李亚男,王乐心,杨帆,张国凯,饶竹,张继红,陈梦洁,冯卓.Fe(VI)/Fenton联合体系氧化降解菲的路径及机理[J].环境科学学报,2021,41(8):3175-3184
Fe(VI)/Fenton联合体系氧化降解菲的路径及机理
- Degradation pathway and mechanisms of phenanthrene by a combined system of Fe(VI) and Fenton
- 基金项目：山西省基础研究计划项目（No.201801D121267）；自然资源部生态地球化学重点实验室开放基金（No.ZSDHJJ201804）；山西省2019年度研究生教育改革研究课题项目
- 李亚男
- 太原理工大学环境科学与工程学院, 晋中 030600
- 王乐心
- 太原理工大学环境科学与工程学院, 晋中 030600
- 杨帆
- 太原理工大学环境科学与工程学院, 晋中 030600
- 张国凯
- 中海国亚环保工程有限公司, 太原 030006
- 张继红
- 太原理工大学环境科学与工程学院, 晋中 030600
- 陈梦洁
- 太原理工大学环境科学与工程学院, 晋中 030600
- 冯卓
- 太原理工大学环境科学与工程学院, 晋中 030600
- 摘要：Fe（VI）/Fenton联合体系降解多环芳烃的效果良好，但其机理及降解路径仍需进一步被探究.采用荧光及GC-MS技术，考察弱酸条件下Fe（VI）降解菲的效果，并对比中性及碱性条件研究其氧化机理，进而分析Fe（VI）/Fenton联合体系对菲的作用机理及菲的降解路径.结果表明，弱酸条件下Fe（VI）氧化菲时，·OH参与反应较少，起氧化作用的可能为中间高价态铁.在该条件下，Fe（VI）对菲的降解效果稍差于中性及碱性，但此时Fe（VI）的高氧化性能可提高菲的矿化效果.联合氧化体系中，菲逐步被氧化、羟基化、脱碳、加氢而最终转化为CO2和H2O，主要的中间产物为邻苯二甲酸酯衍生物和9-芴甲醛衍生物.联合氧化体系可合理利用Fe（VI）氧化过程中产生的Fe（II），并发挥高价态铁与·OH在氧化性能上的优势，实现对菲及产物的降解与矿化.
- Abstract：The combined system of Fe(VI) and Fenton has been found to be effective to degrade polycyclic aromatic hydrocarbons, but the associated mechanisms still need to be further explored. Fluorescence and GC-MS technologies were used to investigate the effects of Fe(VI) on the removal of phenanthrene under weak acid conditions. The oxidation mechanism in the reactions under weak acid conditions were also studied by comparing to that under the neutral and alkaline conditions for further analyzing degradation pathway and the associated mechanisms of phenanthrene removal by the combined system. The results showed that ·OH was less involved in the process of the oxidation of phenanthrene by Fe(VI) under weak acid conditions, and high-valent intermediate iron species might play a major role in the reactions. Under weak acid condition, the removal of phenanthrene by Fe(VI) was slightly less than that under neutral and alkaline conditions. However, due to the high oxidation performance of Fe(VI), the mineralization of phenanthrene under weak acid conditions was higher than that under neutral and alkaline conditions. In the combined system of Fe(VI) and Fenton, phenanthrene was gradually oxidized, hydroxylated, decarbonized, and hydrogenated and finally converted into CO2 and H2O. The main intermediate products were phthalate derivatives and 9-fluorene formaldehyde derivatives. The combined system of Fe(VI) and Fenton can make rational use of Fe (II) produced during the oxidation of Fe(VI), and effectively mineralize and degrade phenanthrene and its products by taking advantages of respective oxidation ability of the high-valent iron species and ·OH.
