臺灣博碩士論文加值系統

在新型微濾膜生物反應器（MF-MBR）系統中應用銀納米粒子（AgNPs）來減輕膜生物污染，用於廢水處理，再利用，同時減少膜生物污損，實現高水質和低能耗。膜生物污損已成為限制膜技術的更廣泛傳播和應用的嚴重缺點。膜生物反應器是一種廢水處理技術，將活性污泥工藝與微濾和超濾相結合，由於穩定的操作性能，高產品水質，減少剩餘污泥產量，被廣泛認為是市政和工業水處理和再利用的有效工具。 ，減少物質風險，廢水再利用和低佔地面積。膜生物反應器技術提供了優於傳統廢水處理系統的競爭優勢，然而，MBR技術的障礙是膜污染問題的高速率因此導致生產率降低和更高的膜更換和操作成本。因此，本研究旨在確定主要污垢和主要污垢機制，如濃差極化，無機沉澱，孔隙阻塞，有機吸附，蛋糕形成和生物污染。該研究還旨在研究在MBR系統中用於廢水處理的膜應用過程中膜污染的不同現象。該研究使用銀納米顆粒（AgNPs，納米銀）來減輕膜生物污損潛力，其中使用微濾（MF）膜。通過在膜表面上使用AgNP的表面塗層，用納米銀修改MF膜組件，以通過新的化學還原方法將銀納米顆粒固定在膜上。研究了用於抗微生物性質，滲透性和銀浸出的任何改變的改性膜。膜生物反應器在良好條件下操作以確保適合細菌生長的環境。該體系的MLSS和MLVSS分別為14860 mg MLSS / L和11345 mg MLVSS / L，最適pH範圍為6.5~8。該體系的COD，PO43 - P和NH4 + -N去除率約為99.7。在兩個操作膜組件的組合中，每天收集的滲透物體積分別為％，97.8％和99.4％，每天收集的滲透物體積接近6L / d，M-AgNPs和M-平膜的平均水通量為5.33L / m2 h和5.15 L / m2 h。通過水通量變化測試，SEM和EDS分析，壓力變化測試以及ABT和VST分析進行結果分析以確定納米銀塗層膜對生物污垢的緩解，其中所有證明使用銀納米顆粒均為陽性。 ，在緩解膜生物污損方面具有很好的抗菌作用。結果表明，納米銀改性膜的滲透性略高於未改性膜。該研究的結果還證實，根據所進行的批次測試的ICP分析，銀修飾膜中的銀浸出最小且不顯著，這低於廢水和水中銀的最大污染物限制（MCL）的國際標準。治療應用由美國環境保護署（USEPA）和世界衛生組織（WHO）建立，濃度為0.1 mg / L，相容且可接受。實驗結果也成功地揭示了AgNPs修飾膜具有很好的抗菌性能，從而減輕了膜的生物污染。

