Heterogeneous catalytic activation of peroxymonosulfate for efficient degradation of organic pollutants by magnetic Cu/Fe3O4 submicron composites
Heterogeneous catalytic activation of peroxymonosulfate for efficient degradation of organic pollutants by magnetic Cu/Fe3O4 submicron composites
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磁性Cu/Fe3O4亚微米复合材料多相催化活化过一硫酸盐高效降解有机污染物
DOI：
10.1016/s1872-2067(16)62566-4
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发表时间：
2017-02-01
影响因子：
16.5
通讯作者：
Tang, Heqing
中科院分区：
文献类型：
--
作者：
Nie, Gang;Huang, Jia;Tang, Heqing
采用水热法制备了磁性Cu-0/Fe 3 O 4亚微米复合材料，并将其作为非均相催化剂用于过一硫酸盐（PMS）的活化和有机污染物的降解.制备的Cu-0/Fe 3 O 4亚微米磁性复合材料由Cu-0和Fe 3 O 4晶体组成，平均粒径约为220 nm。Cu degrees/Fe 3 O 4复合材料能有效催化PMS活化生成单线态氧，从而诱导对罗丹明B、亚甲基蓝、橙子II、苯酚和4-氯苯酚的快速降解。使用0.1 g/L的Cu-0/Fe 3 O 4复合材料诱导完全去除罗丹明B（20 μ mol/L）15 min，亚甲蓝（20 μ mol/L），橙子II在初始pH值为7.0、PMS浓度为0.5mmol/L的条件下，苯酚（0.1mmol/L）30 min、4-氯苯酚（0.1mmol/L）15 min的降解速率分别为20 μ mol/L、20 μ mol/L、20 μ mol/L、20 μ mol/L。当PMS浓度为2.5mmol/L时，30 min内5种污染物的总有机碳（TOC）去除率均达到85%以上。降解速率显著高于单独使用Cu-0或Fe 3 O 4颗粒获得的降解速率。Cu-0/Fe 3 O 4复合材料对PMS的催化活性增强是由于复合材料中Cu-0和Fe 3 O 4晶体的协同作用。通过电子自旋共振和自由基猝灭实验，确定单线态氧是污染物降解的主要活性氧物种。Cu-0/Fe 3 O 4复合材料活化PMS的可能机理是有机污染物向PMS的电子转移导致PMS活化生成O-1（2），从而促进有机污染物的降解。作为磁性催化剂，Cu-0/Fe 3 O 4复合材料易于通过磁性分离回收，并在5个连续降解循环中表现出优异的稳定性。本研究为有机污染物的氧化去除提供了一种简便、绿色的多相催化方法。(C)2016年，中国科学院大连化学物理研究所。Elsevier B. V.出版，保留所有权利。
Magnetic Cu-0/Fe3O4 submicron composites were prepared using a hydrothermal method and used as heterogeneous catalysts for the activation of peroxymonosulfate (PMS) and the degradation of organic pollutants. The as-prepared magnetic Cu-0/Fe3O4 submicron composites were composed of Cu-0 and Fe3O4 crystals and had an average size of approximately 220 nm. The Cu degrees/Fe3O4 composites could efficiently catalyze the activation of PMS to generate singlet oxygen, and thus induced the rapid degradation of rhodamine B, methylene blue, orange II, phenol and 4-chlorophenol. The use of 0.1 g/L of the Cu-0/Fe3O4 composites induced the complete removal of rhodamine B (20 mu mol/L) in 15 min, methylene blue (20 mu mol/L) in 5 min, orange II (20 mu mol/L) in 10 min, phenol (0.1 mmol/L) in 30 min and 4-chlorophenol (0.1 mmol/L) in 15 min with an initial pH value of 7.0 and a PMS concentration of 0.5 mmol/L. The total organic carbon (TOC) removal higher than 85% for all of these five pollutants was obtained in 30 min when the PMS concentration was 2.5 mmol/L. The rate of degradation was considerably higher than that obtained with Cu-0 or Fe3O4 particles alone. The enhanced catalytic activity of the Cu-0/Fe3O4 composites in the activation of PMS was attributed to the synergistic effect of the Cu-0 and Fe3O4 crystals in the composites. Singlet oxygen was identified as the primary reactive oxygen species responsible for pollutant degradation by electron spin resonance and radical quenching experiments. A possible mechanism for the activation of PMS by Cu-0/Fe3O4 composites is proposed as electron transfer from the organic pollutants to PMS induces the activation of PMS to generate O-1(2), which induces the degradation of the organic pollutants. As a magnetic catalyst, the Cu-0/Fe3O4 composites were easily recovered by magnetic separation, and exhibited excellent stability over five successive degradation cycles. The present study provides a facile and green heterogeneous catalysis method for the oxidative removal of organic pollutants. (C) 2016, Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. All rights reserved.