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研究生:石武航
研究生(外文):Wu-Hang Shin
論文名稱:活性碳吸附結合過硫酸鹽氧化三氯乙烯污染物之可行性評估
論文名稱(外文):Evaluation of matrices for activated carbon adsorption and persulfate oxidation of trichloroethylene
指導教授:梁振儒梁振儒引用關係
指導教授(外文):Chen-Ju Liang
學位類別:碩士
校院名稱:國立中興大學
系所名稱:環境工程學系所
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:2008
畢業學年度:96
語文別:中文
論文頁數:89
中文關鍵詞:現址化學氧化法過硫酸鹽活性碳三氯乙烯
外文關鍵詞:In situ chemical oxidationPersulfateActivated carbonTrichloethylene
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三氯乙烯(trichloroethylene,TCE)為國內工業上常使用之氯化有機溶劑,其易揮發且比水重非水相之特性,意外洩漏易進入深層土壤中,對土壤及地下水層形成長久之污染源。透水性反應牆(permeable reactive barriers, PRBs)為反應介質組成之屏障,目的為防止污染物隨地下水流而擴散。填充介質根據反應性分為不同型態。其中活性碳為廣泛使用之填充介質,藉由吸附作用濃縮水體之污染物。然而其吸附容量隨時間累積終達飽和,需置換填充材質。若能直接於地表下進行活性碳再生並降解脫附出之污染物,可減少開挖及處理吸附飽和活性碳之費用。現址化學氧化法(in situ chemical oxidation, ISCO)為不移動污染土壤或污染物將氧化劑導入地表下之整治技術。過硫酸鹽為應用於現址化學整治技術之氧化劑,可藉由熱及化學活化方式產生自由基降解污染物。因活性碳被證實可催化過氧化氫產生自由基,推論此反應亦適用過硫酸鹽,故本研究嘗試結合活性碳吸附與過硫酸鹽氧化能力處理TCE。
實驗結果顯示過硫酸鹽與活性碳反應,過硫酸鹽降解趨勢符合一階反應動力,且活性碳劑量為過硫酸鹽降解之影響因子。氧化劑接觸後之活性碳表面酸性官能基增加因而造成表面酸度上升、比表面積及等電位點降低等現象,並造成活性碳吸附能力下降。活性碳存在下過硫酸鹽氧化三氯乙烯實驗顯示於TCE與活性碳共存下過硫酸鹽降解減緩但仍遵循假一階反應動力,並由TCE隨時間固液相分布情形推論氧化反應發生於液相且有副產物之生成。過硫酸鹽再生活性碳造成吸附相之TCE脱附並可能產生TCE之降解,然而TCE之礦化程度相較於以亞鐵活化過硫酸鹽再生為不顯著,亞鐵活化再生機制則可同時氧化液相及固相污染物。
Chlorinated solvents such as trichloroethylene (TCE) have been widely used in industry. TCE is a dense non aqueous phase liquid and volatile organic compound. When TCE is accidently released in subsurface environment, the natural characteristics of TCE denotes that it could cause extensive groundwater contamination. Among a variety of subsurface remediation techniques, a permeable reactive barrier (PRB) is a permeable zone containing or creating a reactive treatment area oriented to intercept and remediate a contaminant plume. The reactive media such as activated carbon is commonly selected to absorb the pollutants from the groundwater. However, if the activated carbon reaches its adsorption capability, the PRB needs to be rebuilt with new materials or the carbon requires regeneration. Alternatively, in situ chemical oxidation (ISCO) is a remediation technology used to aggressively clean up contaminated area, mostly applicable to a highly concentrated contamination. The persulfate anion is an ISCO oxidant, which can be thermally or chemically activated to generate sulfate radicals for the destruction of organic contaminants. The objectives of this study were to evaluate the potential of the activated carbon PRB in conjunction with ISCO in treating TCE contamination.
The results reveal that persulfate degradation in the presence of activated carbon follows a pseudo-first-order degradation kinetic model and the quantity of carbons is a rate-limiting factor. The surface of activated carbon after contacting with persulfate exhibits significant changes including the increase of surface acidity, the decrease of specific surface area and pH of the point of zero charge and also the reduction of adsorption capacity. Furthermore, persulfate degradation in the presence of TCE and activated carbon appears even slower. The TCE degradation mainly occurred in aqueous phase in the persulfate/activated carbon system. Moreover, when persulfate and iron activated persulfate are used to regenerate activated carbon, the results demonstrate that persulfate oxidation can induce desorption of TCE from carbon surface while iron activated persulfate can simultaneously undergo desorption and oxidization of TCE.
中文摘要……………………………… Ⅰ
Abstract…………………………… Ⅱ
目錄…………………………………… Ⅳ
表目錄………………………………… Ⅶ
圖目錄………………………………… Ⅷ
第一章 緒論………………………… 1
1-1 研究緣起…………………… 1
1-2 研究目的…………………… 2
第二章 文獻回顧…………………… 3
2-1 三氯乙烯污染……………… 3
2-1-1 三氯乙烯之污染狀況……… 3
2-1-2 三氯乙烯物化特性、人體危害及管制標準…… 6
2-2 土壤及地下水整治技術………………………………… 8
2-2-1 現地化學氧化法…………………………………… 8
2-2-2 透水性反應牆…………………………………… 10
2-3 活性碳吸附結合化學氧化法………………………… 14
2-3-1 活性碳特性……………………………………… 14
2-3-2 活性碳再生……………………………………… 22
2-3-3 活性碳與氧化劑之結合應用……………………… 27
第三章 實驗材料與方法………………………………………… 29
3-1 實驗材料………………………………………………… 29
3-2 實驗流程………………………………………………… 31
3-2-1 活性碳對過硫酸鹽降解之影響實驗……………… 33
3-2-2 活性碳吸附動力實驗……………………………… 33
3-2-3 活性碳等溫吸附實驗…………………………………33
3-2-4 活性碳對過硫酸鹽氧化TCE之影響實驗…………… 33
3-2-5 活性碳再生實驗…………………………………… 34
3-3 實驗分析方法…………………………………………… 36
第四章 結果與討論……………………………………………… 43
4-1 活性碳對過硫酸鹽降解之影響………………………… 43
4-1-1 活性碳劑量影響…………………………………… 43
4-1-2 過硫酸鹽濃度影響………………………………… 45
4-2 氧化反應對活性碳表面特性影響……………………… 47
4-2-1 氧化處理前後活性碳表面官能基影響…………… 47
4-2-2 氧化前後活性碳表面結構及元素組成分析……… 49
4-2-3 活性碳氧化前後比表面積、等電位點及酸鹼度值 54
4-3 氧化反應前後活性碳吸附能力影響…………………… 57
4-3-1 活性碳吸附動力實驗……………………………… 57
4-3-2 活性碳吸附動力模式……………………………… 58
4-3-3 活性碳等溫吸附實驗……………………………… 62
4-4 活性碳對過硫酸鹽氧化TCE之影響……………………… 64
4-5 活性碳再生…………………………………………………………... 70
4-5-1 過硫酸鹽再生活性碳…………………………………70
4-5-2 亞鐵活化過硫酸鹽再生活性碳…………………… 73
4-5-3 再生活性碳表面特性分析………………………… 76
4-5-4 不同再生方法之比較…………………………………80
第五章 結論及建議……………………………………………… 82
5-1 結論……………………………………………………… 82
5-2 建議……………………………………………………… 83
第六章 參考文獻………………………………………………… 84
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