The application of silver nanoparticles (AgNPs) for mitigating membrane biofouling in a novel microfiltration membrane bioreactor (MF-MBR) system was proposed for wastewater treatment, and reuse and to simultaneously reduce membrane biofouling, achieve high water quality, and less energy consumption. Membrane biofouling has become a serious drawback limiting the wider spread and application of the membrane technology. Membrane bioreactor is a wastewater treatment technology that combine the activated sludge process with micro- and ultrafiltration and is widely regarded as an effective tool for municipal and industrial water treatment and reuse due to stable operation performance, high product water quality, reduction in excess sludge production, reduction of risk of substances, effluent reuse, and low footprint. Membrane bioreactors technology offers a competitive advantage over conventional wastewater treatment systems however, the impediment of the MBR technology is the high rate of membrane fouling problems consequently resulting to reduction in productivity and higher membrane replacement and operating cost. Hence, this study aims to identify the major foulants and the principal fouling mechanisms such as concentration polarization, inorganic precipitation, pore blocking, organic adsorption, cake formation and biological fouling. The study is also aimed at investigating the different phenomena of membrane fouling during the membrane application in the MBR system for wastewater treatment. This study used silver nanoparticles (AgNPs, nanosilver) to mitigate membrane biofouling potentials in which a microfiltration (MF) membrane was used. The MF membrane modules were modified with nanosilver through the use of surface coating of the AgNPs on the surface of the membrane, to fix the silver nanoparticles on the membrane by a novel chemical reduction approach. The modified membranes for any alterations in antimicrobial properties, permeability, and silver leaching were examined. The membrane bioreactor was operated in good conditions to ensure a suitable environment for the bacterial growth. The MLSS and MLVSS of the system were 14860 mg MLSS/L and 11345 mg MLVSS/L respectively, with an optimum pH range of 6.5 to 8. The system had an approximate COD, PO43--P and NH4+-N removal percentage of 99.7%, 97.8% and 99.4% respectively and the volume of permeate collected per day approximates to 6 L/d in combination of the two operating membrane modules, the M-AgNPs and the M-plain membranes had an average water flux of 5.33 L/m2 h and 5.15 L/m2 h respectively. The results analysis to determine the mitigation of biofouling by the nanosilver coated membrane was performed with the water flux variation test, the SEM and EDS analysis, pressure variation test, and the ABT and VST analysis, in which all proofed positive for using the silver nanoparticles, having great antimicrobial effects in mitigating membrane biofouling. The results revealed that the nanosilver modified membrane showed slightly higher permeability than the unmodified membrane. The results from this study also confirmed that silver leaching from the silver modified membrane was minimal and insignificant according the ICP analysis from the batch tests conducted, which was lower than the international standard for the maximum contaminant limit (MCL) of silver in wastewater and water treatment applications, established by the United States Environmental Protection Agency (USEPA) and the World Health Organization (WHO) at 0.1 mg/L which was compatible and acceptable. The results from the experiment also successfully revealed that the modified membrane with AgNPs displayed great antimicrobial properties thus, mitigated membrane biofouling.

TABLE OF CONTENTS

ABSTRACT i
ACKNOWLEDGEMENT iii
TABLE OF CONTENTS iv
LIST OF FIGURES viii
LIST OF TABLES x

CHAPTER 1: INTRODUCTION 1
1.1 Research Background and Motivation. 1
1.2 Objectives and Scope of the Research 2
1.3 Brief Outline of the Thesis 4

CHAPTER 2: LITERATURE REVIEW 5
2.1 Municipal wastewater and its impacts on the environment 5
2.2 Wastewater characteristics and discharge standards 7
2.3 Conventional biological treatment process versus membrane bioreactors (MBR) 9
2.3.1 Conventional biological treatment process (CASP) 9
2.3.2 Membrane bioreactor (MBR) 11
2.3.3 The merits of MBR over conventional biological process (CBP) 14
2.4 Introduction of membrane 15
2.4.1 Membrane types 15
2.4.2 Microfiltration membrane (MF) 16
2.5 Membrane fouling and mitigation mechanisms 18
2.5.1 Types of membrane fouling 20
2.5.1.1 Organic fouling 20
2.5.1.2 Inorganic fouling 22
2.5.1.3 Biofouling 24
2.5.1.3.1 Effects of biofouling on performance of MF membrane units 26
2.5.1.3.2 Identification of biofouling 28
2.5.1.3.3 Monitoring of membrane biofouling. 28
2.5.2 Classification of membrane fouling. 30
2.5.2.1 Removable and irremovable fouling (Reversible fouling) 30
2.5.2.2 Irreversible membrane fouling 32
2.5.3 Classification of membrane foulants. 32
2.5.4 Mechanisms of membrane fouling. 33
2.5.5 Factors affecting membrane fouling 35
2.5.5.1 Membrane characteristics 35
2.5.5.1.1 Membrane material 35
2.5.5.1.2 Water affinity 36
2.5 .5.1.3 Membrane pore size 36
2.5.5.2 Operating conditions 37
2.5.5.2.1 Aeration rate 37
2.5.5.2.2 Solids Retention Time (SRT) 37
2.5.5.2.3 Food-Microorganisms (F/M) Ratio. 38
2.5.5.2.4 Organic Loading Rate (OLR). 38
2.5.5.3 Feed and biomass characteristics 39
2.5.5.3.1. Mixed Liquor Suspended Solids (MLSS) 39
2.5.5.3.2. Extracellular Polymeric Substances (EPS) 39
2.5.5.3.3. Alkalinity and pH. 40
2.5.6 Membrane biofouling control/mitigation 43
2.5.6.1. Feedback control 43
2.5.6.2. Addition of flux enhancers 43
2.5.6.3 Addition of nanomaterials (e.g. silver nanoparticles) 44
2.5.6.4 Quorum quenching (inhibition of quorum sensing) 45
2.6 Silver nanoparticles (nanosilver) 46
2.6.1. Properties and characteristics behavior of AgNPs 46
2.6.2. Potentials of silver nanoparticles as an antimicrobial/antibacterial foulant 47
2.6.3. Mechanisms of silver nanoparticles action in bacteria and potential for bacterial resistance. 47
2.6.4. Applications of silver nanoparticles (AgNPs) 49
2.6.5 Environmental impacts of using silver nanoparticles (negative effects of AgNPs) 50

