臺灣博碩士論文加值系統

現今水庫優養化情形日益嚴重，而當以UF (Ultrafiltration)薄膜處理優養化原水時，水中自然有機物(NOM)是造成薄膜阻塞的原因之一，而不同材質之薄膜對於其阻塞程度又有所不同，其通量表現與水中有機物組成、薄膜之材質及性質、孔洞大小等皆有關聯，由於本研究之重點在於溶解性NOM對UF膜阻塞之影響，故將採集南台灣水庫優養化天然原水，經 0.45μm薄膜過濾器過濾，然後將濾液，以自行配製之不同鋁形態PACl在不同劑量下進行混凝，探討對水中溶解性有機物去除之情形。再取上澄液用PVC (Polyvinyl Chloride)及CA (Cellulose Acetate)材質之中空絲纖維(Hollow-fiber)膜進行過濾，探討混凝前處理以及不同材質之薄膜對通量之影響及對有機物去除之效果。
混凝前處理結果顯示，在高混凝劑量下，混凝劑PACl0 (B = 0)對溶解性有機物去除效果高於PACl20 (B = 2)。是由於PACl20中鋁物種以聚合鋁(Alb)為主；而PACl0成分以單體鋁(Ala)為主。在高劑量下，混凝劑PACl0在水解過程中形成聚合鋁並消耗鹼度，使pH值降至6.3左右。此pH值接近氫氧化鋁最低溶解度，因此形成大量Al(OH)3(s)，並幫助吸附水中溶解性有機物。
薄膜試驗結果顯示，混凝對PVC膜及CA通量改變皆有正面效果，而由電子顯微鏡(Scanning Electron Microscopy, SEM)觀察膜表面之阻塞物結構，經混凝前處理者與未經混凝者也有明顯不同，顯示混凝改變阻塞物之型態，推測可能使薄膜上cake層趨於多孔性質，進而幫助通量恢復。
PVC膜之通量下降速率隨混凝劑量增加而下降，而經HPSEC (High Performance Size Exclusion Chromatography)分析結果顯示，PVC膜可去除大分子的biopolymers，但對其他分子量之分子則無法去除。且在混凝程序中，隨混凝劑增加，biopolymers去除效果逐漸增加，而PVC膜通量之下降程度逐漸減輕，顯示biopolymers為造成PVC膜阻塞的主要原因。在CA膜通量方面，原水過膜與經混凝後過膜通量有明顯差異，也顯示混凝對通量有恢復效果，但在不同混凝劑量間通量卻無明顯差異。
由HPSEC結果顯示，CA膜除了能去除biopolymers，也可去除部分小分子酸。由於此類小分子酸屬親水性物質，而CA膜屬親水性膜，因此有較高親和力使其被吸附於薄膜上。比較CA膜之通量以及HPSEC之圖譜後發現，在原水過膜通量有兩階段阻塞，是因biopolymers之分子量約105，而CA膜之MWCO (Molecular Weight Cut Off)為100 kDa，因此阻塞形態偏向孔徑密封，造成在初期通量下降較快，隨後cake層形成，通量下降速率減緩而形成兩階段阻塞。再者由於小分子酸不容易被混凝去除，且分子量遠小於薄膜孔洞大小，所以推測即使經過混凝，小分子酸仍有可能在薄膜孔洞內被吸附，因此造成不同混凝劑量間通量差異不大。

