Department of Environmental Engineering, Wuhan University, Wuhan 430079, China; Shenzhen Research Institute of Wuhan University, Shenzhen 518057, China.
Department of Environmental Engineering, Wuhan University, Wuhan 430079, China; Shenzhen Research Institute of Wuhan University, Shenzhen 518057, China.
J Hazard Mater. 2016 May 15;309:87-96. doi: 10.1016/j.jhazmat.2016.01.023. Epub 2016 Jan 13.
The removal of bisphenol A (BPA) in aqueous solution by an oxidation process involving peroxymonosulfate (PMS) activated by CuFe2O4 magnetic nanoparticles (MNPs) is reported herein. The effects of PMS concentration, CuFe2O4 dosage, initial pH, initial BPA concentration, catalyst addition mode, and anions (Cl(-), F(-), ClO4(-) and H2PO4(-)) on BPA degradation were investigated. Results indicate that nearly complete removal of BPA (50 mg/L) within 60 min and 84.0% TOC removal in 120 min could be achieved at neutral pH by using 0.6 g/L CuFe2O4 MNPs and 0.3 g/L PMS. The generation of reactive radicals (mainly hydroxyl radicals) was confirmed using electron paramagnetic resonance (EPR). Possible mechanisms on the radical generation from CuFe2O4/PMS system are proposed based on the results of radical identification tests and XPS analysis. The lack of inhibition of the reaction by free radical scavengers such as methanol and tert-butyl alcohol suggests that these species may not be generated in the bulk solution, and methylene blue probe experiments confirm that this process does not involve free radical generation. Surface-bound, rather than free radicals generated by a surface catalyzed-redox cycle involving both Fe(III) and Cu(II), are postulated to be responsible for the mineralization of bisphenol A.
本文报道了一种利用 CuFe2O4 磁性纳米粒子(MNPs)活化过一硫酸盐(PMS)的氧化过程去除水溶液中双酚 A(BPA)的方法。考察了过一硫酸盐浓度、CuFe2O4 用量、初始 pH 值、初始 BPA 浓度、催化剂添加方式以及阴离子(Cl(-)、F(-)、ClO4(-)和 H2PO4(-))对 BPA 降解的影响。结果表明,在中性 pH 值下,使用 0.6 g/L 的 CuFe2O4 MNPs 和 0.3 g/L 的过一硫酸盐,可在 60 min 内几乎完全去除(50 mg/L)BPA,在 120 min 内去除 84.0%的总有机碳(TOC)。电子顺磁共振(EPR)证实了活性自由基(主要是羟基自由基)的生成。根据自由基识别试验和 XPS 分析的结果,提出了 CuFe2O4/PMS 体系中自由基生成的可能机制。甲醇和叔丁醇等自由基清除剂对反应没有抑制作用,表明这些物质可能不会在体相溶液中生成,亚甲基蓝探针实验证实该过程不涉及自由基生成。推测是表面结合的自由基,而不是涉及 Fe(III)和 Cu(II)的表面催化氧化还原循环生成的游离基,负责双酚 A 的矿化。