| Fe-cyclam/H2O2体系催化降解罗丹明B机制 |
| 摘要点击 1439 全文点击 562 投稿时间：2019-11-02 修订日期：2020-01-02 |
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| 中文关键词 染料废水 cyclam配体 高价铁-氧物质 非自由基 罗丹明B |
| 英文关键词 dye-containing wastewater cyclam ligand FeV-oxo species radical-free rhodamine B |
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| 中文摘要 |
| 传统的利用Fenton反应处理染料废水的方法pH适用范围窄、需大量亚铁盐的持续投加，限制了其应用.工作中成功制备了桥连四氮杂环十四烷铁配合物（Fe-cyclam），在较宽的pH范围（2~7）内都能活化H2O2降解罗丹明B，且在低催化剂条件下（<50 μmol·L-1），对罗丹明B的降解效果优于Fenton反应.该体系能快速降解罗丹明B、酸性红88、酸性橙Ⅱ、活性红24、中性红等多种染料，并对偶氮类染料有较高的选择性.Fe-cyclam的稳定性良好，3次循环降解后，罗丹明B的去除效率依然保持在90%以上.淬灭实验证明该过程为非自由基主导的降解过程，并通过电子顺磁共振（EPR）中捕获到高价铁-氧活性中间体FeV-oxo的生成.本工作证明了基于Fe-cyclam/H2O2体系能高效地降解废水中染料，具有较高的应用潜力. |
| 英文摘要 |
| Fenton reaction is a traditional method for the treatment of dye-containing wastewater. However, this process should be performed in a narrow pH range and requires large amounts of ferrous salt input, limiting its application. In this work, a robust iron complex bearing a cross-bridge cyclam ligand (Fe-cyclam) was successfully prepared. This complex could effectively activate H2O2 to degrade rhodamine B at a pH range of 2-7. The Fe-cyclam/H2O2 system was more effective in the degradation of rhodamine B than the Fenton reaction, when the input [Fe] was lower than 50 μmol·L-1. Moreover, in addition to rhodamine B, the Fe-cyclam/H2O2 system was also capable of degrading dyes such as acid red 88, acid orange II, reactive red 24, and neutral red. This system was more efficient in the degradation of azo dyes than that of triphenylmethane dyes. The removal of rhodamine B remained higher than 90% in three cycle experiments, indicating the excellent stability of Fe-cyclam. The quenching experiments proved that the degradation of rhodamine B by Fe-cyclam/H2O2 was a free-radical-control process. Meanwhile, the electron paramagnetic resonance captured the signals of high valent FeV-oxo species, indicating that FeV-oxo possibly mediated the degradation of rhodamine B in the Fe-cyclam/H2O2 system. This work proves the potential application of Fe-cyclam/H2O2 in the degradation of dyes in a practical environment. |
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