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系統識別號 U0026-0407201815243200
論文名稱(中文) 利用螢光光譜方法分析飲用水水庫集水區溶解性有機物來源及特徵之研究
論文名稱(英文) Characterization and identification of dissolved organic matter sources in a drinking water reservoir using fluorescence spectroscopy methods
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 106
學期 2
出版年 107
研究生(中文) 王家緯
研究生(英文) Jia-Wei Wang
學號 p56051214
學位類別 碩士
語文別 英文
論文頁數 80頁
口試委員 指導教授-張智華
口試委員-葉宣顯
口試委員-陳 如
中文關鍵字 溶解性有機物  螢光激發/發散陣列  平均螢光強度  主成分分析  平行因子分析  相關性 
英文關鍵字 Dissolved Organic Matter  FEEM  AFI  PCA  PARAFAC  Correlation 
學科別分類
中文摘要 溶解性有機物質(DOM)在水體產生色度,味道和臭度,為生成消毒副產物的前驅物質,對人體健康產生危害,目前較多研究針對水處理廠各流程出流水進行檢測,此研究主要對於集水區飲用水水源DOM作特性分析,針對集水區上游旺萊溪及濁水溪進行DOM時間與空間分布調查,利用傳統水質分析指標溶解性有機碳、營養鹽、生化需氧量、濁度、及懸浮固體物,與本研究使用的螢光光譜分析方法作比較。由於傳統水質參數無法找出污染源,因此透過螢光激發/發散陣列(FEEM)分析方法,評估主要的溶解性螢光有機污染源分布。
阿公店水庫為一個多功能型水庫,將收集之原水經由路竹水處理廠處理,以提供高雄地區用水,除公共飲用水外,也涵蓋農業灌溉及路竹科學園區之工業用水,也具備防洪與清淤的操作條件,在每年九月中旬至隔年三月初,依水庫蓄容量多寡,實施越域引水,將旗山溪溪水經引水隧道流入旺萊溪。集水區內土地利用多屬果園及林地,作物以芭樂及棗子為主,為了有效提高產量,大量的有機肥料及化學肥料使用,土壤中有機污染物易隨雨水沖刷至水庫內。
本研究在2017年,三月至十月期間,共採集水樣七次,集水區內有七個採樣點與阿公店出流水,除了採集集水區內的水樣,為了瞭解水庫內之底泥是否會對水質造成明顯影響。在八月份採集底泥一次,藉由分析底泥釋出至水體的溶解性有機物特徵,對庫內水體的影響程度作探討,利用FEEM進行定量,及找出有機污染來源,其中FEEM為最主要的分析,定性使用主成分分析(PCA)方法,對具有相似螢光強度特性進行分類,可做初步螢光溶解性有機物來源特性判別,定量部分採用平均螢光強度(AFI)、平行因子(PARAFAC)分析,AFI是較簡單的分類方法,針對所劃分的區塊內螢光溶解性有機物之螢光強度取平均值,而PARAFAC分析利用MATLAB統計模擬方式,將螢光圖譜分解成獨立物種。最後針對定量的物種與傳統水質參數作Pearson相關性調查。

FEEM結果顯示,在無降雨情況下,且土地利用以果園為主區域以類黃酸(FA)有較強螢光訊號,其次為類腐植酸(HA),而人為有機污染物較低,在採樣前幾日具有效降雨的水樣則會測出更強的螢光強度,因為土壤內的有機肥料隨雨水流入河川。另外PCA定性,可明顯看出在非越域引水期間,螢光溶解性有機物特性主要受濁水溪影響;然而,在越域引水期間則是受到旺萊溪影響; PARAFAC分解及Tucker驗證結果顯示,集水區以類黃酸類與為主,次之為腐植酸類,及低螢光強度的溶解性微生物副產物,另外從水庫底泥DOM的螢光光譜圖中顯示出僅有微量溶解性螢光物質釋出,對於水庫出流水影響不大。
人為活動影響並非造成主要的螢光有機質來源,僅少數幾區人口密度較高的地方,有明顯人為訊號,因此如要針對水體螢光有機物作減量,應以農業施肥觀念為主,人為生活污水採用分流方式收集。以傳統水質搭配螢光光譜分析方法,能有效找出污染源。
英文摘要 Dissolved organic matters easily generate color, taste, and odor in waterbodies. These matters are also a precursor of disinfection by-products (DBPs) that are harmful to the human health. At present, more and more researchers devoted to detecting the outflow from various processes in water treatment plants. This study mainly analyzes the DOM of drinking water in the catchment, characterize the temporal and spatial distribution of DOM in Wang-Lai creek and Zhuo-Shui creek in the upstream catchment, and uses the conventional analysis of water quality parameters, such as non-purgeable dissolved organic carbon (NPDOC), nutrients, biochemical oxygen demand (BOD), turbidity and suspended solid (SS). Compared with the fluorescence spectroscopy method used mainly in this study, because conventional water quality parameters can’t find the pollution sources, fluorescence excitation/emission matrix (FEEM) analysis methods were used to evaluate the distribution of major fluorescent dissolved organic pollution sources.
A-Gong-Dian (AGD) reservoir is a multi-functional reservoir that raw water enters Lu-Zhu water treatment plant to supply water for Kaohsiung area. In addition to public drinking water, it also includes agricultural irrigation and industry in the Lu-Zhu Science Park. It also has the operating conditions for flood control and dredging, and implements water trans-basin diversion according to the reservoir capacity from around mid-September to the beginning of March every year to divert water from the Qi-Shan creek, through the tunnel flows into Wang-Lai creek. The land use in the catchment area is mostly orchard and forest. The crops are mainly guava and jujube. In order to enhance production, a large number of organic fertilizers and chemical fertilizers are used. These matters are easily flushed into the creek with rainwater and soil.
