王会敏,聂文善,唐瑶,雷鸣,唐和清.ZnMnxCo2-xO4活化过一硫酸盐降解有机污染物[J].环境科学学报,2021,41(2):486-494
ZnMnxCo2-xO4活化过一硫酸盐降解有机污染物
- Degradation of organic contaminants by peroxymonosulfate activated with ZnMnxCo2-xO4 as a heterogeneous catalyst
- 基金项目：国家自然科学基金（No.21707170）；中央高校基本科研业务费专项资金项目（No.CZT20019）
- 王会敏
- 中南民族大学资源与环境学院, 武汉 430074
- 聂文善
- 中南民族大学资源与环境学院, 武汉 430074
- 唐瑶
- 中南民族大学资源与环境学院, 武汉 430074
- 雷鸣
- 中南民族大学资源与环境学院, 武汉 430074
- 唐和清
- 中南民族大学资源与环境学院, 武汉 430074
- 摘要：分别以Zn（CH3COO）2·2H2O、Mn（CH3COO）3·2H2O和Co（CH3COO）2·4H2O为锌源、锰源和钴源，采用溶胶-凝胶自燃烧法成功制备了ZnMnxCo2-xO4（x=0~2）复合物，并用X射线衍射和X射线光电子能谱对其进行表征.同时，还研究了Mn/Co物质的量比、催化剂用量及PMS用量对目标污染物降解的影响.结果表明，该复合物可催化活化过一硫酸钾（PMS）降解有机污染物，当催化剂中x=0.8，催化剂投加量为0.2 g·L-1，PMS用量为0.4 mmol·L-1（0.25 g·L-1）时，20 μmol·L-1（10 mg·L-1）罗丹明B（RhB）可在15 min内完全降解.ZnMn0.8Co1.2O4的高催化活性主要归功于Mn3+和Co2+的协同效应.将ZnMnxCo2-xO4-PMS体系用于亚甲基蓝、结晶紫、金橙、双酚A、4-氯酚等其他污染物的降解，也取得了较好的效果.基于电子自旋共振ESR和自由基猝灭实验的结果，可以推测该反应体系中活性物种为硫酸根自由基和羟基自由基.
- Abstract：ZnMnxCo2-xO4 was successfully prepared by a sol-gel autocombustion method using Zn(CH3COO)2·2H2O, Mn(CH3COO)3·2H2O and Co(CH3COO)2·4H2O as sources of zinc, manganese and cobalt, respectively. The obtained ZnMnxCo2-xO4 was characterized by X-ray diffractometry and X-ray photoelectron spectrometry. It was found that the catalysts could activate potassium peroxymonosulfate (PMS) to degrade organic contaminants. The use of 0.2 g·L-1 ZnMn0.8Co1.2O4 and 0.4 mmol·L-1(0.25 g·L-1) PMS led to the complete degradation of 20 μmol·L-1 (10 mg·L-1) RhB within 15 min. It was also investigated the effect of Mn/Co molar ratio, catalysts load, and PMS concentration on the catalytic activities of ZnMnxCo2-xO4. The highly catalytic activity of ZnMnxCo2-xO4 was ascribed to the synergistic effect between Mn3+ and Co2+. The catalytic system also degraded efficiently other pollutants including methylene blue, crystal violet, golden orange, bisphenol A, and 4-chlorophenol. Based on electron spin-resonance (ESR) measurements and the free radical quenching studies, it was confirmed that the generated active species in the catalytic system involved both sulfate radical (SO4·-) and hydroxyl radical (·OH).
