過硫酸鹽(Persulfate)高級氧化為近年來現地化學氧化法(ISCO)常用的方法，經由催化反應後會產生自由基破壞污染物結構，對許多有機物均有良好的去除能力。在實際應用中，地下水環境中的氯鹽會影響過硫酸鹽的氧化效果，其具體影響為何目前仍有很大的爭議。為了探討氯離子對過硫酸鹽氧化的影響，本研究利用自由基平衡模式及酸性環境下過硫酸鹽氧化p-CBA的反應計算硫酸根自由基(SO4-.)生成速率，建立受氯鹽干擾下過硫酸鹽氧化動力模式及氯鹽影響判斷模式，針對該模式以五種探針化合物(甲醇、乙醇、酚、乙醯苯胺、酸橙7)進行驗證，並分析對實際目標污染物甲基第三丁基醚(MTBE)的處理效果。
研究中列出氯鹽在過硫酸鹽氧化系統中主要的自由基反應式，並以各反應式速率常數值建立系統中自由基生成預測模式，並根據探針物質的氧化反應動力求得各種物質的k_(p〖SO〗_4^(-.) )及k_(p〖Cl〗_2^(-.) )，由此k值可建立氧化反應預測模式，並從反應動力的比值可建立氯鹽影響比值(φ)，透過該比值比較可推斷氯鹽對過硫酸鹽氧化系統的影響為促進或抑制。
由自由基生成預測結果可得知不同氯離子濃度在系統中自由基生成量，不存在氯鹽的氧化系統的SO4-.濃度為1.61×10-11M，氯鹽存在時Cl2-.的濃度為2.8~3.2×10-10M，顯示系統中Cl2-.為主要自由基物種；由實驗結果可得到，甲醇、乙醇的去除效率受到氯離子的影響而抑制，於反應30分鐘內最多減少40%左右的去除效率，其他物質較無法看出受氯鹽的影響程度，於30分鐘內皆可達到95%以上的去除率，與動力預測模式比較，可發現整體的相對誤差皆小於30%，證明該預測模式應用於受氯鹽影響的系統時有良好的準確性。由影響模式中甲醇、乙醇、乙醯苯胺φ值均小於1，代表氯鹽作用於系統中將造成抑制作用，可呼應氧化實驗結果隨著氯離子的劑量增加則降解受到抑制20~40%不等；酸橙7φ值大於1，對應實驗結果在反應10分鐘內透過氯離子作用將增加20%的去除效率。MTBE的氧化系統中，由影響模式φ值大於1可判斷MTBE為受到添加氯離子而加強去除效率的物質，但φ值相當接近1較難判斷看出結果差異性，比較氧化實驗與動力預測其誤差為14%，顯示模式可以合理預測MTBE的氧化反應。一般而言，該預測模式應用於多種污染物受氯離子作用所造成之影響預測具有高度的準確性，可發展應用於其他實際污染物的影響預測。

Persulfate is an emerging oxidant used in in-situ chemical oxidation(ISCO) for soil and groundwater remediation. The chemical can be activated with different methods to generate sulfate radical(SO4-.) and hydroxyl radical(OH.), leading to the oxidation of many organic contaminants present in groundwater. Although persulfate has become one of the important ISCO oxidant, the effect of chloride, a common co-existing anion in many groundwater systems in Taiwan, on the production of the radicals remained unclear. In this study, effect of chloride on the production of radicals in a UV assisted persulfate system is studied. A probe compound, p-CBA, was first employed to measure the formation rate constant of SO4-.. Based on the rate constants, a kinetic model considering the impact of chloride was built. The model was verified with five probe compounds including phenol, methanol, ethanol, acetanilide and acid orange 7, and then employed to the prediction of the degradation rate of MTBE.
Based on the chain reaction of radicals in persulfate/chloride system, a model was established to estimate the formation of two major radicals under steady state. Then rate models for the oxidation of probe compounds and targeted organic compounds may be estimated from appropriate reaction rate constants. To quantify the impact of chloride on the reaction rate, chloride impact factor(φ) representing the rate with chloride relative to that without chloride in the system, was calculated.
Based on the experimental results obtained, the concentration of sulfate radical in the UV/persulfate system was 1.61×10-11M in chloride free system. With the presence of chloride of 1-100mM, dichlorine radical is the dominant radical, with 2.8-3.2×10-10M in the system. Chloride may slow the degradation rates of methanol and ethanol by 40%, while for other probe compounds, no effect on the rates were observed. The rate models were able to describe the experimental data, with mostly less than 30% of relative errors, indicating that the models are reasonable. When applying the models for MTBE, the models predicted degradation of MTBE very well, with only 14% of error. It may be concluded the radical-based rate model described all the experimental data reasonably well and may be used in the systems with other contaminants.

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