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系統識別號 U0026-2507201411445200
論文名稱(中文) 混凝對水中各類溶解性有機物之去除與後續UF薄膜堵塞之關係
論文名稱(英文) The effect of coagulation on each fraction of DOM removal and UF membrane fouling
校院名稱 成功大學
系所名稱(中) 環境工程學系
系所名稱(英) Department of Environmental Engineering
學年度 102
學期 2
出版年 103
研究生(中文) 林晉皞
研究生(英文) Chin-Hao Lin
電子信箱 p56014181@mail.ncku.edu.tw
學號 p56014181
學位類別 碩士
語文別 中文
論文頁數 111頁
口試委員 口試委員-陳孝行
口試委員-黃良銘
指導教授-葉宣顯
中文關鍵字 天然有機物  薄膜材質  混凝前處理  薄膜堵塞 
英文關鍵字 Natural organic matter  membrane material  coagulation pretreatment  membrane fouling 
學科別分類
中文摘要 現今,隨著對水資源的需求及水質標準之逐漸增高,UF薄膜應用在飲用水處理日益廣泛。然而,薄膜堵塞使得通量迅速下降的現象是UF運用上的一大瓶頸。在許多研究中發現,NOM是造成薄膜堵塞的主要物質,因此如何在其進入薄膜系統之前去除是一個值得研究的課題。
本研究目的在於探討混凝前處理對各類溶解性有機物之去除與後續UF薄膜通量下降減緩之關係。首先,分別採集阿公店水庫水與金門太湖淨水廠慢砂濾出流水作為研究之對象。所採集之水樣先經匣式過濾器以去除水中懸浮性顆粒與微生物,接著以明礬於不同劑量下進行混凝前處理,並收集其沉澱後之上澄液,作為後續薄膜過濾之進流水。利用PVC (Polyvinyl chloride)與CA (Cellulose acetate)兩種不同材質之中空纖維膜,於定壓條件下行端點式過濾,並將過濾前後之水樣進行水質分析。主要利用高效能粒徑排除層析儀(HPSEC)連接線上型OC及UV/vis偵測器,分析水中有機物之分子量分佈及特性,並搭配Peak-fit軟體量化之。然後再就溶解性有機物之去除與UF通量下降緩解間之關係進行探討。
實驗結果顯示,親水性之Biopolymer類有機物是造成本研究中薄膜堵塞的主要物質,當其濃度越高,於過濾初始階段,通量下降越明顯。不同材質之薄膜會對各類溶解性有機物有些許不同的作用,除了Biopolymer之外,PVC膜屬疏水性膜,對Humic substance有少量的攔除作用;而CA膜屬親水性,則會對低分子量有機酸有些去除效果。但當進流水所含Biopolymer類有機物濃度較高時,亦可能抑制膜對其他類有機物之去除。
混凝前處理對各類溶解性有機物之去除,會受到添加劑量、原水性質,以及有機物特性所影響,也間接的影響到後續各材質薄膜過濾時,通量下降的減緩程度。疏水性之物質較容易被混凝所去除,其中以Humic substance最為明顯,而親水性之Biopolymer則需在較高劑量下,才有較明顯的去除效果,推測原因在於此時pH值已降至適合大量固態氫氧化鋁生成之範圍,藉由吸附或沉澱絆除之機制而去除之。至於混凝對其他較小分子之有機物,去除效果有限。就路竹而言,混凝劑的增加可提昇對Biopolymer類有機物之去除而減緩PVC膜之堵塞,但對於小分子有機酸的去除較為不易,使其有機物吸附於親水性之CA膜上,而導致對其堵塞之減緩效果受限。就金門而言,PVC與CA膜皆因混凝後Biopolymer濃度仍然過高,而使通量提升之效果不明顯。
整體而言,當Biopolymer含量較高時,會主導通量的下降趨勢;然而當其去除到一定程度後,通量的下降可能會逐漸受到其他有機物的影響。
英文摘要 The effect of coagulation on each fraction of DOM removal and UF membrane fouling

CHIN-HAO LIN
HSUAN-HSIEN YEH
Department of Environmental Engineering, Cheng Kung Univeristy, Tainan, Taiwan

