博碩士論文 88346005 詳細資訊




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姓名 陳錫金(Hsi-Jien Chen)  查詢紙本館藏   畢業系所 環境工程研究所
論文名稱 界面活性劑Octylphenol Polyethoxylates生物降解與復育之研究
(Study on Biodegradation and Bioremediation of Surfactant Octylphenol Polyethoxylates)
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摘要(中) 烷基苯酚聚氧乙烯醇類(Alkylphenol polyethoxylates, APEOn)化合物常用於做為界面活性劑和清潔劑,其種類包括壬基苯酚聚氧乙烯醇(Nonylphenol polyethoxylates, NPEOn)和辛基苯酚聚氧乙烯醇(Octylphenol polyethoxylate, OPEOn),APEOn生物降解代謝產物包括壬基苯酚(Nonylphenol, NP)和辛基苯酚(Octylphenol, OP)及其帶有一單位氧乙烯醇的代謝物如Nonylphenol mono-ethoxylate (NPEO1)和Octylphenol mono-ethoxylate (OPEO1)被推論具有生物荷爾蒙性質,此代謝物在環境中當濃度到達一定程度時,就足以對野生動物和人類之內分泌功能造成干擾作用,且此類物質之毒性及難分解性較未分解前之界面活性劑為高,因此,世界許多國家已將APEOn類化合物列為管制使用之對象。由於OPEOn之烷基結構較為簡單,且OP之雌激素效應為NP之10至20倍,因此,本研究以OPEOn為對象,用以評估OPEOn及其代謝產物之生物復育效果,五株從土壤和底泥篩出之OPEOn分解菌中,以30℃,200 rpm恆溫振盪之斜面培養,以OPEOn為唯一碳源,進行五菌株水溶液中生長和OPEOn生物降解效率之評估。土壤縮模(Microcosm)則被用以模擬生物復育程序以評估生物復育之效果,三株外添加菌Pseudomonas nitroreducens TX1、Pseudomonas putida TX2和Pseudomonas sp. OP2亦被添加於土壤中以降解OPEOn及其代謝產物。研究結果顯示,五株環境中所篩出之OPEOn分解菌中,菌株E獲得最大比生長率0.56 h-1和95% OPEOn初級降解效果,菌株A比其他四菌株更能於高OPEOn濃度中生存。對五菌株而言,在5,000 mg/L OPEOn-MSB medium中,1,200 mg/L至1,600 mg/L之(NH4)2SO4濃度,為較適切之氮源使用量,pH 7則為最適之生長環境條件,關於OPEOn及OP之生物復育方面,OPEOn及其代謝產物確實可經由添加外添加菌和土壤原生菌之作用而降解,在91天的實驗操作中,有98%以上的OPEOn達成初級分解,約75%之OP在縮模土壤生物復育過程中降解。直接添加菌株Pseudomonas sp. OP2,可於70天的實驗操作中,提高約25%之OP降解效果。OPEOn土壤中降解路徑分析則找到三種新的代謝產物,包括octylcatechol,butylphenol Polyethoxylates (1 to 3 ethoxylate unit)和phenol。微生物菌相分析顯示菌株Brucellaceae bacterium, Stenotrophomonas maltophilia and Aeromonas hydropila在土壤中之優勢表現,而外添加菌株TX1,TX2及OP2皆能在添加之後,成為縮模土壤中之優勢菌種。本研究證實OPEOn及其代謝產物透過外添加菌添加之生物復育程序為一可行之方法。
摘要(英) Alkylphenol polyethoxylates (APEOn) including nonylphenol polyethoxylates (NPEOn) and octylphenol polyethoxylates (OPEOn) were used very commonly in surfactants and detergents. The biodegradation metabolites of APEOn including nonylphenol (NP), octylphenol (OP), nonylphenol mono-ethoxylate (NPEO1) and octylphenol mono-ethoxylate (OPEO1) are supposed to imitate the natural hormones. The levels of these metabolites present in the environment may be sufficient to disrupt endocrine function in wildlife and humans. These compounds are more toxic and resistant to biological degradation than the parental surfactants. Therefore, the use of APEOn has been limited in many countries. Since