State Environmental Protection Key Laboratory of Environmental Risk Assessment and Control on Chemical Process, East China University of Science and Technology, Shanghai, 200237, China.
Environmental Engineering and Science Program, Department of Biomedical, Chemical and Environmental Engineering (DBCEE), College of Engineering and Applied Science, University of Cincinnati, Cincinnati, OH, 45221-0012, USA.
Environ Sci Pollut Res Int. 2018 Jun;25(16):15733-15742. doi: 10.1007/s11356-018-1708-9. Epub 2018 Mar 25.
This study presents a performance comparison of Fe(II)-catalyzed sodium percarbonate (SPC), Fe(II)-EDDS-catalyzed SPC, and of the innovative hydroxylamine hydrochloride (HA)-Fe(II)-EDDS-catalyzed SPC for the degradation of trichloroethylene (TCE) in water. TCE degradation was greater in the Fe(II)-EDDS-catalyzed SPC system compared to the Fe(II)-catalyzed SPC system, indicating the effectiveness of adding EDDS as an enhancement factor for the removal of TCE. Moreover, TCE degradation was faster in the HA-Fe(II)-EDDS-catalyzed SPC system compared to the Fe(II)-EDDS-catalyzed SPC system, illustrating that HA can play a synergistic role in TCE degradation. Analysis of iron distribution in the three systems demonstrated that EDDS addition maintained iron in soluble form, and that the generation of soluble ferrous from ferric iron was expedited with addition of HA. Studies using nitrobenzene and carbon tetrachloride probes provided insights on the generation of hydroxyl radical (HO) and superoxide anion radical (O) in the three systems. A gradual increasing contribution of O to TCE removal in Fe(II)-catalyzed SPC, Fe(II)-EDDS-catalyzed SPC, and HA-Fe(II)-EDDS-catalyzed SPC systems was verified through free-radical scavenger tests. Finally, monitoring of Cl concentrations manifested the complete dechlorination of TCE. A possible mechanism of TCE degradation involving two pathways of HO oxidation and O reaction was proposed.
本研究对 Fe(II)催化过碳酸钠(SPC)、Fe(II)-EDDS 催化过碳酸钠和创新的盐酸羟胺(HA)-Fe(II)-EDDS 催化过碳酸钠降解水中三氯乙烯(TCE)的性能进行了比较。Fe(II)-EDDS 催化过碳酸钠体系中 TCE 的降解大于 Fe(II)催化过碳酸钠体系,表明添加 EDDS 作为增强因子去除 TCE 的有效性。此外,HA-Fe(II)-EDDS 催化过碳酸钠体系中 TCE 的降解速度快于 Fe(II)-EDDS 催化过碳酸钠体系,表明 HA 可以在 TCE 降解中发挥协同作用。对三种体系中铁分布的分析表明,EDDS 的添加使铁保持可溶形式,而添加 HA 则加速了高铁向可溶性亚铁的生成。使用硝基苯和四氯化碳探针的研究提供了关于三种体系中羟基自由基(HO)和超氧阴离子自由基(O)生成的见解。通过自由基清除剂试验验证了 Fe(II)催化过碳酸钠、Fe(II)-EDDS 催化过碳酸钠和 HA-Fe(II)-EDDS 催化过碳酸钠体系中 O 对 TCE 去除的贡献逐渐增加。Cl 浓度的监测表明 TCE 完全脱氯。提出了一种涉及 HO 氧化和 O 反应两种途径的 TCE 降解可能机制。