臺灣博碩士論文加值系統

綜觀國內、外土壤污染事件發現其污染來源以事業廢水不當排放、有害廢棄物任意棄置及地下油管破裂或油槽鏽蝕老化為主，在這些土壤污染事件中普遍以油品污染較受矚目。針對油品污染場址的特性差異而有許多復育技術的運用，但在經濟及技術考量下，電動力法確實為可行性高的現地整治技術。本研究首先探討溫度、含水率及生物降解等環境因子對TPH-D(總石油碳氫化合物-柴油)及BTEX（苯、甲苯、乙苯及二甲苯合稱）在老埤系中削減影響，進而分析TPH-D及BTEX在老埤系中的移動性，最後探討在不同電極、電解液種類與濃度變化、土壤種類及腐植土添加量等配製中，TPH-D及BTEX經電動力法復育後削減變化。
結果顯示，當TPH-D及BTEX受到不同溫度及含水率影響，其削減率均是以含水(55%含水率)高於不含水(風乾土)，其中以40℃(55%含水率)為最高；另也發現，因試驗時間最長只有45天，BTEX受到生物降解作用並不顯著，但TPH-D在滅菌與否的比較中發現，其衰減率稍有差異，倘若能延長反應時間，生物應有時間及空間進行β-氧化反應，分解油品污染物。
在土壤管柱淋洗試驗中(未通電)，TPH-D受到溶解度影響其移動性皆比BTEX慢，不論是TPH-D或BTEX的移動性快慢依序為石英砂＞老埤系+石英砂 1:1 (w/w)＞老埤系＞老埤系+2.5wt%腐植土。通電後，TPH-D與BTEX皆有往陰極移動趨勢，其中以BTEX較顯著，其在陰極區的濃度以石英砂(以0.1M NaCl為電解液,2330 mg/kg)較高，而老埤系+2.5wt%腐植土(以蒸餾水為電解液,1017 mg/kg)較低。由此可證，土壤質地、電解液種類及溶解度等均是油品移動性的考量參數。
在電動力法復育受油品污染土壤方面，經電壓40Volts分別通電21及45天後，BTEX及TPH-D在老埤系中的削減率(含自然衰減率)皆可達90% (C/Co)以上，且削減率依序為鈦棒電極組(以0.1M NaCl為電解液)＞鐵網電極組(以0.1M NaCl為電解液)＞鈦棒電極組(以蒸餾水為電解液)＞鐵網電極組(以蒸餾水為電解液)；經與無觸媒效應的石墨棒電極對照組比較後發現，鈦棒及鐵網電極腐蝕產生的Ti(OH)4 (X-ray鑑定為TiO2水解後的產物) 及無定形鐵Feo (以Fe+2及Fe+3型態佔優勢) 確實可進行催化作用，提昇油品削減率。TPH-D及BTEX在供試土壤中皆較符合Freundlich 等溫吸附曲線，呈現多層吸附現象；當腐植土添加量漸增時，TPH-D及BTEX削減率會有隨之降低的趨勢，且不同腐植土添加量與油品的削減趨近線性關係，顯示有機質含量多寡確實為電動力法的重要影響因子。

Soils may be contaminated by petroleum-hydrocarbon via routes such as unseemly discharge of industrial wastewater﹑unsuitable disposal of hazardous wastes and spill from oil tank rustiness. Remediation technology selection must be depend on site specific. Electrokinetic technology (EK) is a feasible method for efficiently and economically remediate contaminated soil under certain circumstance. The objectives of study is to evaluate the reducing effects of TPH-D (Total Petroleum Hydrocarbon-Diesel) and BTEX (Benzene﹑Toluene﹑Ethylbenzene and Xylene) in Lao-Pi soil under different environmental conditions such as temperature﹑moisture contents and biodegradation. We also investigate the reducing variations after EK remediation using different electrodes﹑electrolytes﹑soil series and humic substance(HS) addition.
The results indicate that the reducing rate of TPH-D and BTEX which changed by temperature and moisture contents were as follows: 55% of moisture contents＞dry basis, and that in 40℃ (with 55% of moisture contents) had the highest rate. The biodegradation of BTEX was not noticed after 45 days. It was conjectured that the variations will increased with a longer test period.
