臺灣博碩士論文加值系統

聚丙烯腈人造纖維亦稱為壓克力棉，主要用做紡織布用紗等用途，每年的生產量至少16萬公噸以上。聚丙烯腈人造纖維製程廢水(Polyacrylonitrile，PAN)中含有高濃度的碳氮化合物，TKN/COD比值高達0.15-0.26，總凱氏氮中有機氮佔64%以上，顯示此廢水不僅含高比例氮化物，且以有機氮化物為主。為有效去除廢水中的有機物與氮化物，本研究係以高溫厭氧脫氨/中溫無氧脫硝/中溫好氧硝化三段式流體化床組合程序處理PAN人造纖維製程廢水，期能藉由第一段高溫厭氧脫氨反應槽將廢水中難分解的有機氮轉化，並同時將長鏈的大分子化合物裂解成小分子的有機碳，使第二段脫硝槽中微生物能利用有機碳與迴流之硝酸鹽進行脫硝反應，第三段硝化槽再將第一段厭氧槽裂解形成的氨氮轉化為硝酸鹽，再返送回脫硝槽進行脫硝反應產生氮氣，而達到有效去除有機物與氮化物的目的。
本研究利用批次試驗的方式，分別嘗試以高溫厭氧、中溫脫硝與中溫硝化個別程序處理PAN廢水。於高溫厭氧環境下，以PAN廢水為基質進行生物分解反應時，所得到的反應動力曲線符合抑制型Haldane模式，顯示高濃度PAN廢水對於高溫厭氧菌群具抑制作用。另一方面，於中溫無氧環境下，以脫硝菌分解PAN廢水，脫硝菌群所能利用的碳源有限，若依產氣速率的快慢，將PAN廢水中的COD分為三類，分別為是脫硝菌易分解的部分、可分解的部分與不易分解的部分，在COD的比例上，分別為27%、19%與54%。最後，以硝化菌直接分解PAN廢水的實驗結果顯示，硝化菌所能利用的有機物僅佔30%，且無法有效裂解有機氮；同時實驗結果亦證實高濃度PAN廢水對於硝化菌具有明顯的抑制作用，其所殘留的有機物會抑制硝化作用的進行。
於研究期間發現PAN廢水含有高濃度的硫酸鹽，因此採用選擇不同的策略研究硫酸鹽於對於高溫厭氧微生物的影響，結果發現在預先去除廢水中的硫酸鹽後，再添加蔗糖做為輔助基質時，可以得到最佳的有機氮裂解效果。
三段式生物程序處理PAN廢水的操作上；第一個試程由於廢水成分的變動性大，生物分解功能不穩定。因此於第二個試程中添加蔗糖做為輔助基質，結果顯示可以明顯的提升處理效果。第三個試程中則嘗試以兩段式脫硝/硝化程序處理PAN廢水，但處理效果則有限。因此於第四個試程中串連三反應槽，高溫厭氧脫氨反應槽經強化培養後，已能有效裂解有機氮，降低對後續程序的影響，而能穩定的提升處理效果，最終出流水COD與有機氮濃度分別為175 mg/L與13 mg N/L。另一方面，由生物活性的結果也可發現，第四個試程中的活性亦較高。
最後以分子生物技術針對高溫厭氧反應槽中降解PAN廢水菌群進行探討。由變性明膠電泳的結果顯示，在不同的體積負荷下，微生物族群的多樣性有明顯的變化；此外，應用螢光原位雜交技術，並配合共軛焦顯微鏡的觀察，可以發現高溫厭氧脫氨反應槽中，以α－Proteobacteria與δ－Proteobacteria的族群為主，亦含有high G+C content與可以產生氫氣的Clostridium等微生物。

This research investigated the process performance of three-stage bioreactors treating PAN wastewater with high-strength nitrogenous compounds. By the water quality analysis of the PAN manufacturing wastewater, high concentration of organic nitrogen were found and the TKN/COD ratios were achieved 0.15-0.26 that indicated the complicated characteristics in biodegradation for the PAN wastewater. In order to enhanced biodegradation of nitrogenous compounds in PAN wastewater, a combined three-stage process of thermophilic anaerobic / anoxic denitrification / aerobic nitrification fluidized beds was employed. In the three-stage process, nitrogenous compounds were effectively degraded in thermophilic anaerobic fluidized bed, and organic carbon was removed in the denitrification fluidized bed. In the other way, nitrifiers could oxide the residual organic nitrogen and ammonia to nitrate completely in the final stage of aerobic nitrification fluidized bed.
In the beginning, a series of batch study in PAN wastewater degraded by three individual process, which were thermophilic anaerobic, anoxic denitrification, and aerobic nitrification process. The biodegradation study clearly showed that high concentration of PAN wastewater would inhibit the thermophilic anaerobes, and the biokinetic in PAN wastewater obeyed to Haldane inhibition model. On the other hand, denitrifers could utilized limited organic carbon in PAN wastewater for denitrification, and according to nitrogen production profiles, in the total COD of PAN wastewater, 27% were easily degraded, 19% were degradable, and 54% were hard to be degraded. For nitrification, the result of biokinetic study showed that high strength organic compounds would inhibit the bioactivity of nitrifiers.
In order to effectively convert organic nitrogen into ammonia in thermophilic anaerobic situation, the pre-removed strategy of sulfate and sucrose-adding would increase the activity of thermophilic anaerobes.
By the process control for treating PAN wastewater, the operation was not stable in the first period due to the variation of wastewater, including concentration and components of wastewater. In the second period, the operation performance got better in three stage process for adding sucrose as co-substrates. PAN wastewater was treated by only two stage process (anoxic denitrification / aerobic nitrification) in the third period, PAN wastewater could not be effectively degraded. In the fourth period, the three-stage process was operated again. Because the thermophilic anaerobe were enhanced in degrading nitrogenous compounds, the operation became stable and better in treating PAN wastewater. The concentration of effluent in three-stage process of COD and organic nitrogen were 175 mg/L and 13 mg/L, respectively. By the way, the bioactivity test showed the better activities for denitrifiers and nitrifiers in the fourth period.
Finally, the microbial biology technology was applied to the microbial population in the thermophilic anaerobic reactor. From the result of DGGE, the diversity of PAN-degrading bacteria would change in different volume loading. The bacteria communities in the thermophilic anaerobic fluidized bed were studied by fluorescent in situ hybridization (FISH) and confocal laser scanning microscopy(CLSM). Alpha and delta－Proteobacteria dominated the bacteria population, and some high G+C content bacteria and Clostridium could be characterized in this system.

