EDDS螯合Fe(Ⅲ)活化过硫酸盐技术对TCE的降解效果

The Degradation Performance of Trichloroethylene by Means of Fe(Ⅲ)-EDDS Activated Persulfate Process

  • 摘要: 为解决传统Fe(Ⅱ)活化过硫酸盐过程中Fe有效性较低的问题,采用可生物降解的EDDS(乙二胺二琥珀酸)螯合Fe(Ⅲ)活化过硫酸盐处理水溶液中的TCE(三氯乙烯),考察c(过硫酸盐)、c〔Fe(Ⅲ)〕/c(EDDS)〔下称Fe(Ⅲ)/EDDS〕、溶液初始pH以及阴离子浓度对TCE降解效果的影响,并研究体系中产生的活性氧自由基. 结果表明:c(过硫酸盐)为15.0 mmol/L、Fe(Ⅲ)/EDDS为4时,60 min内TCE去除率达99.7%;提高c(过硫酸盐)、Fe(Ⅲ)/EDDS均有利于TCE降解,但超过一定限值后对TCE去除效果增强不明显;溶液初始pH(3~11)越高,TCE去除率越低;加入Cl-、HCO3-、SO42-和NO3- 4种阴离子均会抑制TCE降解,抑制程度表现为HCO3->Cl- >SO42->NO3-;自由基清扫试验证实体系中存在SO4-·、·OH和O2-·等3种活性氧自由基,·OH对TCE的降解起主导作用. 因此,EDDS螯合Fe(Ⅲ)活化过硫酸盐技术能够产生以·OH为主的活性氧自由基,从而快速高效去除水溶液中TCE,但降解过程受水质参数影响.

     

    Abstract: To improve iron availability in the traditional Fe(Ⅱ)-activated persulfate (PS) process, degradation performance of trichloroethylene (TCE) in a Fe(Ⅲ)-(S,S)-ethylenediamine-N,N'-disuccinic acid (EDDS) activated PS system was studied, and the generation of reactive oxygen species (ROS) was investigated by means of radical scavenger tests. The effects of various factors, including initial PS concentration, Fe(Ⅲ)/EDDS molar ratio, solution pH and common anions in groundwater (Cl-, HCO3-, SO42- and NO3-) were evaluated. When the initial PS concentration was 15.0 mmol/L and Fe(Ⅲ)/EDDS molar ratio was 4,9.7% of TCE was removed in 60 min. TCE removal was found to be enhanced with increase of PS concentration and Fe(Ⅲ)/EDDS molar ratio, but did not further increase when either PS concentration or Fe(Ⅲ)/EDDS molar ratio was overdosed. In addition, elevating the initial solution pH value (from pH 3 to 11) led to decreases in TCE removal rate. Cl-, HCO3-, SO42- and NO3- adversely affected TCE degradation performance, and the extent of inhibition followed the sequence:HCO3->Cl- >SO42->NO3-. Radical scavenger tests showed that SO4-·, ·OH and O2-· were all responsible for TCE degradation in the PS-Fe(Ⅲ)-EDDS system, and ·OH was the dominant radical. In conclusion, the Fe(Ⅲ)-EDDS activated PS process was effective for TCE removal in aqueous solution, while ·OH played a critical role in the system. However, TCE degradation performance was affected by the solution matrix, which could be encountered in real contaminated groundwater.

     

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