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研究生:郭庭瑜
研究生(外文):Ting-YuKuo
論文名稱:以四氧化三鐵奈米顆粒降解電子產業排放廢水中溴化戴奧辛及多溴聯苯醚之研究
論文名稱(外文):Utilizing Fe3O4 Nanoparticles to DecomposePBDD/Fs and PBDEs in the Wastewater Effluents from Electronic Industry
指導教授:林達昌
指導教授(外文):Ta-Chang Lin
學位類別:碩士
校院名稱:國立成功大學
系所名稱:環境工程學系碩博士班
學門:工程學門
學類:環境工程學類
論文種類:學術論文
論文出版年:2013
畢業學年度:101
語文別:英文
論文頁數:84
中文關鍵詞:多溴聯苯醚四氧化三鐵溴化戴奧辛電子產業廢水
外文關鍵詞:PBDEsPBDD/FsFe3O4 nanoparticleselectronic industrywastewater.
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本研究自行合成四氧化三鐵奈米顆粒並進行降解電子產業廢水中多溴聯苯醚(PBDEs)及溴化戴奧辛(PBDD/Fs)毒性之評估。藉由SEM、ESEM-EDS、TEM與XRD特性分析可證明所合成的為奈米級Fe3O4其粒徑約在20 nm,顆粒呈圓球狀且因本身磁性而發生團聚現象。Fe3O4其比表面積平均值為73.86 m2/g,孔隙體積則為0.25 ml/g。使用奈米級Fe3O4降解電子產業廢水中PBDEs及PBDD/Fs濃度,隨著使用劑量濃度增加(~12.5 g/L),其去除率亦逐漸上升,24 hr後去除率分別為88.0 %及89.6 %。將二者反應狀況其線性化後所得反應速率常數kobs最高各達0.074 hr-1及0.083 hr-1,半衰期各為2.4 hr及1.0 hr。劑量濃度增加也促使其反應速率常數逐漸上升,而比表面積反應速率常數kSA下降。此外,若PBDD/Fs以毒性當量濃度計算,其使用較低之Fe3O4劑量濃度(2.5 g/L與5.0 g/L)無法使毒量當量濃度降低。但若使用較高之劑量(12.5g/L),則較能確保毒性當量濃度能與質量濃度一致,隨時間有下降之趨勢,其反應速率常數Kobs為0.069 hr-1。在奈米級Fe3O4回收試驗結果中,汙泥模擬組與清水對照組經兩次回收質量回收率平均值可提高至94.7 %與99.7%,奈米級Fe3O4顆粒可經由外加磁場固液分離,大幅提高實廠應用之可行性。
This study utilized Fe3O4 nanoparticles to degrade polybrominated dibenzo-p-dioxins/dibenzofurans(PBDD/Fs) and polybrominated diphenyl ethers(PBDEs) in the effluents from electronic industry. The SEM, ESEM-EDS,TEM and XRD analysis showed that the synthesized Fe3O4 nanoparticles are spherical with particle size about 20 nm, however, are aggregated due to its magnetic characteristics. In addition, the mean specific surface area of the Fe3O4 nanoparticles is 73.86 m2/g, and the corresponding pore volume is 0.25 ml/g. The removal efficiencies of PBDEs and PBDD/Fs in the effluent from wastewater treatment plants by Fe3O4 nanoparticles gradually increased with the increase of the dose concentration (~12.5 g/L), and reached 88.0 % and 89.6 %, respectively, after 24 hr.
In this study, pseudo-first-order kinetics are used to describe the degradation of PBDEs and PBDD/Fs in the effluents from wastewater treatment plants by Fe3O4 nanoparticles. The pseudo-first-order rate constant (Kobs) for PBDEs and PBDD/Fs gradually increased with the increase of the dose concentration (~12.5 g/L), and reached 0.074 hr-1 and 0.083 hr-1, respectively, while the corresponding surface-area-normalized rate coefficient (kSA) decreased with the increase of the dose concentration. For PBDD/Fs, the TEQ concentration in the effluent could raise, if the dose concentration of Fe3O4 nanoparticles was lower (2.5 g/L and 5.0 g/L). However, a higher dose concentration (12.5 g/L) still ensured the decline of both the PBDD/F mass and TEQ concentration. Its Kobs was 0.069 hr-1, and the half-life was 6.2 hr.
Recovery tests of Fe3O4 nanoparticles aim to evaluate the recovery rate of Fe3O4 nanoparticles by applying an external magnetic field in effluent wastewater sample. The result showed that the mean Fe3O4 nanoparticles recovery rates in effluent wastewater sample and control sample (the deion water) could reach 94.6% and 99.7%, respectively, revealing the feasibility of Fe3O4 nanoparticles on treating wastewater from electronic industry.

Contents
摘要 I
Abstract II
誌謝 IV
Contents 1
List of tables 3
List of figures 4
Chapter 1 Introduction 6
Chapter 2 Literature Review 8
2.1 Introduction of PBDEs and PBDD/Fs 8
2.1-1 Physical and chemical properties of PBDEs 8
2.1-2 Potential formation for PBDD/PBDF 12
2.1-3 Life cycle of PBDEs 14
2.1-4 Demand and usage 16
2.1-5 Toxicity in environment 17
2.1-6 Industrial pollution 18
2.2 Introduction of Fe3O4 19
2.3 Synthesis of Fe3O4 22
2.4 Application of Fe3O4 in environment assignment 24
2.5 Fe3O4 kinetic mechanism 26
Chapter 3 Experiment methods 29
3.1 Objectives and study framework 29
3.2 Materials 31
3.3 Preparation of Magnetic Nanomaterials 32
3.4 Characterization of Fe3O4 33
3.4-1 Morphology 33
3.4-2 XRD 35
3.4-3 BET (Brunauer-Emmett-Teuller) surface area 37
3.5 Recovery test 38
3.6 Batch experiments for debromination of PBDD/Fs and PBDEs 40
3.7 Kinetic analysis 41
3.8 Analyses of PBDEs and PBDD/Fs 43
Chapter 4 Results and discussion 45
4.1 The characteristics of Fe3O4 Nanoparticle 45
4.1-1The morphologic analysis 45
4.1-2 ESEM-EDS analysis 48
4.1-3 X-Ray Diffraction (XRD) 50
4.1-4 BET 52
4.2 Recovery efficiency of Fe3O4 nanoparticles with the external magnetic field 53
4.3 Degradation of PBDD/Fs and PBDEs in the effluents from wastewater treatment plants of electronic industry by using Fe3O4 nanoparticles 54
4.3-1 Degradation of PBDE concentration 54
4.3-2 Degradation of PBDD/F concentration 58
4.4 Kinetic analysis of the degradation of PBDD/Fs and PBDEs in the effluents from wastewater treatments of electronic industry by Fe3O4 nanoparticle 66
4.4-1 PBDEs Kinetic analysis 67
4.4-2 PBDD/Fs Kinetic analysis 70
4.4-3 PBDD/F TEQ kinetic analysis 73
Chapter 5 Conclusions and Suggestions 76
References 78

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