Eutrophication is becoming a serious problem for reservoirs today. Natural organic matter (NOM) may cause fouling when using UF (Ultrafiltration) membrane to treat eutrophicated source water. Fouling phenomena can be varied with the organic contents in the feed water, membrane material, and pore size, etc. In this study, the effect of coagulation pretreatment and the material of hollow-fiber UF membrane on NOM fouling was studied. The source water from an eutrophic reservoir in souther Taiwan was collected. As this study was focused on the dissolved organic part, the source water was firstly filtered by 0.45 μm membrane filter. Secondly, the filtrate was subjected to coagulation by laboratory-prepared polyaluminum chloride (PACl), with different basicity (B value). Then the filtrated and the caogulation-treated water were filtered through bench-scale hollow-fiber UF membrane unit under constant pressure. Two kind of UF membranes with different material were tested, namely polyvinyl chloride (PVC) and cellulose acetate (CA).
The coagulation results show that at high dosage PACl0 (B = 0) had high dissolved organic removal that of PACl20 (B = 2). The explanation is: the dominant aluminum species in PACl0 are monomeric aluminum species (Ala), while those in PACl20 are polymeric aluminium species (Alb). At higher dosage, the hydrolysis of PACl0 to form polymeric aluminum species, would consume alkalinity, and drop the pH to lower value, around 6.3. At this pH value, large amount of Al(OH)3(s) could form, and facilitate the DOC removal via adsorption.
Coagulation pretreatment was found to improve the performance of both PVC and CA based UF membrane filtration by reducing flux decline rate. Based on SEM images, it can be noticed that cake layer structure on fouled membranes were different between those from feed water with and without precoagulation. Apparently, coagulation altered the cake layer, probably made it more porous.
Based on the results from HPSEC (High Performance Size Exclusion Chromatography), the PVC membrane was found to remove only the microorganism-related extracellular polymer substance (EPS) fraction of NOM, while the CA membrane removed portion of low-molecular weight acids (LMW acids), in addition to EPS fraction. LMW acids could be removed because it was hydrophilic, and tented to be adsorbed by hydrophilic CA membranes. Further, the flux decline rate of PVC membrane was found to be reduced with increasing PACl dosage of precoagulation. As the EPS removal during coagulation was also increased with increasing coagulant dosage, it is speculated that EPS were the main foulant of PVC membrane.
For CA membrane, the flux decline rate curve of the un-precoagulated feed water showed two stages type, with a fast decline first stage, and a low second decline stage after that. It was speculated that the initial fast flux decline was caused by pore blocking, as the molecular weight of large amount of EPS in the un-precoagulated feed water was closed to the pore size of CA membrane. Further, the effect of PACl dosage on CA membrane flux decline was not as obvious as that of PVC membrane. This is probably due to the lower coagulation removal efficiency of LMW acids, which may cause membrane fouling by adsorption inside the pore.

摘要 I
Abstract III
誌謝 V
目錄 VI
圖目錄 IX
表目錄 XII
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 水體優養化所衍生之問題 3
2-2 水中有機物之特性 5
2-2-1 NOM之簡介 5
2-2-2 水體有機物鑑定分析技術 7
2-2-2-1螢光偵測有機物之原理及特性 7
2-2-2-2 SEC偵測分子量之原理及特性 12
2-3 混凝程序 16
2-3-1 混凝機制 16
2-3-2 鋁鹽之水解型態 22
2-4 薄膜程序 24
2-4-1 薄膜種類及過濾機制 24
2-4-2 薄膜材質 26
2-4-3 薄膜模組 29
2-4-4過濾方式及流動狀態 29
2-4-5 UF薄膜簡介、過濾原理及應用 31
2-5 薄膜阻塞 33
2-5-1 薄膜阻塞型態 33
2-5-2 NOM所引起之薄膜阻塞 35
2-6 混凝前處理和薄膜過濾 38
2-6-1 混凝前處理對薄膜效能之改善 38
2-6-2 混凝前處理對薄膜效能之負面影響 40
2-6-3 混凝劑量與操作條件對薄膜效能之影響 41
第三章、實驗程序與方法 45
3-1 實驗程序 45
3-2 混凝劑聚氯化鋁之製備 47
3-3 混凝瓶杯試驗 49
3-4 薄膜過濾實驗 50
3-5 水質分析 53
3-5-1 殘餘鋁分析 53
3-5-2 pH值 54
3-5-3 UV254吸光值 54
3-5-4 濁度 54
3-5-5 非揮發溶解性有機碳(NPDOC) 55
3-5-6 膠羽表面電位測定 56
3-5-7 高性能粒徑排除層析儀 58
3-5-8 螢光激發/發散陣列光譜儀 60
3-6 膜表面分析 60
第四章、結果與討論 61
4-1混凝結果 61
4-1-1 原水性質分析 61
4-1-2 不同混凝劑對原水混凝結果比較 65
4-2薄膜過濾結果 73
4-2-1 PVC膜過濾結果分析 73
4-2-2 CA膜過濾結果分析 80
4-2-3 PVC與CA膜過濾結果比較 87
第五章 結論與建議 89
5-1結論 89
5-2建議 90
引用文獻 91

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