首页> 外文学位 >Modified Fenton's reagent: The use of complexed ferrous iron in the degradation of methyl tert-butyl ether (MTBE) in aqueous solutions and soil matrices.
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Modified Fenton's reagent: The use of complexed ferrous iron in the degradation of methyl tert-butyl ether (MTBE) in aqueous solutions and soil matrices.

机译:改良的Fenton试剂:在水溶液和土壤基质中使用复合亚铁降解甲基叔丁基醚(MTBE)。

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The degradation and kinetics of methyl tert-butyl ether (MTBE) by hydrogen peroxide at near-neutral pH were investigated using classical Fenton's reagent and a modified Fenton's reagent (ferrous iron chelated with ethylenediaminetetraacetic acid, EDTA). Dilute aqueous MTBE (100–400 μg/L) solutions were degraded in batch and continuously hydrogen peroxide-fed stirred-tank reactor (CFSTR) with Fe (II) and Fe(II)-EDTA present as a catalyst at constant pH. The modified Fenton's reagent significantly increased the degradation of MTBE (6.2–71%) in a batch reactor at near-neutral pH (5.5 to 7.5) when compared to classical Fenton's reagent (0.69–5.09%) under the same conditions. The modified Fenton's reagent extended the normal operating pH range for classical Fenton's reagent from 3–4 to 3–8.5. The reaction was more effectively controlled using the CFSTR. MTBE degradation of up to 99% in 60 minutes was achieved in the CFSTR with 0.17M hydrogen peroxide fed to the reactor at 40 mL/hr. A MTBE degradation mechanism by hydroxyl radicals is presented and rate constants were determined. The MTBE degradation rate constants were found to be pseudo-first order between pH 5.5 and 7.5 using Fe(II)-EDTA.; The degradation of MTBE in soil slurries (12.58 soil/L) was also investigated using Ottawa sand, Kaolin clay, and Na-Montmorillonite clay in CFSTR. Fe(II)-EDTA was present as a catalyst in 0.01M sodium bicarbonate buffer solution. MTBE degradation of up to 99% was achieved in the CFSTR in 60 minutes.; MTBE and degradation product concentrations were measured using a purge-and trap GC-FID method. Two major oxidation by-products were observed in the aqueous solution and soil slurries, tert-butyl formate and tret-butyl alcohol. Decomposition of hydrogen peroxide by Fe(II)-EDTA contributed to a decreased extent of MTBE removal, i.e., mole MTBE destroyed per mole of hydrogen peroxide consumed. The dissolved oxygen concentration increased significantly with time as the hydrogen peroxide decomposed.
机译:使用经典的Fenton试剂和改良的Fenton试剂(亚铁二胺四乙酸螯合的亚铁,EDTA)研究了pH值接近中性时过氧化氢对甲基叔丁基醚(MTBE)的降解和动力学。分批降解MTBE稀水溶液(100–400μg/ L),并在恒定pH值下,以过氧化氢为原料的搅拌釜反应器(CFSTR)连续搅拌,其中Fe(II)和Fe(II)-EDTA作为催化剂存在。与相同条件下的经典Fenton试剂(0.69–5.09%)相比,改良的Fenton试剂在分批反应器中在接近中性pH(5.5至7.5)时显着提高了MTBE的降解(6.2–71%)。改良的Fenton试剂将经典Fenton试剂的正常运行pH范围从3-4扩展到了3-8.5。使用CFSTR可以更有效地控制反应。在CFSTR中,以40 mL / hr的速度向反应器中加入0.17M的过氧化氢,可在60分钟内使MTBE降解高达99%。提出了由羟基自由基引起的MTBE降解机理,并确定了速率常数。使用Fe(II)-EDTA发现,MTBE降解速率常数在pH 5.5至7.5之间为伪一级。还使用CFSTR中的渥太华砂,高岭土和Na-蒙脱石粘土研究了土壤浆液中MTBE的降解(12.58土壤/ L)。 Fe(II)-EDTA作为催化剂存在于0.01M碳酸氢钠缓冲溶液中。 CFSTR在60分钟内达到了高达99%的MTBE降解。使用吹扫捕集GC-FID方法测量MTBE和降解产物浓度。在水溶液和土壤浆液中观察到两种主要的氧化副产物:甲酸叔丁酯和叔丁醇。 Fe(II)-EDTA分解过氧化氢有助于减少MTBE的去除程度,即每消耗一摩尔过氧化氢破坏的MTBE摩尔数。随着过氧化氢的分解,溶解氧的浓度随时间显着增加。

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