電動力是近年來較受重視之土壤現地整治技術，利用重金屬污染物在電場中較具遷移性之特性，以電動力去除土壤中銅、鎘、鉻、砷、鉛、鈷、汞、鋅等重金屬，去除率可超過90%以上。雖然電動力整治技術已經在重金屬污染土壤現場被廣泛使用，但是複雜的重金屬傳輸反應及電化學現象並沒有被進一步了解。這些反應包括：離子擴散，離子交換、氧化還原、物理化學性吸附、礦化分解、鹽類沈澱及有機螯合等，因此，本研究之主要目的包括(1)研究銅吸附在土壤主要成分(Al2O3、SiO2)之微細結構及受其電場影響之移動性；(2)利用EXAFS(X射線吸收光譜之延伸區微細結構)研究重金屬在土壤中之結構及其涉及之物理化學反應；(3)電動力驅動之EDTA螯合污染土壤中銅之化學結構變化；(4)土壤中銅-腐植質(Cu-HS)之化學反應機制；及(5)進行電動力處理半導體製程中化學機械平坦化(chemical mechanical planarization)所產生(含微奈米銅)污泥之精細結構研究。另外，我們也進行去除發電廠所產生汞蒸氣污染之研究。
　　實驗結果顯示，以5V/cm之電場作用180分鐘後，分別有54%及27%之銅從SiO2和Al2O3表面移動到陰極，XANES光譜顯示，銅吸附在SiO2表面主要是以外層錯合物(outer-sphere complexes)型式存在，然而吸附在Al2O3表面之銅則以外層錯合物(inner-sphere complexes)型式居多。電動力驅動下，銅在SiO2表面移動性較高，因為銅以edge-sharing bidentate之型式與Al2O3鍵結(EXAFS光譜之結果)。
　　電動力處理含腐植質之銅污染土壤之研究，結果顯示土壤中銅之主要物種為50%之Cu-HS(銅-腐植質錯化物)、28%之CuCO3、11%之Cu2O及11%之CuO。FTIR光譜顯示，銅與腐植質可能是以unidentate complex型式存在。EXAFS數據顯示，距中心銅原子1.94 Å及2.17 Å處，分別有赤道向(equatorial)氧原子3.6個和軸向(axial)氧原子1.4個，經過180分鐘電動力反應，軸向Cu-O鍵距增加0.15 Å，推測可能是腐植質之羰酸基(carboxylic acid groups)與水分子產生配位交換(ligand exchange)反應，約50%之銅-腐植質錯化物從土壤中溶解至水相，71%之水相銅離子遷移至陰極。
　　加入0.01 M之EDTA於受銅污染土壤中可提高電動力去除效率約10%，主要是因為EDTA可將銅從土壤表面溶出形成水相Cu-EDTA錯化物，但受電場及陽極電解水所產生的酸影響，Cu-EDTA中之羰酸基(carboxylic acid groups)被水分子取代，而形成銅的水合物遷移至陰極。
　　以電動力方法也應用於回收半導體製程中化學機械平坦化所產生含奈米銅之污泥，實驗顯示之奈米CuO(14%)之移動性較其塊狀(bulk) CuO高，可能是奈米CuO活性較高，易溶於水，或是奈米銅受電場影響直接往陰極移動。
　　另外，在美國勞倫斯柏克萊實驗室中，我們以硝酸蒸氣及鹵素氣體來氧化氣態汞蒸氣污染物，結果顯示溴氣可有效氧化元素汞為二價汞，且形成之產物易溶於後續之氣體吸收塔而去除，初步經濟效益評估結果顯示，以溴氣來去除發電廠中產生之汞污染，是相當經濟且可行的(與傳統活性碳吸附法比較可節省經費約六到十七倍)。
　　本論文研究之主要成果包括：(1)銅吸附在Al2O3及SiO2表面之微細結構，尤其發現在電場作用下，銅在SiO2表面移動性較高；(2)在電場的影響下，銅-腐植質錯化物與水分子產生配位交換(ligand exchange)反應，使銅溶於水相，以銅的水合物遷移至陰極；(3)EDTA enhance電動力處理污染土壤之可能反應機制；(4)在電場作用下，奈米CuO與塊狀(bulk)CuO之移動性；及(5)針對發電廠所產生之汞蒸氣污染，提供一個新穎且經濟有效之方法。

　　Electrokinetic remediation (EKR) has been becoming one of the most feasible technologies for in-situ soil decontamination. However, the complex transport phenomena, electrochemistry and complexation reaction paths involved in the EKR is still not well understood. Thus, the main objective of this work was to study the speciation of copper in heavy copper contaminated soils during EKR by EXAFS, XANES, solid-state NMR (SSNMR), FTIR, electron paramagnetic resonance (EPR) and X-ray photoelectron spectroscopy (XPS). An in-situ EXAFS cell was used to reveal the possible reaction pathway during EKR. In addition, EKR of sludges was also conducted to extend the applications.