Summary
The effect of coagulation pretreatment on NOM removal from two sources water, namely Lu-Jhu and Kinmen, and on the following UF membrane fouling control was investigated. Two kinds of membrane, made from PVC and CA, were used. The dissolved organics were characterized by HPSEC with UV/Vis and DOC detectors. The results confirmed the hydrophilic biopolymer, which existed in water with high concentration, as the major foulant which caused severe flux decline in the initial stage of UF membrane filtration. Besides biopolymers, PVC and CA membrane also removed small amounts of humic substances and LMW acids, respectively. However, if the concentration of biopolymers was too high, the removal of other organic fractions could be inhibited. Coagulation pretreatment preferably removed biopolymers and humic substances over LMW acids, and the latter was more easily absorbed by CA membrane than PVC membrane. Therefore, the effect of increasing alum dosage on membrane fouling control could be more significant for PVC membrane than for CA membrane. Generally speaking, flux decline was dominated by biopolymers, if it existed in high concentration. The effect of other dissolved organic fractions could become significant, only after the concentration of biopolymers had been reduced to certain level.

Key words: Natural organic matter (NOM), membrane material, coagulation pretreatment, membrane fouling.


INTRODUCTION
As the demand for water sources and its quality increased, the applications of ultrafiltration membrane in drinking water treatment has been more popular. UF membrane can be used to remove particulate matter, microorganic, especially pathogenic protozoa, such as Giardia and Crytosporidia, from source water. However, the phenomenon of rapid flux decline induced by membrane fouling is still a main problem. In literature, NOM has been found to be the major material which caused severe membrane fouling. NOM is a very complex heterogeneous matrix of organic compounds with wide ranges in molecular weight (MW), and with diversified characteristic, which can be originated from the catchment, such as humic substances, and from the water body itself, such as the extracellular polymeric substance (EPS). However, the results from various researchers, concerning the fraction of the organic matter which causes major fouling is still not conclusive or sometimes even contradictory. The objective of this research is to investigate the relationship between the removal of each fraction of dissolved organic matter (DOM) by coagulation pretreatment and the reduction of flux decline in the following UF membrane filtration. The HPSEC with UV/Vis and DOC detectors were used to characterize the NOM of both feed water and permeate, and to clarify the major foulant in UF membrane filtration.

MATERIALS AND METHODS
1.UF feed water preparation
There were two sources of water used in this study, namely that from Lu-Jhu reservoir and slow sand filter effluent of Tai-hu water treatment plant located in Kinmen. As this study was focused on the effect of dissolved organic matter on membrane filtration, the source waters were first filtered by cartridge filters (1.2/0.5 μm & 0.45μm disposable capsule filter, Millipore Corporation, USA) to remove algae and other suspended solids. Then, the filtrate was coagulated by alum with the conventional jar test apparatus and procedure. After that the supernatant was collected, and used as the feed water for the UF membrane filtration.

2.UF membrane filtration
Constant-pressure filtrations (0.68 bar), with PVC (polyvinyl chloride) or CA (cellulose acetate) UF membranes, were conducted with bench-scale dead-end membrane testing system. Single hollow fiber with inside-out flow pattern was used. Membrane flux was determined by weighting the permeate in a top-loading balance at timed intervals with computerized data acquisition.

3.Water quality analysis
The water samples, including source water, feed water and permeate from UF membrane filtration, were analyzed for general physicochemical characteristics, such as pH, turbidity, alkalinity, NPDOC, and UV254. High performance liquid chromatography (HPLC)- size exclusion chromatography (SEC) with sequential on-line ultraviolet (UV) and organic carbon (OC) detectors was used to characterize the composition of dissolved organic matter as a function of apparent molecular weight (AMW). Peak-fitting technique (with software PeakFit) was used to analyze the chromatograms.

