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系統識別號 U0026-0812200915245510
論文名稱(中文) 前氧化及鈣離子對UF膜處理含藻原水阻塞影響之研究
論文名稱(英文) The effect of preoxidation and calcium ion on UF membrane fouling when treating algae suspensions
校院名稱 成功大學
系所名稱(中) 環境工程學系碩博士班
系所名稱(英) Department of Environmental Engineering
學年度 97
學期 2
出版年 98
研究生(中文) 王婉綺
研究生(英文) Woan-chi Wang
學號 p5696119
學位類別 碩士
語文別 中文
論文頁數 113頁
口試委員 口試委員-楊金鐘
口試委員-林財富
口試委員-吳哲宏
指導教授-葉宣顯
中文關鍵字 EPS  薄膜阻塞  臨界通量  鈣離子  前氧化 
英文關鍵字 membrane fouling  EPS  preoxidation  critical flux  calcium ion 
學科別分類
中文摘要 薄膜程序對優養化原水中所含之藻類有良好之去除率,但藻體細胞及其所分泌胞外物質(extracellular polymeric substance, EPS),與水中背景物質相互作用所造成之阻塞(fouling),為薄膜程序發展之一大瓶頸。前氧化,如加氯,常用以控制薄膜之生物阻塞(biofouling),但亦可能刺激藻體分泌更多之胞外物質,而造成有機阻塞。
本研究選擇藍綠菌(Microcystis aeruginosa)及綠藻(Chodatella sp.)為試驗對象,在實驗室經純種培養後,配製為仿優養化原水之含藻懸浮液,並以高錳酸鉀及臭氧進行前氧化,同時添加鈣離子,再以UF膜(材質regenerated cellulose, MWCO 10 kDa)過濾之,比較不同變因下薄膜阻塞現象。而為了不使藻體細胞在經前氧化後破裂,有釋出胞內物質之虞,本研究另以流式細胞儀搭配FDA及SYTOX兩種螢光染劑,觀察藻體在不同劑量前氧化劑下之受損情形,並依據流式細胞儀之偵測結果決定前氧化劑量。在選擇適當劑量後,分別以未經氧化及經不同前氧化劑氧化之M. aeruginosa及Chodatella sp.懸浮液及其Soluble EPS,以UF膜進行階段性改變壓力試驗,觀察臨界通量(critical flux)變化,並選擇適當壓力作為後續固定壓力試驗之依據。而固定壓力實驗則用以觀察不同鈣離子濃度及不同前氧化劑對含藻懸浮液過膜之阻塞現象變化。
流式細胞儀實驗結果顯示,兩種藻對高錳酸鉀的抵抗能力皆較臭氧強,而M. aeruginosa對臭氧的抵抗能力較Chodatella sp.佳,應係因M. aeruginosa胞外黏質層較厚之故。而由UF膜過濾實驗可知,兩種藻之Soluble EPS幾乎不會造成薄膜阻塞,藻體累積於薄膜表面所形成的濾餅層才是造成通量下降的主要原因。未氧化之M. aeruginosa懸浮液可造成相當嚴重之阻塞,而 Chodatella sp.僅造成輕微阻塞。兩種藻在經高錳酸鉀氧化後,M. aeruginosa 因凝聚形成膠羽而使通量下降較未氧化者減緩,Chodatella sp.則因分泌出膠狀EPS而造成通量之下降較未氧化者明顯。若系統中含有鈣離子,則兩種藻在經高錳酸鉀氧化後,皆可形成較大膠羽,M. aeruginosa懸浮液之通量幾乎無下降現象,而Chodatella sp.之通量下降較無鈣離子濃度者低,但通量仍低於未氧化者。此外,兩種藻在經臭氧氧化後,僅M. aeruginosa懸浮液之藻體表面電位受到改變,其界達電位絕對值在經臭氧氧化後減小,但即使藻體穩定性改變,在不同鈣離子含量之系統中,對於通量的改變則沒有太大影響。
由ATR-FTIR分析藻體表面官能基,可知兩種藻皆有蛋白質及多醣體、羧基等成分。而在經高錳酸鉀及臭氧氧化後,兩種藻皆有胺基酸中C-N鍵之波峰產生,顯示在氧化劑確實可改變藻體之表面性質,此變化可能為藻體表面之某種蛋白質成分在經氧化劑氧化後的改變或分泌出的。應與Chodatella sp.懸浮液經高錳酸鉀氧化後所分泌出之膠狀EPS有所關聯。
英文摘要 Membrane processes have high removal efficiency for algal cells that contained in the eutrophic source water. However, the fouling problem caused by both algal cells and the extracellular polymeric substances (EPS) that interact with the background materials in water is the major obstruct to the further development of membrane processes. Preoxidations, such as adding chlorine, are used to control the biofouling of membrane. However, it may also stimulate algae to secret more EPS and cause organic fouling.