　　In simplified soil EKR systems (SiO2 or Al2O3), by XANES, it was found that the main copper species on SiO2 and Al2O3 were outer-sphere complexes (aqueous Cu(II)) (80%) and inner-sphere complexes (Cu/Al2O3) (59%), respectively. The mobility of copper in the Al2O3 matrix during EKR was less than that in the SiO2 system possibly because of the strong bonding between copper and Al2O3 surfaces with the edge-sharing bidentate mode (inner-sphere complexes). It was found that about 54% and 27% of Cu(II) on SiO2 and Al2O3, respectively were migrated to the cathode under the electric field (5 V/cm) for 180 min.
　　Speciation of copper-humic substances (HS) in the EKR of the contaminated soil was also studied by in-situ EXAFS and XANES spectroscopies. The least-square fits of the XANES spectra suggested that the main copper species in the contaminated soil were Cu-HS (50%), CuCO3 (28%), Cu2O (11%) and CuO (11%). By FTIR, Cu-HS as an unidentate complex was observed. The Cu-HS in the contaminated soil possessed equatorial and axial Cu-O bond distances of 1.94 and 2.17 Å with coordination numbers (CNs) of 3.6 and 1.4, respectively. In the EKR process, the axial Cu-O bond distance in the Cu-HS complexes was increased by 0.15 Å, which might be due to a ligand exchange of the Cu-HS with H2O molecules in the electrolyte. After 180 min of EKR, about 50% of the Cu-HS complexes (or 24% of total copper) 　　　ｉn the soil were dissolved and formed [Cu(H2O)6]2+ in the electrolyte and 71% (or 17% of total copper in the soil) of which were migrated to the cathode under the electric field (5 V/cm).
　　In the ethylenediaminetetraacetic acid (EDTA)-enhanced EKR of soils, the main copper species in the contaminated soil were CuCO3 (41%), CuO (40%) and adsorbed copper (Cu/SiO2) (19%). The fitted EXAFS data showed that the bond distance of Cu-(O)-Si was 3.25 Å with a coordination number (CN) of 1.0 in the second shells, suggesting a chemical interaction between copper and the soil surfaces. 　　In the presence of EDTA (0.05 M), a Cu-EDTA complex having the equatorial and axial Cu-O bond distances of 1.96 Å and 2.21 Å, respectively, was observed. The EPR spectra showed that copper (Cu(II)) was complexed with EDTA in a square-plannar arrangement with four oxygen-containing groups. Interestingly, after 180 min of EKR, the axial Cu-O bond distance was increased by 0.1 Å. The perturbation might be attributed to the possibility that the weak-field carboxylic acid groups of EDTA in the equatorial plane of Cu(II) were replaced by the strong-field water molecules.
　　In the EKR of a CMP sludge, the main copper species in the sludge were Cu(OH)2 (73%), nano CuO (14%) and CuO (13%). About 85% of the copper were dissolved (possibly formed [Cu(H2O)6]2+) in the electrolyte and 13% of which was migrated to the cathode under the electric field (5 V/cm) for 120 min. In addition, it was found that nano CuO has a higher mobility than its bulk CuO during EKR, which may be due to at least two possibilities: (1)nano copper has a higher dissolution rate; (2) nano CuO may be migrated directly to cathode.
　　An exploratory study for oxidation of gas-phase mercury by nitric acid vapor and halogen gas was also conducted. Arrhenius expression for the oxidation of gas phase mercury by bromine gas is 8.4×10-16 exp [-(554 ± 69)/T] cm3 molecule-1s-1, corresponding to a rate coefficient of (1.3 ± 0.3)×10-16 cm3 molecule-1s-1 at 294 K and an activation energy of 4.6 ± 0.6 kJ mol-1. The cost for 90% removal of mercury from a simulated flue gas of power plants by Br2 gas was estimated to about 5000$/lb, which is a cost-effective method compared to other technologies. In addition, the oxidation products and excess bromine gas are easy to handle since the oxidized form of mercury can subsequently be removed by the dissolution in an aqueous gas absorber or by the adsorption on sorbents in a baghouse or electrostatic precipitator.

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