the simpler structure of the alkyl group than NPEOn, and the OP obtain10 to 20 fold higher of the estrogenic effect than NP, the OPEOn was dealing with this study to be the target compound for the evaluation of OPEOn and its metabolites bioremediation efficiency. Five strain of OPEOn degrader which isolated from soil and sediments were evaluated in the aquatic medium using OPEOn as the sole carbon source at 30℃, 200 rpm shaking culture. The microcosms assimilated the bioremediation were employed for the evaluation of OPEOn and OP bioremediation efficiency. The exogenous strains of Pseudomonas nitroreducens TX1, Pseudomonas putida TX2, and Pseudomonas sp. OP2 were also utilized to biodegraded OPEOn and metabolites in the soil. The results of this study showed, for five strains of OPEOn degrader, strain E obtained the maximum specific growth rate of 0.46 h-1 and degradation efficiency of 95% for OPEOn primary biodegradation. Strain A can be sustained in the highest OPEOn concentration than the other four strains. The nitrogen source of (NH4)2SO4 with the concentration of 1,200 to 1,600 mg/L and pH 7 were also the feasible growth condition for the five strains in 5,000 mg/L OPEOn-MSB medium. Regarding to the bioremediation of OPEOn and OP, the exogenous degrader and soil indigenous microorganisms approved the OPEOn and metabolites biodegradation in the soil. In 91 days bioremediation period, over 98% of OPEOn and 75% of OP have been degraded in the soil. By the OP directly bioremediation process, around 25 % OP could be degraded in the soil in 70 days bioremediation period by the addition of the exogenous Pseudomonas sp. OP2. The analyzed of OPEOn biodegradation pathway in the soil was also conducted and three novel intermediates including octylcatechol, butylphenol polyethoxylates with 1-3 ethoxylate unit, and phenol had been found. The analysis of bacterial community in the soil was shown the predominant strains of Brucellaceae bacterium, Stenotrophomonas maltophilia and Aeromonas hydropila in the soil. Additionally, all three exogenous bacteria of strain TX1, TX2, and OP2 were also predominant in the soil. The bioremediation of OPEOn and its metabolites by the exogenous strains were therefore noted in this research.
關鍵字(中) ★ 界面活性劑
★ 土壤縮模
★ 辛基苯酚
★ 辛基苯酚聚氧乙烯醇
★ 生物復育
★ 生物降解
關鍵字(英) ★ Biodegradation