In the soil washing experiments (nonelectrify), the mobility was influenced by solubility that make TPH-D moved slower than BTEX. The mobility of TPH-D or BTEX in different medium were all as follows: quartz sand ＞ Lao-Pi series and quartz sand (1:1,w/w)＞Lao-Pi series＞Lao-Pi series with2.5wt% HS. After electrifying, both TPH-D and BTEX had tendency to move to cathode, and BTEX moved faster than TPH-D. The concentration of BTEX on cathode in quartz sand (electrolytes were 0.1M NaCl, 2330mg/kg) was higher than in Lao-Pi series with2.5wt% HS (electrolytes were distilled water, 1017mg/kg). It demonstrated that the soil texture﹑electrolyte types﹑solubility and Koc were all need to be considered in petroleum mobility in soils.
After 21 and 45 days electrified under 40 volts , the reducing rate (C/C0) of TPH-D and BTEX in Lao-Pi series were both excess 90%, and the order of using electrode were as follows: Ti electrodes (electrolytes were 0.1M NaCl)＞iron net electrodes (electrolytes were 0.1M NaCl) ＞Ti electrodes (electrolytes were distilled water)＞iron net electrodes (electrolytes were distilled water). Comparing with Ti or iron net with graphite electrode that without catalyzer effect, we found that Ti(OH)4 (hydrolysate of TiO2 by X-ray identification) and Feo (Fe2+ and Fe3+ were dominant species) which were come from Ti and iron net electrodes corroded could catalysis and improve oil reducing rate. Due to the multiple-layer adsortion characteristics of TPH-D and BTEX on soil surface, the adsorption is fit for Freundlich isotherm. The TPH-D and BTEX reducing rate significantly decreased while increase in HS addition. Organic matter contents were proved to be the critical factor of EK efficiency.

目 錄
頁次
中文摘要 ..................................................................................... Ⅰ
英文摘要 ..................................................................................... Ⅲ
誌謝 ............................................................................................. Ⅴ
目錄 ............................................................................................. Ⅵ
表索引 ......................................................................................... XIII
圖索引 ......................................................................................... XV
第一章 前言 ..................................................................……..... 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 有機污染之特性及現況 ...................................................... 3
2.2 油品介紹 .............................................................................. 4
2.2.1 石油的成分 ....................................................................... 4
2.2.2 油品的分類 ....................................................................... 5
2.3 油品污染物的來源及宿命 .................................................. 9
2.4 油品污染物對環境的衝擊 .................................................. 11
2.4.1 油品污染物對空氣的影響 ............................................. 11
2.4.2 油品污染物對土壤的影響 ............................................. 11
2.4.3 油品污染物對水體的影響 ............................................. 11
2.5 油品污染場址的健康風險評估 ........................................ 13
2.6 污染指標 ............................................................................ 13
2.6.1 TPH-D .......................................................................….... 13
2.6.2 BTEX ................................................................................ 14
2.6.3 法令規範 ......................................................................... 16
2.7 土壤污染整治復育技術 .................................................... 17
2.7.1 土壤管柱清洗復育 ......................................................... 17
2.7.2 低溫熱脫附 ..................................................................... 18
2.7.3 土壤蒸氣萃取法 ............................................................. 18
2.7.4 臭氧氧化法 ..................................................................... 19
2.7.5 Fenton氧化法 ................................................................. 20
2.7.6 土壤生物復育技術 ......................................................... 20
2.8 電動力法復育技術介紹 .................................................... 21
2.8.1 電化學理論之應用 ........................................ 21
2.8.2 電動力法復育技術之演進 ............................................. 24
2.8.3 電動力法技術之應用 ..................................................... 25
2.8.4 電動力法復育技術原理及機制 ..................................... 26
2.8.5 電動力法復育技術之影響因子 ..................................... 30
2.8.6 電動力法復育技術相關參數簡介 ................................. 35
2.8.7 油品污染物通電後分解產物推估 ................................. 37
第三章 材料與方法 ................................................................. 38
3.1 試驗藥品 ............................................................................ 38
3.2 試驗設備 ............................................................................ 38
