此篇論文在於利用石墨烯複合材料應用於廢水處理之研究。研究中建立一高效率的石墨烯複合吸附材料之製備方法，並具有高吸附性、耐久度以及再利用性，並藉由添加其他材料合成出的石墨烯複合材料，可呈現出針對特定物質的選擇性吸附效果，可實際應用於商業化的廢水處理技術。
首先在具有乙二醇的溶劑裡，利用微波輔助法製備出還原氧化石墨烯/活性碳 (rGO/AC) 複合材料，此複合材料具有層次性的孔洞結構並且具備出色的電吸附特性。製備出rGO/AC電極不但可達到18.6 ± 1.2 mg g−1 的電吸附量外，並有極佳的倍率以及循環穩定性，將可實際應用於電容脫鹽 (CDI) 技術中。
接著此研究利用氧化石墨烯 (GO)以及鎂錳層狀雙氫氧化物 (LDH) 之複合物，利用一超高效率之電輔助方法並應用於廢水中磷酸跟的移除和回收技術。藉由施加可變換的電壓差，可控制LDH複合材料表面和磷酸跟之間的靜電作用力，而達到0.79 mg‐P g−1 min−1和3.56 mg‐P g−1 min−1之卓越的磷酸跟吸附和脫附速率。
第三此研究展示出一環境友善之抗菌吸附材料，並對於廢水中的磷酸跟有極佳的選擇性及回收能力。此研究利用亞洲福木之葉子為天然的生物模板，並將MgMn-LDH以及GO原位成長於上。此複合材之磷酸跟吸附量可達到244.08 mg-P g-1 而脫附率為85.8%，其極佳的磷永續利用性在於此材料具有層次性的孔狀結構並提供眾多的磷活性吸附點，將可實際應用於自然水體的再生技術。

This thesis aims to explore the effective methods for wastewater treatment using graphene composite materials. In this study we developed efficient processes for fabricating graphene-adsorbent composite with high adsorption capacity, long-term stability, and recyclability. With the introduction of various materials, the graphene composites possess species-specific selectivity, which is practical for commercial wastewater treatment.
Firstly, reduced graphene oxide (rGO)/activated carbon (AC) composites with hierarchically porous structure performing excellent electrosorption property was prepared in the presence of ethylene glycol (EG) under microwave irradiation. The rGO/AC composite electrode performs outstanding electrosorption capacity of 18.6 ± 1.2 mg g−1 having excellent rate performance and reversibility, which is applicable for capacitive deionization (CDI).
Second, we reported an ultra-efficient electro-assisted process for high selective removal-recycle of phosphate in wastewater based on graphene oxide (GO)/MgMn-layered double hydroxide (LDH) composites. Tunable applied potential difference controls the electrostatic interactions between the LDH composites and the phosphate, which results in the superior adsorption and desorption rates of 0.79 and 3.56 mg‐P g−1 min−1, respectively.
Thirdly, this study demonstrates an eco-friendly antimicrobial adsorbent with high selective recycling of phosphate in wastewater. It adopted Garcinia subelliptica leaves as a natural bio-template, where MgMn-LDH and GO can be grown in situ. The phosphate sustainability with adsorption capacity and desorption rate of 244.08 mg-P g-1 and 85.8%, respectively, can be achieved owing to a hierarchical porous structure and more phosphate-specific active sites, which are practical for reconstruction aquatic communities.

摘要 iii
Abstract iv
Acknowledgement v
Table of contents vii
List of tables x
List of figures xi
Chapter 1 Overview 1
1.1 Introduction to wastewater treatment 1
1.1.1 Membrane method 1
1.1.2 Coagulation method 2
1.1.3 Adsorption method 3
1.1.4 Advanced oxidations method 4
1.1.5 Biological method 5
1.1.6 Electrosorption method 6
1.2 Introduction to carbon materials 7
1.2.1 Activated carbon 7
1.2.2 Graphene oxide 8
1.2.3 Reduced graphene oxide 9
1.3 Introduction to layered double hydroxide 9
1.3.1 Adsorption mechanisms of LDHs 10
1.3.2 Factors affecting adsorption of LDHs 11
1.3.3 Calcination and memory effect 11
1.3.4 Regeneration of LDH 12
1.4 Aims of this investigation 12
Chapter 2 Experiments and characterizations 22
2.1 Synthesis of GO 22
2.2 Preparation of 3D porous rGO/AC-p composites 23
2.3 Preparation of MgMn-LDH and GO/MgMn-LDH composites 23
2.4 Fabrication of electrodes 24
2.4.1 Fabrication of rGO/AC-p and AC-p electrodes 24
2.4.2 Fabrication of LDH composites electrodes 24
2.5 Preparation of leaf-templated GO/MgMn-LDH composite 24
2.6 Electrochemical measurements of rGO/AC-p electrode 25
2.6.1 Cyclic voltammetry measurement 25
2.6.2 Electrochemical impedance spectrometry 26
2.6.3 Electroactive surface area measurement 26
2.6.4 Electrosorption capacities and charge efficiency 27
2.7 Electrochemical characterization of the LDH composites electrodes 28
2.8 Measurements of pollutants uptake and release 28
2.9 Phosphate adsorption capacity and kinetics 28
2.10 Antimicrobial ability study of LDH composites 29
2.11 Density functional theory total energy calculations: 29
2.12 Characterization techniques 30
Chapter 3 Microwave-assisted method for highly electrosorptive reduced graphene oxide/activated carbon composite electrode 32
3.1 Research background 32
3.2 Results and discussion 33
3.2.1 The mechanisms of EG as a dielectric medium 33
3.2.3 The structure characterizations of composites 34
3.2.4 Characterizations of wettability and functionality 35
3.2.5 Electrochemical properties of electrodes 37
3.2.6 Characterizations of the mechanisms for microwave irradiation process 39
3.2.7 Characterizations of CDI performance 40
3.3 Summaries 42
Chapter 4 Electro assisted selective uptake / release of phosphate using graphene oxide/MgMn-layered double hydroxide composite 57
4.1 Research background 57
4.2 Results and discussion 58
4.2.1 Continuously electro-assisted selective phosphate adsorption-desorption 58
4.2.2 Structure and elemental characterizations of LDH composites 59
4.2.3 Characterizations of morphologies and porosity 62
4.2.4 Characterizations of the elements and bondings of the LDH composites 64
4.2.5 Electrochemical characterizations of LDH composites 64
4.2.6 Electro-assisted phosphate adsorption-desorption performance 65
4.2.7 The mechanisms of selective phosphate electrosorption-desorption 67
4.3 Summaries 68
Chapter 5 Green treatment of phosphate from wastewater using a porous bio-templated graphene oxide/MgMn-layered double hydroxide composite 83
5.1 Research background 83
5.2 Results and discussion 84
5.2.1 Phosphate uptake and release 85
5.2.2 Characterizations of the hierarchical porous structure of LDH composites 85
5.2.3 Characterizations of the compositions of LDH composites 86
5.2.4 Characterizations of the variations of nanostructures by in situ TEM 88
5.2.5 Characterizations of the elements and bondings of the LDH composites 89
5.2.6 Characterizations of practical phosphate sustainability in wastewater 91
5.2.7 The investigations of selective phosphate adsorption 94
5.3 Summaries 95
Chapter 6 Conclusions 114
References 116
Publications 125

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