In this study, two algal species, namely Microcystis aeruginosa and Chodatella sp., were chosen as the target species. The algal cells, harvested from axenic cultures in the lab, were used to prepare synthetic algae suspensions. Different amount of calcium ion were also added to simulate the hardness in various eutrophic source waters. The major objective of this research is to study the effect of preoxidation by either potassium permanganate or ozone on the fouling phenomena of the subsequent UF membrane (regenerated cellulose, MWCO 10 kDa) filtration of the synthetic algae suspensions. In order to avoid damaging algal cells and releasing intracellular substances, the flow cytometry technique with FDA and SYTOX fluorescent dye were used to determine the appropriate preoxidants dosage. Then the original and the preoxidized synthetic algal suspensions were filtered through UF membrane separately. In order to estimate the critical flux, stepwise increase in the transmembrane pressure (TMP) was conducted, maintaining each TMP for 30 min, and the corresponding permeate flux were recorded. The same UF membrane filtrations were also conducted for the solution containing only soluble EPS.
The results from flow cytometry show that ozone caused cell damage at much lower dosage than that of potassium permanganate. However, M. aeruginosa has more resistance to ozone than Chodatella sp., probably due to the thicker extracellular mucilage layer of the former. The results from UF membrane filtration experiments show that the solution, contained only soluble EPS, caused almost no flux decline. When algae cell suspensions were filtered through UF membrane, the flux decline was mainly caused by the cake layer which consisted of algae cells deposited on membrane surface. The original M. aeruginosa suspension caused much serious fouling than that of Chodatella sp. After preoxidation by potassium permanganate, the flux decline of M. aeruginosa suspension though UF membrane was minor than that without preoxidation, as permanganate oxidation caused some algal cell aggregation. However, permanganate preoxidation caused more serious flux decline for Chodatella sp. suspension compared to that without preoxidation. This probably was due to the release of gelatinous EPS by the Chodatella sp. after permanganate oxidation. With the addition of calcium ion into the algae suspension, the floc formation after permanganate preoxidation for both algae species was further promoted, and flux decline rate reduced. This is speculated to be due to the bridging effect of Ca2+ ion between negatively charged algal cell surface and MnO2 (s), the reduced product of potassium permanganate. For preozonation, as it did not alter the floc size distribution, its effect on flux decline was also insignificant.
As far as the functional groups of algae cell surface are concerned, the ATR-FTIR spectrums reveal that these two algae have components of protein, polysaccharides, and carboxyl group … etc. With preoxidation with either permanganate or ozone, there were some alternations of the cell surface, such as the formation of C-N bound peak of amino acid. This may indicate the change or release of protein components after preoxidation, and may be related to the release of gelatinous EPS after Chodatella sp. was preoxidized by permanganate.
論文目次 摘要 I
Abstract III
誌謝 VI
目錄 VII
表目錄 X
圖目錄 XI
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 優養化對淨水程序之影響 3
2-2 薄膜程序 4
2-2-1 薄膜種類及過濾機制 4
2-2-2 薄膜材質 6
2-2-3 薄膜模組 8
2-2-4 過濾方式及流動狀態 8
2-3 UF膜之簡介與應用 10
2-4 薄膜積垢與濃度極化 13
2-4-1 薄膜積垢(Membrane fouling) 13
2-4-2 濃度極化(Concentration polarization) 16
2-5 臨界通量 17
2-5-1 臨界通量(Critical flux) 17
2-6 藻類胞外聚合物質 19
2-6-1 藻類胞外物(Extracellular polymeric substances, EPS) 19
2-6-2 EPS對薄膜阻塞之影響 21
2-7 前氧化劑 22
2-7-1 前氧化劑之作用 22
2-7-2 高錳酸鉀(Potassium permanganate, KMnO4) 23
2-7-3 臭氧(Ozone, O3) 24
2-8 鈣離子對薄膜阻塞之影響 25
2-9 流式細胞儀 27
2-9-1 染劑之應用(FDA及SYTOX) 27
2-9-2 流式細胞儀 28
第三章 實驗材料與方法 30
3-1 實驗流程規劃 30
3-2 含藻懸浮液配製 32
3-2-1 藻類純種培養 32
3-2-2 人工藻液之製備 35
3-2-3 Soluble EPS之製備 35
3-2-4 藻類計數 35
3-3 氧化試驗 39
3-3-1 臭氧試驗 39
3-3-2 高錳酸鉀 41
3-3-3 二氧化錳製備 42
3-4 一般水質分析 43
3-4-1 導電度(Conductivity) 43
3-4-2 pH值 43
3-4-3 粒徑分析 43
3-4-4 界達電位(Zeta potential) 44
3-4-5 膠羽之觀察 45
3-5 薄膜試驗 46
3-5-1 薄膜試驗裝置 46
3-6 流式細胞儀 48
3-7 藻體表面官能基分析 49
第四章 結果與討論 50
4-1 氧化劑量之決定 50
4-1-1 染色時間測試 50
4-1-2 人工藻液經氧化後之細胞完整性觀察 53
4-2 臨界通量試驗 58
4-3 固定壓力試驗 72
4-4 不同鈣離子濃度對薄膜阻塞之影響 88
4-5 以人工製備MnO2取代KMnO4 之比較 91
4-6 藻體表面官能基 97
第五章 結論與建議 102
5-1 結論 102
5-2 建議 104
參考文獻 105
附錄 112
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