臺灣博碩士論文加值系統

畜牧業所排放的廢水一直受到外界關注，其中養豬廢水具有高濃度有機物質與懸浮固體物，需經適當處理才能進行排放，以免造成環境污染。本研究利用高級氧化處理程序(advanced oxidation process, AOPs)中的大氣電漿(atmospheric plasma, AP)來去除養豬廢水有機污染物，藉由不同電漿參數(電漿功率、空氣流量、不同體積及COD/氨氮負荷)來探討養豬廢水有機污染物降解之影響，找出較佳的操作參數。四環黴素(Tetracycline, TC)，為新興汙染物的一種，常添加於動物飼料以提升抵抗力，因此常存在畜牧廢水中。藉由試驗中得到最佳條件於添加TC之養豬廢水及TC配製溶液中進行降解試驗，探討其電漿降解效能、有機物去除效率、反應參數。以螢光激發/放射光譜(EEM)、紫外光/可見分光光度計(UV-Visible)進行分析，利用液相層析質譜儀(LC-MS)及高效能液相層析儀(HPLC)分析中間產物及提出降解途徑。

研究結果顯示，以較佳的電漿操作條件(電漿功率(156 W)、空氣流量(5 L/min)、水樣體積(250 mL)及溫度(25°C))降解養豬廢水，有良好之COD及氨氮降解率。以電漿降解8小時，各批次養豬廢水之BOD去除率介於47~100%、TOC之去除率介於52~92%、COD去除率介於55~95%、氨氮去除率介於45~99%。大部分批次皆有測出亞硝酸鹽氮，其濃度先上升後降，而硝酸鹽氮濃度則持續上升。

TC配製溶液之降解效率及TOC去除率皆隨著時間增加而上升，於240分鐘後，TC濃度降至ND，但TOC無法完全去除。添加至不同養豬廢水中之TC降解率為81%~100%，而其TOC去除率為79%~92%、COD去除率為88%~91%、BOD去除率為59%~88%、氨氮去除率為80%~93%。在養豬廢水、TC配製溶液及添加TC至養豬廢水各水樣UV-vis分析中，各吸收峰強度隨電漿降解時間增加而先升後降或消失，唯獨TC配製溶液產生一個新的吸收峰，其強度隨電漿降解時間增加而增加。

在螢光特性分析中，各養豬廢水皆會於區域I (類酪氨酸)/區域Ⅱ(類色氨酸)及區域Ⅳ(可溶性微生物副產物)分別出現螢光峰，其強度皆隨電漿降解時間增加而變弱；TC配製溶液於跨區域Ⅲ(類富裡酸&黃腐酸)、區域Ⅳ(可溶性微生物副產物)及區域Ⅴ(類腐植酸)有一螢光峰，其強度會隨電漿降解時間增加而增強。TC經電漿降解產生質荷比(m/z) = 427、409、460、443、399、476、459、415、425、441、431、382、490、508、448、446、479、495、411、426、417(1)及417(2)之中間產物。

Livestock wastewater, including swine wastewater from animal husbandry has long been concerned for high organic and suspended solid pollutants which need to be properly treated before discharge to avoid environmental pollution. In this study, we investigated the feasibility of using an atmospheric plasma (AP) advanced oxidation process (AOP) to remove organic pollutants from swine wastewater. We explored the better operating condition of this process through testing various operating parameters (plasma power, air flowrate, water volume, and COD/NH3-N loading). Tetracycline (TC), one of environmental emerging contaminants and the most commonly used antibiotics to animal agriculture, is often found in livestock wastewater. Therefore, this study used the obtained better AP operating condition for the degradation of organic pollutants in swine wastewater and prepared solutions to explore the degradation efficiencies of organic pollutants and reaction kinetic parameters. Moreover, fluorescence excitation-emission matrix (EEM) and Ultraviolet-Visible (UV-Vis) tests were conducted to evaluate the plasma-degradation characteristics of water matrices during operations. Liquid chromatography-mass spectrometry (LC-MS), and high performance liquid chromatography (HPLC), analyses were performed to identify the intermediates (products) and pathways of TC plasma-degradation.



The results show that good COD and ammonium nitrogen degradation efficiencies of swine wastewater were achieved by using the better operating condition (plasma power (156 W), air flow (5 L/min), different volumes (250 mL), and temperature (25°C)). After plasma-degradation for 8 hours, the removal rates of TOC, COD, BOD, and NH3-N were 47%-100%, 52%-92%, 55%-95%, and 45%-99%, respectively. The concentration of nitrite nitrogen in most of the wastewater samples increased first and then decreased, while that of nitrate nitrogen increased with increasing operation time.