3.3 試驗材料 ............................................................................ 39
3.3.1 土壤樣品 ......................................................................... 39
3.3.2 油品種類 ......................................................................... 40
3.3.3 電解液種類 ..................................................................... 40
3.3.4 電極種類 ......................................................................... 40
3.3.5 觸媒種類 ......................................................................... 42
3.4 實驗流程 ............................................................................ 43
3.5 土樣基本性質分析 ............................................................ 44
3.6 油品污染土配製 ................................................................ 47
3.7 油品污染物檢量線配製 .................................................... 48
3.8 油品污染物定性分析 ........................................................ 48
3.9 吸附曲線分析試驗 ............................................................ 50
3.10 油品污染物自然衰減分析 …............................................ 50
3.11 實驗條件分析 ......……........................................…..…… 50
3.11.1 萃取液種類 ……........................................................... 50
3.11.2 萃取時間 ………........................................................... 51
3.11.3 改變溫度與含水率環境對油品衰減影響 ................... 51
3.11.4 生物降解對油品衰減影響 ………............................... 51
3.12 油品污染物移動性試驗 .................................................. 52
3.12.1 未通電前土壤管柱淋洗試驗 ....………....................... 52
3.12.2 通電後油品移動性分析 .....…….................................. 53
3.13 電動力法復育油品污染土壤試驗 .................................. 53
3.13.1 改變電解液種類及濃度對油品污染物削減影響 ..…. 53
3.13.2 改變電極種類對油品污染物削減影響 ....................... 53
3.13.3 改變土壤種類對油品污染物削減影響 ....................... 55
3.13.4 改變腐植土添加量對油品污染物削減影響................. 55
3.14 印證實驗 .......................................................................... 56
3.14.1 鈦棒腐蝕產物及高純度TiO2 X-ray鑑定分析 ............ 56
3.14.2 添加高純度觸媒對油品削減影響 ............................... 56
3.14.3 照光試驗 …................................................................... 57
3.15 氣相層析儀分析條件 ...................................................... 57
3.16 簡易試驗品質管制分析 .................................................. 58
3.17 油品削減率計算 .............................................................. 60
第四章 結果與討論 ................................................................. 62
4.1 土樣基本性質分析結果 .................................................... 62
4.2 等溫吸附曲線分析結果 .................................................... 65
4.3 油品污染物自然衰減分析結果 ........................................ 68
4.4 實驗條件分析結果 ............................................................ 69
4.4.1 萃取時間及溶劑種類 ..................................................... 69
4.4.2 改變溫度及含水率對油品衰減影響 ............................. 72
4.4.3 生物降解對油品衰減之影響 ......................................... 74
4.5 油品污染物移動性試驗 .................................................... 75
4.5.1 柴油TPH-D移動性試驗 ................................................. 75
4.5.2 九五無鉛汽油BTEX移動性試驗 .................................. 77
4.6 電動力法復育油品污染土壤試驗 …................................ 80
4.6.1 電動力法綜合參數分析 ................................................. 80
4.6.2 TPH-D ............................................................................... 90
4.6.2.1 電解液種類及濃度變化對TPH-D削減率影響........... 90
4.6.2.2 電極種類對TPH-D削減影響 ..................................... 90
4.6.2.3 改變土壤種類對TPH-D削減影響 ............................. 92
4.6.2.4 改變腐植土添加量對TPH-D削減影響 ...................... 93
4.6.3 BTEX ................................................................................ 96
4.6.3.1 電解液種類及濃度變化對BTEX削減影響 .............. 96
4.6.3.2 電極種類對BTEX削減影響 ...................................... 97
4.6.3.3 改變土壤種類對BTEX削減影響 ............………...... 99
4.6.3.4 改變腐植土濃度對BTEX削減影響 .......................... 100
4.6.4 電極腐蝕量與油品污染物削減關係 ............................. 102
4.6.4.1 電極-鈦棒 ..................................................................... 102
4.6.4.2 電極-鐵網 ..................................................................... 105
4.7 印證試驗 ............................................................................ 109
4.7.1 鈦棒腐蝕產物及高純度TiO2 X-ray 鑑定分析 ............. 109
4.7.2 通電後無定形鐵含量分析 ............................................. 110
4.7.3 添加高純度觸媒對TPH-D削減影響 ............................ 111
4.7.4 添加高純度觸媒對BTEX削減影響 ............................. 112
4.7.5 照光試驗 ......................................................................... 113
4.8 電力耗損 ............................................................................ 116
第五章 結論與建議 ...........................….................................. 118
參考文獻 ..................................................................................... 121
作者簡介 ..................................................................................... 134

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