不同土壤/水系統下酵素對PAHs分解作用之影響

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劉庚樺(Keng-Hua Liu) 查詢紙本館藏

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論文名稱

不同土壤/水系統下酵素對PAHs分解作用之影響
(Effects of enzyme biodegrade PAHs in different soil-water systems)

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摘要(中)

多環芳香烴化合物因在環境中自行分解不易，為提升其去除效率，將界面活性劑淋洗與生物復育同時進行，其會因許多因子影響造成不同之結果。本實驗選用鈣蒙特石，及Triton X-100與Brij 35兩種界面活性劑，利用laccase來分解含不同界面活性劑水/土系統中之naphthalene與phenanthrene，目的在探討多環芳香烴化合物，在不同界面活性劑—水—土壤系統的傳輸行為對生物分解的影響。
實驗結果顯示水溶液系統中，laccase在含Triton X-100與Brij 35之溶液中皆會促進PAHs的分解作用，又因微胞比單體為更有效之分佈介質，使得含微胞相時的溶液能促使生物分解速率加快。另外由於Brij 35碳氫鏈較Triton X-100碳氫鏈長許多，形成之微胞結構較大，造成較大的立體結構障礙，故含1.5CMC Triton X-100溶液對PAHs分解率大於Brij 35。土壤/水系統中兩種界面活性劑仍具促進分解作用，且酵素可直接利用溶於水溶性微胞與吸附性微胞之PAHs，使得當平衡溶液為1.5CMC時分解速率大於0.5CMC。分別比較土相與水相之分解情形，因PAHs與酵素在水相之質傳速率大於土相，使得分解行為在水相中較明顯。將酵素固定在鈣蒙特石上，分解在不同界面活性劑溶液的PAHs結果顯示，Triton X-100有促進分解作用，但Brij 35卻有抑制分解之現象，推測原因為固定化後之酵素在Brij 35系統下產生構型改變，故抑制酵素對PAHs之分解。

摘要(英)

The hydrophobicity of polycyclic aromatic hydrocarbon compounds (PAHs) results in these compounds being strongly sorbed to soils. The use of surfactants may change the sorption behavior of PAHs in soil environment. Biodegradation is believed an important pathway for removal of PAHs contamination from soil-water systems. The aim of this study was to evaluate the degradation capability of fungal laccase in degrading PAHs including naphthalene and phenanthrene contained in soil-water systems with nonionic surfactants. The nonionic surfactants selected were Triton X-100 and Brij 35. A comparative study was carried out by application of free and immobilized laccases in the soil-water system.
In aqueous, addition of Triton X-100 and Brij 35 resulted in enhancement the biodegradation of PAHs. When micelles existed in water systems, PAHs biodegradation was greater than that of below critical micelle concentration (CMC). The same results were also found in soil-water systems. The phenomena can be ascribed to more PAHs partition on into micelles than that of monomers. This situation leading to bioavailable on micellar phase is more effective. To compare the biodegradation rate in difference phase, the results show that in aqueous phase was higher than that of soil phase. On immobilized laccase systems, an inhibition biodegradation in the presence of Brij 35 was observed, and an opposite effect presented in the presence of Triton X-100. Differences phenomenon in bioavailability may correlate with steric hindrance of immobilized laccase and longer polyoxyethylene chain of Brij 35.

關鍵字(中)

★ 界面活性劑
★ PAHs
★ 酵素
★ 固定化

關鍵字(英)

