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通过形成羟基和硫酸根自由基,磁性多孔铜铁氧体催化过一硫酸盐氧化高效降解莠去津。

Efficient degradation of atrazine by magnetic porous copper ferrite catalyzed peroxymonosulfate oxidation via the formation of hydroxyl and sulfate radicals.

机构信息

State Key Laboratory of Urban Water Resource and Environment, Harbin Institute of Technology, Harbin 150090, People's Republic of China.

出版信息

Water Res. 2013 Sep 15;47(14):5431-8. doi: 10.1016/j.watres.2013.06.023. Epub 2013 Jun 20.

DOI:10.1016/j.watres.2013.06.023
PMID:23916710
Abstract

Magnetic porous copper ferrite (CuFe2O4) showed a notable catalytic activity to peroxymonosulfate (PMS). More than 98% of atrazine was degraded within 15 min at 1 mM PMS and 0.1 g/L CuFe2O4. In contrast, CuFe2O4 exhibited no obvious catalytic activity to peroxodisulfate or H2O2. Several factors affecting the catalytic performance of PMS/CuFe2O4 were investigated. Results showed that the catalytic degradation efficiency of atrazine increased with PMS and CuFe2O4 doses, but decreased with the increase of natural organic matters concentration. The catalytic oxidation also showed a dependence on initial pH. The presence of bicarbonate stimulated atrazine degradation by PMS/CuFe2O4 at low concentrations but inhibited the degradation at high concentrations. Furthermore, the reactive species for atrazine degradation in PMS/CuFe2O4 system were identified as hydroxyl radical (HO) and sulfate radical (SO4(·-)) through competition reactions of atrazine and nitrobenzene, instead of commonly used alcohol scavenging, which was not a reliable method in metal oxide catalyzed oxidation. Surface hydroxyl groups of CuFe2O4 were a critical part in radical generation and the copper on CuFe2O4 surface was an active site to catalyze PMS. The catalytic degradation of atrazine by PMS/CuFe2O4 was also effective under the background of actual waters.

摘要

磁性多孔铜铁氧体(CuFe2O4)对过一硫酸盐(PMS)表现出显著的催化活性。在 1 mM PMS 和 0.1 g/L CuFe2O4 下,15 分钟内超过 98%的莠去津被降解。相比之下,CuFe2O4 对过二硫酸盐或 H2O2 没有明显的催化活性。研究了影响 PMS/CuFe2O4 催化性能的几个因素。结果表明,莠去津的催化降解效率随 PMS 和 CuFe2O4 剂量的增加而增加,但随天然有机物浓度的增加而降低。催化氧化也依赖于初始 pH 值。碳酸氢根的存在在低浓度下刺激 PMS/CuFe2O4 对莠去津的降解,但在高浓度下抑制降解。此外,通过莠去津和硝基苯的竞争反应,确定 PMS/CuFe2O4 体系中莠去津降解的活性物质为羟基自由基(HO)和硫酸根自由基(SO4(·-)),而不是常用的醇清除法,这在金属氧化物催化氧化中不是一种可靠的方法。CuFe2O4 的表面羟基基团是自由基生成的关键部分,CuFe2O4 表面上的铜是催化 PMS 的活性位点。在实际水样的背景下,PMS/CuFe2O4 对莠去津的催化降解也是有效的。

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