Activation of sodium percarbonate with ferrous ions for degradation of chlorobenzene in aqueous solution: mechanism, pathway and comparison with hydrogen peroxide

被引:31
作者
Zhang, Sai [1 ]
Hu, Xuebin [1 ]
Li, Li [1 ]
Huangfu, Xiaoliu [1 ]
Xu, Yingzhi [1 ]
Qin, Yuhang [1 ]
机构
[1] Chongqing Univ, Minist Educ, Key Lab Ecoenvironm Three Gorges Reservoir Reg, Chongqing 400045, Peoples R China
关键词
degradation pathway; Fe2+-catalysed; Fe2+/Fe3+-conversion; free radicals; pH; ADVANCED OXIDATION PROCESSES; FENTON-LIKE PROCESSES; ZERO-VALENT IRON; EFFICIENT TRANSFORMATION; CARBONATE RADICALS; WASTE-WATER; BY-PRODUCTS; HYDROXYL; KINETICS; REMOVAL;
D O I
10.1071/EN17137
中图分类号
O65 [分析化学];
学科分类号
070302 ; 081704 ;
摘要
Sodium percarbonate (SPC) could be applied as a strong oxidant to degrade organic compounds activated by transition metals. In this study, the degradation performance of chlorobenzene (CB) in the Fe2+-catalysed SPC system was investigated at different Fe2+ and SPC concentrations and pH conditions. Fe2+/Fe3+ conversion was also studied, and the SPC system was compared with the H2O2 and H2O2/Na2CO3 systems. Free radicals were identified through scavenging tests and electron paramagnetic resonance (EPR) experiments, and the reaction intermediates and by-products were determined as well. The results show that CB was completely removed when the molar concentration ratio of Fe2+/SPC/CB was 8 : 8 : 1 and that the decomposition of CB increased as the initial Fe2+/SPC dosage increased. The optimal molar concentration of Fe2+/SPC/CB was 2 : 1 : 1, and the degradation rate was inhibited when increasing or decreasing Fe2+ or SPC. CB degradation was not significantly affected by variation of initial pH, and the variation of pH during the degradation process corresponded well with the degree of Fe2+ to Fe3+ conversion and the formation of (OH)-O-center dot. It was confirmed that (OH)-O-center dot, O-2(center dot-) and O-1(2) participate in the degradation process. Moreover, not all the (OH)-O-center dot takes part in the degradation process, as some transforms into O-2(center dot-) and O-1(2). The same degradation efficiency was obtained when replacing SPC by equal stoichiometric amounts of H2O2, compared with inhibition with the addition of Na2CO3. Further, a likely degradation pathway for CB is proposed based on the identified products. These results show that the Fe2+/SPC system can form the basis of a promising technology for the remediation of CB-contaminated groundwater.
引用
收藏
页码:486 / 494
页数:9
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