This study collected water samples 7 times from March to October in 2017, there are seven sampling points and the AGD outflow. In addition to collecting water samples in the catchment area, in order to understand whether the sediment in the reservoir has a significant effect on water quality. The sediment collected in August, through analyzed the dissolved organic matters characterization released from sediment, assess the degree of influence to the reservoir. Using FEEM quantification, and find out the fluorescent pollution source, FEEM is the major analysis method in this study. The fluorescence spectrum quality using principal component analysis (PCA) method, classified the similar fluorescence intensity characteristics, it can regard as preliminary discrimination, which may derive from the same pollution source. The quantitation adopts average fluorescence intensity (AFI) and parallel factor (PARAFAC). AFI is a simple classification method, the average of fluorescence organic matter intensity in the region. The PARAFAC analysis uses statistical modeling to decompose the fluorescence spectrum into an individual component. Finally, utilize the Pearson correlation between quantitative components and conventional water quality parameters.
The FEEM results showed that in the shortage of precipitation, and the land use of orchard-based area fulvic acid-like (FA) has a higher fluorescent intensity, followed by humic acid-like (HA), while the lower anthropogenic organic pollutants fluorescent intensity. Before sampling date, water samples with effective precipitation will measure higher fluorescence intensity. Because organic fertilizers in the soil flush into the river mixing with rainwater. In addition, through PCA qualitative analysis, it could be clearly observed that in the non-transbasin diversion, the fluorescent organic matter is mainly affected by the Zhuo-Shui creek, and in the transbasin diversion is affected by Wang-Lai creek. The PARAFAC decomposition and Tucker’s convergence coefficient validation results show that the water collection area is fulvic acid-like is dominated, followed by humic acid-like, and last is soluble microbial by-products (SMP).
The influence of anthropogenic activities is not the main source of fluorescent organic matter. Only a few areas where population density is high. Therefore, if we dedicated to reducing the amount of fluorescent organic matter in water bodies, we should adopt the concept of agricultural fertilization, and domestic sewage should be diverted. The conventional water quality combined with fluorescence spectroscopy analysis method can effectively identify the pollution source.
論文目次 CONTESTS
摘要 I
ABSTRACT III
致謝 VII
CONTESTS VIII
LIST OF TABLES XI
LIST OF FIGURES XII
CHAPTER 1 INTRODUCTION 1
1.1 Background 1
1.2 Research motivation 2
1.3 Research objective 3
1.4 Thesis structure 4
CHAPTER 2 LITERATURE REVIEW 5
2.1 What’s DOM 5
2.1.1 DOM sources 5
2.1.2 DOM characterization 5
2.1.3 The effect of coagulation 6
2.1.4 The effect of human health 7
2.1.5 Membrane fouling 8
2.2 DOM characterization methods 8
2.2.1 Dissolved organic carbon (DOC) 8
2.2.2 Ultraviolet visible (UV-Vis) absorbance 9
2.2.3 Specific UV- absorbance (SUVA) 9
2.2.4 Fluorescence Excitation Emission Matrix (F-EEM) 11
2.2.5 Principal Component Analysis (PCA) 13
2.2.6 Parallel Factor Analysis (PARAFAC) method 15
2.2.7 High Performance Size Exclusion Chromatography 16
2.3 Application of DOM characteristic in water quality management 17
2.3.1 River 17
2.3.2 Lake 18
2.3.3 Sediment 18
2.3.4 Marine 18
2.3.5 Water Treatment Plant (WTP) 19
2.3.6 Waste water treatment plant (WWTP) 19
2.4 Current status 20
CHAPTER 3 METHOLOGY 21
3.1 Study area 21
3.1.1 Location 21
3.1.2 Land use 25
3.1.3 Sampling frequency 29
3.2 Conventional analysis methods 30
3.2.1 Non-purgeable dissolved organic carbon (NPDOC) 30
3.2.2 UV-Visible and specific UV absorbance (SUVA) 30
3.3 Sediment released 31
3.4 Characteristic methods 34
3.4.1 Fluorescence EEM spectroscopy 34
3.4.2 Principal Component Analysis (PCA) 35
3.4.3 Parallel factor analysis (PARAFAC) modeling 35
CHAPTER 4 RESULTS AND DISCUSSION 39
4.1 Conventional water quality 39
4.2 The temporal and spatial distribution of DOM quality in reservoir and catchment 43
4.2.1 Spatial and temporal distribution of FEEM 43
4.3 Quantity the fluorescence intensity 47
4.3.1 Spatial distribution 47
4.3.2 Temporal distribution between non-transbasin diversion and transbasin diversion 50
4.4 Non-transbasin / Transbasin diversion comparison 53
4.5 Dimensional reduction of fluorescence spectrum 53
4.5.1 FEEM-PCA 54
4.5.2 FEEM-PARAFAC 56
4.6 Comparison of the compounds in non-transbasin and transbasin diversion 60
4.7 Reservoir released test 62
4.8 The correlation between human and agriculture sources 64
4.8.1 The correlation in the non-transbasin diversion period 64
4.8.2 The correlation in the transbasin diversion period 67
4.8.3 Summary 70
CHAPTER 5 CONCLUSIONS 71
5.1 Conclusions 71
5.2 Suggestions 72
CHAPTER 6 REFERENCES 73

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