Carbon Nitride (GCN) Composites for Photocatalytic Degradation of Pollutants under Visible-light Irradiation
指導教授：	董瑞安 Doong, Ruey-An
口試委員:	吳劍侯 Chien, Hou-Wu 蘇鎮芳 Su, Jenn-Fang 陳慶隆 Chen, Ching-Lung 林亮毅 Lin, Liang-Yi
學位類別：	博士 Doctor
系所名稱：	原子科學院 - 生醫工程與環境科學系 Department of Biomedical Engineering and Environmental Sciences
論文出版年：	2023
畢業學年度：	111
語文別：	英文
論文頁數：	230
中文關鍵詞：	光催化、石墨氮化碳、共摻雜、MnO2 、結構 Z 型光催、PMS
外文關鍵詞：	photocatalyst, GCN, co-doping, MnO2, Z-scheme, PMS
相關次數：	點閱：3 下載：0
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基於半導體的光催化技術是一種有效解決方案解決全球能源短缺。石墨氮化碳 (g-C3N4) 基材料最近被用做廢水淨化的光催化劑。為了增加g-C3N4的載流子和電荷傳輸，故研究了修飾的進展和修飾的相關功能，例如應用於光催化性能的形態特徵、元素摻雜、缺陷工程和異質結構。近年來，共摻雜和基於g-C3N4的異質結構之材料受到很大的關注，摻雜已被廣泛應用於調節 g-C3N4 的催化活性，這可以改變其理化特性，例如電子遷移率和電導率。同時，異質結構 Z 型光催化劑改善了載流子分離，提高了光催化效率，顯著提升了太陽能利用和轉換性能，因此，本論文為設計和製備g-C3N4基光催化劑提供了可能的趨勢，可有效去除廢水中的有機污染物。首先，磷氟共摻雜的g-C3N4縮小了能隙，改善了電荷分離，縮短了擴散長度，從而提高了電導率和電子傳輸速率。因此，在不同環境條件下，CNPF 的四環素光降解率比原始 g-C3N4高了 4.2 至 11.7 倍。其次，將花瓣狀的MnO2 與 B、S 共摻雜 g-C3N4 (CNBS) 管雜化，設計出一種新型空心核殼 Z 型異質結構，促進光生載流子的分離，在最佳反應條件下(CNBS/MnO2 的劑量 = 0.5 g L-1，pH = 7 和時間 = 15 分鐘）表現出令人滿意的 99% DCF (20 mg L-1) 降解率，PMS 劑量 = 0.06 mM。綜上所述，本研究開發了一種新型環保型 g-C3N4基催化劑，具有低成本、高效率，可用於廢水處理中有機污染物的選擇性降解.

One effective solution for addressing the global energy shortage is semiconductor-based photocatalytic technology. Graphitic carbon nitride (GCN)-based materials have recently been used as photocatalysts for wastewater decontamination. To increase the carrier and charge transport perceptions of GCN, the modification advancements and related functions of the modification were approached, such as morphological characteristics, elemental dopants, deficit engineering, and heterojunction, which were applied in photocatalytic performance. Recently, co-doping and the construction of GCN-based heterostructures have been hot topics recently. Doping has been widely utilized as an efficient method to regulate the catalytic activity of GCN, which could change its physiochemical properties, such as electron mobility and conductivity. Meanwhile, heterojunction Z-scheme photocatalysts enhanced charge carrier separation for increased photocatalytic effectiveness, boosting solar energy utilization and conversion performance impressively. Therefore, this thesis provides the possible tendency in designing and fabricating GCN-based photocatalysts, which effectively eliminate organic contaminants from wastewater. Firstly, phosphorous and fluorine co-doped GCN narrowed the band gap, increases the electric conductivity and electron transfer rate by reducing the diffusion length, boosting the charge separation. As a result, the CNPF shows a tetracycline photodegradation rate 4.2-11.7 times greater than that of pure GCN all over a range of environmental conditions. Secondly, flower-like MnO2 is hybridized with B, S co-doped GCN (CNBS) tube design a novel hollow core-shell Z-scheme heterojunction, promoting photon-generated carrier separation. Under the optimum reaction condition (dosage of CNBS/MnO2 = 0.5 g L−1, pH = 7 and time = 15 min) exhibited satisfactory 99% removal photodegradation of DCF (20 mg L-1) with PMS dosage =0.06 mM. To sum up, our research developed a unique low-cost and highly effective GCN bases-catalyst for the various degradation of organic pollutants in wastewater treatment

Contents
ABSTRACT    iii
OUTLINE    v
LIST OF TABLES    ix
LIST OF FIGURES    xi
ABBREVIATIONS, UNITS, AND SYMBOLS    xvii
Chapter 1: Introduction    1
1. Motivation    1
2. Overviews of PPCPs    5
2.1. Classification of PPCPs    5
2.2. Environmental transport routes of PPCPs.    7
3. Advanced oxidation process in PPCPs removal    15
4. Overviews of photocatalyst    23
4.1. Solar energy utilization    23
4.2. Mechanism of Photocatalysis    25
4.3. Heterostructure Photocatalysts    27
5. Aim and objectives    31
6. Thesis outline    35
.  Chapter 2: Overview of photocatalysts and strategies    36
1. Graphitic carbon nitride (GCN)    37
1.1. Structure of GCN    37
1.2. Electronic properties of GCN    40
1.3.  Applications of GCN    41
2. Synthesis strategies    45
2.1. Bottom-up approaches.    45
2.2. Top-down approaches.    49
2.3. Modification approaches    52
2.4. Strategies for Engineering GCN    59
3. Functional modification    59
3.1. Defects    59
3.2. Heterojunction construction with GCN    71
3.3. Peroxymonosulfate (PMS)    78
4. Manganese dioxide (MnO2)    88
4.1. Structure of Manganese oxides    89
4.2. Synthesis of MnO2 and its composites    97
Chapter 3: Material and Methodology    102
1. Reagent and chemical    102
2. Photocatalyst preparation    102
2.1. Synthesis of F, P-codoped GCN (CNPF)    102
2.2.  Synthesis of hollow B, S co-doped GCN (CNBS)    103
2.3.  Synthesis CNBS@MnO2 nanocomposites    103
3. Characterization of photocatalyst    104
4. Photocatalytic degradation of phototocalyst    105
4.1. Photocatalytic activity of CNPF toward TC degradation    105
4.2. Photodegradation of DCF by CNBS@MnO2    105
5. Toxicity assay    106
Chapter 4:  Results and discussion    108
1. Supramolecular self-assembly of F, P-codoped tubular graphitic carbon nitride with enhanced visible-light-driven photocatalytic activity for tetracycline degradation    108
1.1. Characterization of CNPF-x photocatalysts    108
1.2. Optical property and band structure of CNPF-x    117
1.3. Photocatalytic degradation of TC over CNPF-x    122
1.4.  Effect of environmental parameters on TC photodegradation    124
1.5. Reusability and possible mechanism    130
1.6. Conclusions    136
2. Z-scheme S, B co-doped GCN nanotube@MnO2 heterojunction with visible-light-responsive for enhanced photodegradation of diclofenac by peroxymonosulfate activation    138
2.1. Morphology and microstructure of CNBS@MnO2 photocatalysts    138
2.2. Optical and electrochemical properties    144
2.3. Photocatalytic activity of CNBS@MnO2 toward DCF degradation    147
2.4. Identification of reactive oxidation species    160
2.5. Degradation pathway    171
2.6. Conclusions    173
Chapter 5: Conclusions and future scope of the work    174
1. Conclusions    174
2. Future scope of the work    176
List of publications    180
References    182


                                

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