口試合格證書 I
中文摘要 II
英文摘要 IV
目錄 VI
表目錄 IX
圖目錄 XI
照片目錄 XV
第一章 前言 1
第二章 文獻回顧 5
2-1 PAN人造纖維製造流程 5
2-1-1 聚丙烯腈人造纖維種類及性質 5
2-1-2 聚丙烯腈人造纖維製造流程 6
2-2 氮的循環 10
2-2-1 自然界中氮的角色 10
2-2-2 固氮作用 10
2-2-3 氮的同化 12
2-2-4 氨化 12
2-2-5 硝化 12
2-2-6 厭氧氨氧化作用 13
2-2-7 硝酸鹽的還原 13
2-2-8 廢水處理中氮代謝機制的角色 16
2-3 脫硝作用 17
2-3-1 呼吸性脫硝 17
2-3-2 化學性脫硝 18
2-3-3好氧脫硝 18
2-3-4 影響脫硝的因素 20
2-4 硝化作用 25
2-4-1 自營性硝化作用 25
2-4-2異營性硝化作用 30
2-4-3影響硝化作用的參數 31
2-5 含氮污染物去除程序 36
2-5-1傳統生物厭氧硝化脫硝三段式組合程序 36
2-5-2 近十年新發展的生物脫硝硝化程序 40
2-6 厭氧作用 43
2-6-1 厭氧生物分解作用 43
2-6-2硫化氫的抑制作用 45
2-6-3 硫酸還原菌與甲烷生成菌之競爭關係 46
2-7 分子生物在生物程序中的應用 49
2-7-1 利用分子生物方法研究微生物 49
2-7-2 分子生物技術在生物處理程序上的應用 53
第三章 實驗設備與方法 56
3-1水質分析項目 56
3-1-1一般水質分析項目 56
3-1-2特殊水質分析 57
3-2生物活性與反應特性檢驗法 58
3-2-1批分式BOD瓶比攝氧速率實驗 58
3-2-2生化電解呼吸儀比攝氧速率實驗 59
3-2-3生化甲烷潛能試驗 61
3-2-4批分式血清瓶生化氮氣產能試驗 63
3-2-5氣泡式呼吸儀進行生化氮氣產能試驗 67
3-3三段式生物厭氧/脫硝/硝化流體化床 70
3-3-1高溫厭氧導流管式流體化床 70
3-3-2脫硝流體化床 71
3-3-3硝化導流管式流體化床 72
3-3-4三段式生物厭氧脫氨/無氧脫硝/好氧硝化組合程序 73
3-4固定生物膜生物質量之測定 74
3-5分子生物技術 76
3-5-1採樣 76
3-5-2 DNA萃取 76
3-5-3聚合酵素連鎖反應 78
3-5-4瓊脂膠體電泳 79
3-5-5微生物指紋譜之建立 80
3-5-6螢光原位雜交 81
3-6電子顯微鏡之生物菌相觀察 84
第四章 結果與討論 85
4-1聚丙烯腈人造纖維製程廢水水質特性分析 85
4-2聚丙烯腈廢水生物可分解性研究 87
4-2-1高溫厭氧系統處理聚丙烯腈廢水生物分解性研究 88
4-2-2無氧脫硝系統處理聚丙烯腈廢水生物分解性研究 93
4-2-3好氧硝化系統處理聚丙烯腈廢水生物分解性研究 98
4-3三段式流體化床連續流處理功能探討 101
4-3-1第一試程 廢水變異性對三段式處理功能之探討 104
4-3-2第二試程 外加蔗糖提升有機氮裂解率試程 116
4-3-3第三試程 兩段式組合程序處理聚丙烯腈廢水之可行性 128
4-3-4第四試程 三段式程序處理聚丙烯腈廢水 139
4-3-5各試程生物活性之探討 151
4-4高溫厭氧反應槽脫氨控制因子 163
4-4-1馴化後之高溫厭氧污泥處理聚丙烯腈廢水之生物分解性研究 163
4-4-2高溫厭氧污泥處理不含硫酸鹽之聚丙烯腈廢水之生物分解性研究 168
4-5高溫厭氧環境分解聚丙烯腈廢水微生物多樣性研究 172
4-5-1DNA萃取方法的比較 172
4-5-2高溫厭氧污泥族群複雜度分析 179
4-5-3應用螢光原位雜交技術評估高溫厭氧污泥族群分布狀況 182
4-6掃描式電子顯微鏡菌相觀察 186
第五章 結論與建議 196
5-1結論 196
5-2建議 198
參考文獻 199

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