RESULTS AND DISCUSSION
1.The source water from Kinmen contained higher concentration of dissolved organic than Lu-Jhu, but the opposite is true for SUVA values, which meant the organic matter from Kinmen was more hydrophilic than that of Lu-Jhu. HPSEC-OCD results also showed that the dominant organic fractions for Kinmen and Lu-Jhu were biopolymers (29.1 %) and humic substances (32.9 %), respectively.
2.For both PVC and CA membranes, the flux decline was more significant for the source water from Kinmen than that from Lu-Jhu. Biopolymer was the major organic fraction removed by UF membrane, therefore it also was considered as the major foulant. Further, the higher the biopolymer concentration was, the more significant the initial flux decline would be.
3.For Lu-Jhu water, in addition to biopolymer, PVC membrane removed small amount of humic substances, while CA membrane removed part of LMW acids. However, for Kinmen water, besides biopolymers, no significant removal for other organic fractions was detected.
4.Humic substances were easily removed by alum coagulation, while biopolymers could be removed only under higher alum dosage, probably through the mechanism of enhanced coagulation. The removal of lower molecular weight organic fractions were minor.
5.Concerning the effect of increasing alum dosage on the flux decline control for the following UF membrane filtration, the results show that, for Lu-Jhu water, increasing alum dosage effectively reduced the flux decline rate of PVC membrane. However, the effect on CA membrane was minor. For Kinmen water, the effect on increasing alum dosage on flux decline control was insignificant for both PVC and CA membranes.

CONCLUSION
1.The hydrophilic biopolymer was significantly removed by UF membrane, and confirmed as the major foulant. If existed in high concentration, it could cause sharp flux decline at the initial stage of filtration.
2.UF membranes also removed small amount of humic substances or LMW acids. However, the existence of high concentration of biopolymers could inhibit this phenomenon.
3.Coagulation pretreatment preferably removed biopolymers and humic substances over LMW acids, and the latter was more easily absorbed by CA membrane than PVC membrane. Therefore, the effect of increasing alum dosage on membrane fouling control could be more significant for PVC membrane than for CA membrane.
4.Generally speaking, flux decline was dominated by biopolymers, if it existed in high concentration. The effect of other dissolved organic fractions could become significant, only after the concentration of biopolymers had been reduced to certain level.
論文目次 目錄
摘要 I
Abstract III
誌謝 VII
目錄 IX
表目錄 XII
圖目錄 XIII
第一章 前言 1
1-1研究緣起 1
1-2研究目的 2
第二章 文獻回顧 3
2-1天然有機物 3
2-1-1 NOM之生成來源 3
2-1-2 NOM對淨水處理的影響 4
2-1-3 NOM特性分析 4
2-1-4螢光光譜儀(Fluorescence Spectrometry)偵測有機物原理與特性 9
2-1-5粒徑排除層析儀偵測有機物原理與特性 16
2-2薄膜處理程序 21
2-2-1薄膜種類 21
2-2-2薄膜模組 23
2-2-3過濾方式及流動狀態 25
2-2-4 UF薄膜介紹 27
2-2-5 UF薄膜材質 30
2-3薄膜堵塞 32
2-3-1薄膜堵塞之機制 32
2-3-2可逆與不可逆堵塞 33
2-3-3堵塞物質 34
2-3-4 NOM產生之薄膜堵塞 35
2-4混凝程序 37
2-4-1混凝機制 37
2-4-2鋁鹽之混凝 40
2-4-3混凝去除NOM 42
2-4-4混凝前處理對UF薄膜堵塞之改善 44
2-4-5混凝前處理對薄膜效能之負面影響 46
2-4-6混凝操作條件對薄膜效能之影響 47
第三章 實驗流程與方法 51
3-1實驗流程 51
3-2混凝瓶杯試驗 53
3-3薄膜過濾試驗 53
3-4水質分析 57
3-4-1 pH值 57
3-4-2 濁度 57
3-4-3 鹼度 57
3-4-4非揮發溶解性有機物(Non-Purgable Dissolved Organic Carbon, NPDOC)分析 58
3-4-5 UV254吸光值 59
3-4-6螢光激發/發散陣列光譜(Fluorscence Excitation/Emission Matrix, F-EEM)分析 60
3-4-7高效能粒徑排除層析儀(High Performance Size Exclusion Chromatography, HPSEC) 61
3-5薄膜表面接觸角分析 64
第四章 結果與討論 65
4-1水樣性質分析 65
4-2水樣性質對薄膜通量變化之影響 72
4-3薄膜材質親疏水性之通量變化比較 77
4-4混凝前處理 80
4-5混凝前處理對薄膜通量下降之影響 89
4-5-1路竹結果 89
4-5-2金門結果 92
第五章 結論與建議 95
5-1結論 95
5-2建議 96
參考文獻 97
附錄 109
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