★ immobilized
★ enzyme
★ PAHs
★ surfactants

論文目次

目次頁次
目錄………………………………………………………………….. Ⅰ
圖目錄……………………………………………………………….. Ⅳ
表目錄……………………………………………………………….. Ⅵ
第一章前言
1-1 研究緣起…………………………………………………… 1
1-2 研究目的與內容…………………………………………… 3
第二章文獻回顧
2-1 多環芳香烴化合物(PAHs)………………………………… 4
2-1-1 定義及來源………………………………………...... 4
2-1-2 特性…………………………………………………... 4
2-1-3 毒性…………………………………………………... 5
2-1-4 污染現況……………………………………………... 5
2-2 非離子界面活性劑………………………………………… 7
2-2-1 界面活性劑之定義與種類…………………………... 7
2-2-2 性質…………………………………………………... 7
2-2-3 界面活性劑在污染防治的應用……………………... 9
2-3 酵素………………………………………………………… 9
2-3-1 特性與種類…………………………………………... 9
2-3-2 固定化酵素…………………………………………... 11
2-4 PAHs於水/土系統之傳輸行為……………………………. 16
2-5 非離子界面活性劑於水/土系統傳輸行為………………... 17
2-6 非離子界面活性劑於水/土系統對PAHs之作用………… 18
2-7 PAHs於水/土系統之生物分解……………………………. 20
2-7-1 PAHs之生物分解……………………………………. 20
2-7-2 生物分解PAHs之代謝途徑………………………… 22
2-7-3 酵素於PAHs生物分解過程扮演之角色…………… 25
2-8 PAHs於水-土-界面活性劑系統之生物分解……………… 29
第三章實驗內容與材料
3-1 實驗內容…………………………………………………… 31
3-2 實驗方法…………………………………………………… 33
3-2-1不同水相系統中free laccase對PAHs之分解……….. 33
3-2-1-1 水相系統酵素活性分析………………………… 33
3-2-1-2 水相系統free laccase對PAHs之分解………… 33
3-2-2 水-土系統中free laccase對PAHs之分解………….. 34
3-2-2-1 水-土系統酵素活性分析……………………….. 34
3-2-2-2 水-土系統free laccase對PAHs之分解……….. 36
3-2-3 固定化酵素系統之PAHs分解……………………… 39
3-2-4 lacccase對界面活性劑之分解實驗…………………. 39
3-3 實驗設備…………………………………………………… 41
3-3-1 電子天平……………………………………………... 41
3-3-2 水平震盪器…………………………………………... 41
3-3-3 高速離心機…………………………………………... 41
3-3-4 氣相層析儀-火焰離子化偵測器……………………. 41
3-3-5 積分儀………………………………………………... 42
3-3-6 分光光度計…………………………………………... 42
3-3-7 高效能液相層析儀…………………………………... 42
3-3-8 均質機(pellet pestle)…………………………………. 42
3-3-9 總有機碳分析儀……………………………………... 43
3-3-10 溶氧度計……………………………………………. 43
3-4 實驗材料…………………………………………………… 43
3-4-1 土壤…………………………………………………... 43
3-4-2 非離子界面活性劑…………………………………... 44
3-4-3 多環芳香烴化合物…………………………………... 45
3-4-4 酵素…………………………………………………... 46
3-4-5 萃取溶液……………………………………………... 46
3-4-6 其他溶液……………………………………………... 48
第四章結果與討論
4-1 實驗相關基質與操作條件測試…………………………… 50
4-1-1 PAHs於水相系統回收率……………………………. 50
4-1-2 PAHs於土壤-界面活性劑-水系統回收率………….. 51
4-1-3 乳化現象…...………………………………………… 52
4-1-4 活性測試…...………………………………………… 53
4-1-5 laccase對界面活性劑之分解…...…………………… 55
4-2 不同水相中free laccase對PAHs之分解…………………. 57
4-2-1 laccase在含Triton X-100溶液中對PAHs之分解作用…………………………………………………… 57
4-2-2 laccase在含Brij 35溶液中對PAHs之分解作用….. 60
4-2-3 比較PAHs在不同界面活性劑系統之生物有效性… 62
4-3 不同水—土相系統中free laccase對PAHs之分解………. 66
4-3-1 水/土--Triton X-100系統中laccase於對PAHs之分解…………………………………………………….. 66
4-3-2 laccase於水/土--Brij 35系統下之對PAHs之作用… 70
4-3-3 比較PAHs於不同水--土--界面活性劑系統中之分解…………………………………………………….. 74
4-4 固定化酵素之PAHs分解………………………………….. 76
4-4-1 Triton X-100系統中酵素固定化對PAHs之分解…... 76
4-4-2 Brij 35系統中酵素固定化對PAHs之分解………... 80
4-4-3 固定化酵素於不同系統下對PAHs分解之比較…… 84
4-4-4 自由態酵素與固定化酵素對分解PAHs之影響……. 86
第五章結論與建議
5-1 結論………………………………………………………… 88
5-2 建議………………………………………………………… 89
參考文獻…………………………………………………………….. 91

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指導教授

李俊福(Jiunn-Fwu Lee)

審核日期

2003-7-11

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