★ Bioremediation
★ Surfactant
★ Microcosm
★ Octylphenol Polyethoxylates
★ Octylphenol
論文目次 摘要 I
ABSTRACT II
目錄 III
圖目錄 VIII
表目錄 XIV
第一章 前言 1
1.1研究緣起 1
1.2研究之重要性 3
1.3 研究目的與架構 5
第二章 文獻回顧 9
2.1 界面活性劑之定義,分類,性質與使用 9
2.2 界面活性劑之性質 13
2.3 界面活性劑對環境之影響 16
2.4非離子性界面活性劑對環境所造成之污染 17
2.5非離子性界面活性劑之生物分解 18
2.6 烷基苯酚聚氧乙烯醇類界面活性劑(APEOn)之來源與特性 22
2.6.1 APEOn之種類,分布與特性 22
2.6.2 APEOn代謝產物之生成、流佈與環境特性 22
2.6.3 APEOn代謝產物之環境荷爾蒙效應 28
2.6.4 APEOn分解菌 34
2.6.5 APEOn之微生物分解機制 37
2.7 生物復育 .44
2.7.1土壤環境因子對生物復育之影響 .45
2.7.2環境因子對生物分解作用之影響 .51
2.7.3生物復育技術與環境因子控制相關研究現況 54
2.8 土壤縮模設計 59
2.9 本章總結 .59
第三章 材料與方法 .62
3.1 研究流程 .62
3.2 研究材料 64
3.2.1界面活性劑 .64
3.2.2 MSB (Minimal Salts Basal medium). 64
3.2.3菌種來源與特性 .67
3.2.4土壤來源與特性 .73
3.2.5本研究所使用之化學藥品 75
3.2.6本研究所使用之儀器設備 76
3.3 實驗規畫 77
3.3.1 菌株水溶液中生長與特性分析 .77
3.3.2 OPEOn水溶液中分解特性分析 .77
3.3.3 水溶液中菌株生長與OPEOn分解動力分析 78
3.3.4 不同土壤含水率條件下微生物分解OPEOn批次實驗 78
3.3.5 土壤縮模中OPEOn生物復育分析 79
3.3.6 土壤縮模中OPEOn理論礦化量分析 82
3.3.7 土壤縮模中OPEOn生物分解代謝路徑分析 .86
3.3.8 土壤縮模中OPEOn及OP生物復育特性分析 86
3.3.9 土壤縮模中OP生物分解菌相分析 89
3.4 分析方法 .89
3.4.1 水溶液中OPEOn萃取方法 89
3.4.2 水溶液中OPEOn 及其代謝產物濃度之HPLC分析方法 89
3.4.3 水溶液中微生物量OD600分析方法 .90
3.4.4 水溶液中OPEOn中間代謝物LC/MS分析方法 .90
3.4.5 土壤中OPEOn,OP及其可能之代謝產物之萃取 .91
3.4.6 土壤中微生物菌量分析方法 .91
3.4.7 微生物與土壤表面SEM分析方法 .92
3.4.8 數據處理與分析 92
第四章 水溶液中OPEOn之生物降解 .93
4.1 OPEOn分解菌之生長條件分析 93
4.1.1 起始濃度對OPEOn分解菌生長之影響 .93
4.1.2 氮源對OPEOn分解菌生長之影響 97
4.1.3 pH對OPEOn分解菌生長之影響 101
4.1.4 外添加H2O2 .104
4.1.5 OPEOn分解菌生長動力分析 108
4.2水溶液中OPEOn之降解 .111
4.2.1起始濃度對OPEOn降解之影響 111
4.2.2氮源對OPEOn降解之影響 114
4.2.3 pH對OPEOn降解之影響 118
4.3 水溶液中OPEOn生物分解路徑分析 .120
4.4 本章總結 126
第五章 土壤縮模中OPEOn生物復育特性分析 127
5.1 土壤含水率對OPEOn生物復育效果之影響 .127
5.2 土壤中OPEOn之生物復育評估 128
5.2.1 土壤通氣對OPEOn生物降解之影響 .129
5.2.2 溫度對OPEOn生物降解之影響 131
5.2.3 外添加菌對OPEOn生物降解之影響 134
5.2.4 不同OPEOn起始濃度對OPEOn生物復育之影響 .142
5.2.5 不同外添加菌量對OPEOn生物復育之影響 146
5.2.6 不同外添加菌對OPEOn生物復育之影響 151
5.3 土壤中OP之累積 157
5.3.1 土壤縮模曝氣對OP累積之影響 .157
5.3.2 土壤縮模溫度對OP累積之影響 .158
5.3.3 土壤縮模中不同微生物組成對OP累積之影響 160
5.3.4 土壤縮模中不同外添加菌對OP累積之影響 .164
5.4 土壤中OP之生物復育效果之評估 166
5.4.1 不同OPEOn分解菌對OP生物復育影響 166
5.4.2不同OP分解菌對OP生物復育影響 170
5.5 土壤縮模中OPEOn 及OP生物復育之菌相變化 .179
5.6 土壤原生菌OPEOn生物降解路徑之探討 187
5.7 本章總結 199
第六章 結論與建議 .201
6.1 結論 ..201
6.2 建議 ..203
參考文獻 205
附錄一 226
附錄二 227
附錄三 228
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指導教授 曾迪華、黃雪莉
(Dyi-Hwa Tseng、Shir-Ly Huang)
審核日期 2005-1-27
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