In the prepared solution, the TC degradation efficiency and TOC removal rate increased with the increase of plasma-degradation time. After 240 minutes, the concentration of TC decreased to ND, but that of TOC did not. The removal efficiencies of TOC, COD, BOD, and NH3-N were 79%-92%, 52%-92%, 40%-95%, and 45%-100%, respectively. The absorption peaks detected in UV-vis analysis for the swine wastewater samples with/without TC addition and prepared TC solution exhibited decreasing intensity and finally disappeared as the electrolysis time increased. Only the prepared TC solution had a new absorption peak and its intensity increased with increasing plasma-degradation time.

In fluorescence analysis, each swine wastewater showed fluorescence peaks in region I (tyrosine-like)/region II (tryptophan-like) and region IV (soluble microbial by-product), respectively, while the prepared TC solution had a fluorescence peak across the region III (fulvic acid-like), region IV (soluble microbial by-product), and region V (humic acid-like). However, the intensities of fluorescence peaks in swine wastewater decreased but that of TC prepared solution increased with the increase of operation time. The TC in prepared solution was degraded by plasma into the intermediates with m/z = 427, 409, 460, 443, 399, 476, 459, 415, 425, 441, 431, 382, 490, 508, 446, 479, 495, 411, 426, 417(1) and 417(2).

摘要 I

Abstract III

謝誌 V

目錄 VI

表目錄 X

圖目錄 XIII

第一章 前言 1

1.1 研究起緣 1

1.2 研究目的 2

第二章 文獻回顧 3

2.1 畜牧養殖的現況與概述 3

2.1.1 畜牧廢水之議題 4

2.2 新興汙染物概述(EC) 5

2.2.1 藥品與個人護理用品(PPCPs) 6

2.2.2 抗生素(Antibacterial) 8

2.2.2.1 環境中的抗生素 9

2.3 四環黴素(Tetracycline, TC) 10

2.4 大氣電漿(Atmospheric plasma, AP) 13

2.4.1 電漿活性水(Plasma activated water, PAW) 16

2.5 螢光激發/放射光譜(Excitation-Emission Matrix, EEM) 19

2.6 螢光區域整合法(Fluorescence regional integration, FRI) 19

2.7 紫外光可見光分光光譜儀(UV-Visible) 21

第三章 研究設備及方法 22

3.1 實驗設備與方法 22

3.1.1實驗藥品與材料 22

3.1.2儀器與設備 24

3.1.2.1總有機碳分析儀(TOC) 26

3.1.2.2多參數攜帶式比色計與重鉻酸鉀迴流法(COD) 27

3.1.2.3凱氏氮蒸餾器與氨氮離子分光光度計 28

3.1.2.4高效能液相層析儀(HPLC) 29

3.1.2.5紫外光/可見光分光光度計(UV-Visible) 31

3.1.2.6螢光分光光譜儀(EEM) 32

3.1.2.7液相層析質譜儀(LC-MS) 33

3.2 實驗規劃流程圖 35

3.3 實驗方法 36

3.3.1 養豬廢水基本水質分析 36

3.3.2 電漿降解養豬廢水之試驗 38

3.3.3 電漿降解TC之試驗 40

3.3.4 不同養豬廢水添加TC之電漿降解試驗 40

3.3.5 試驗結果計算 40

第四章 結果與討論 45

4.1 養豬廢水基本水質分析與電漿處理試驗條件 45

4.1.1 養豬廢水原水基本水質檢測結果 45

4.1.2養豬廢水經電漿降解試驗前後水質分析變化 47

4.2 養豬廢水之電漿降解試驗 50

4.2.1 電漿功率對養豬廢水降解之影響 50

4.2.1.1 不同電漿功率對養豬廢水電漿降解之比能耗 56

4.2.2 空氣流量對養豬廢水降解之影響 57

4.2.2.1 不同空氣流量對養豬廢水電漿降解之比能耗 62

4.2.3 不同體積對養豬廢水降解之影響 63

4.2.3.1不同體積對養豬廢水電漿降解之比能耗 68

4.3 不同有機物濃度養豬廢水之電漿降解試驗 69

4.3.1 不同有機物濃度對養豬廢水降解之影響 69

4.3.2 不同有機物濃度對養豬廢水電漿降解之比能耗 74

4.4 四環黴素之電漿降解試驗 75

4.4.1 四環黴素之電漿降解效率與結果 75

4.5 添加四環黴素於養豬廢水電漿降解試驗 77

4.5.1 添加四環黴素於養豬廢水電漿降解試驗結果 77

4.5.2 添加四環黴素於養豬廢水電漿降解之影響 78

4.6 各批次TOC、COD及氨氮去除率與反應速率常數k值比較 83

4.7 養豬廢水及四環黴素電漿降解之UV-vis變化探討 85

4.8 螢光特性分析 90

4.9 四環黴素電漿降解之中間產物探討 97

第五章 結論與建議 112

5.1 結論 112

5.2 建議 113

參考文獻 114

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