CHAPTER 3: MATERIALS AND METHODS 53
3.1 Experimental design 53
3.2 Materials and experimental equipment 55
3.2.1 Membrane material 55
3.2.2 Experiment equipment/apparatus 56
3.3 Synthesis and preparation of silver nanoparticles (AgNPs) 57
3.3.1 Synthesis of silver nanoparticles (nanosilver). 57
3.3.2 Detection and analysis of silver nanoparticles 60
3.4 Preparation of the microfiltration (MF-membrane) modules. 61
3.4.1 Preparation of the membrane material and membrane module. 61
3.4.2 Attachment/fixing and analysis of the silver nanoparticles onto the MF- membrane 62
3.4.3 Silver nanoparticles concentration analysis on the membrane surface 64
3.5 Measurement and analytical methods 65
3.5.1 Water flux and pressure variation analysis 65
3.5.2 Membrane fouling analysis. 66
3.5.3 Phosphate analysis 67
3.5.4 Nitrogen analysis 67
3.5.5 Silver nanoparticles (AgNPs) analysis (Stability analysis). 67
3.6 Activated sludge source and feed solution preparation for the MF-MBR system. 68
3.6.1 Activated sludge source 68
3.6.2 Feed solution preparation for the MF-MBR system. 68
3.6.3 Preparation of chemicals and reagents 69

CHAPTER 4: RESULTS AND DISCUSSION 70
4.1 Bioreactor treatment results 70
4.1.1 pH and temperature variation in the bioreactor 70
4.1.2 COD variation and removal efficiency 71
4.1.3 MLSS and MLVSS variation in the bioreactor 72
4.1.4 Nutrients variation and removal efficiency in the system 74
4.2 Silver nanoparticles characteristics 75
4.2.1 Transmission electron microscopy (TEM) analysis of the AgNPs 75
4.2.2 UV-vis analysis of the silver nanoparticles (AgNPs) 75
4.3 Membrane properties and characterization 76
4.4 Stability of AgNPs containing membrane and silver leaching analysis 78
4.4.1 Stability of the silver containing membrane (M-AgNPs) 78
4.4.2 Silver leaching analysis of the silver coated membrane (M-AgNPs) 79
4.5 Membrane fouling (biofouling) analysis 80
4.5.1 Membrane performance for water filtration (water flux variation) 80
4.5.2 Pressure variation test analysis (working pressure test) 82
4.5.3 Specific flux and specific flux decline analysis by linear model. 84
4.5.4 SEM and EDS biofouling analysis of the membranes after the experiment 86
4.5.5 Fourier-transform infrared spectroscopy (FTIR) analysis 90
4.5.6 Attached biomass test (ABT) and volatile solid test (VST) analysis 91

CHAPTER 5: CONCLUSION AND RECOMMENDATIONS 96
5.1 Conclusion 96
5.2 Recommendations 97
REFERENCES 98
APPENDIX 1: NOMENCLATURE AND ABBREVIATION 105

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