Catalytic degradation of diethyl phthalate in aqueous solution by persulfate activated with nano-scaled magnetic CuFe2O4/MWCNTs

Catalytic degradation of diethyl phthalate in aqueous solution by persulfate activated with nano-scaled magnetic CuFe2O4/MWCNTs
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纳米磁性CuFe2O4/MWCNTs活化过硫酸盐催化降解水溶液中邻苯二甲酸二乙酯

DOI:
10.1016/j.cej.2016.04.096
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发表时间:
2016-10
影响因子:
15.1
通讯作者:
Wang Zunyao
Wang Zunyao
中科院分区:
工程技术1区
文献类型:
--
作者:
Zhang Xiaoling;Feng Mingbao;Qu Ruijuan;Liu Hui;Wang Liansheng;Wang Zunyao

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邻苯二甲酸二乙酯(DEP)是一种广泛应用于化工行业的增塑剂,已被列为内分泌干扰物。因此,迫切需要开发降解DEP的方法,以降低其生态风险。本研究采用溶胶-凝胶燃烧法制备了铁氧体铜修饰的多壁碳纳米管磁性纳米颗粒(CuFe2O4/MWCNTs MNPs)作为降解DEP的催化剂,通过扫描电镜、透射电镜、傅里叶变换红外光谱、氮气吸收、x射线衍射和x射线光电子能谱对催化剂进行了表征。研究了过硫酸盐(PS)对DEP的催化降解,考察了催化剂负载、PS浓度、温度和ph等因素对其降解效果的影响。结果表明,CuFe2O4/MWCNTs MNPs对DEP具有较高的催化活性、稳定性和可回收性。特别是,从重复使用的CuFe2O4/MWCNTs中,金属离子的浸出可以忽略不计(浓度< 0.4%),表明其具有抗氧化性。电子顺磁共振分析证实,在PS体系中加入CuFe2O4/MWCNTs可以加速自由基dotOH和SO4 -自由基点的生成,猝灭实验进一步证实了催化反应以SO4 -自由基点为主。鉴定了降解中间体,并提出了降解途径。总的来说,本研究为CuFe2O4/MWCNTs活化PS在室温下去除DEP提供了实用知识。
Diethyl phthalate (DEP), a plasticizer widely used in chemical industry, has been classified as an endocrine disruptor. Therefore, it is urgent to develop methods for degradation of DEP to minimize its ecological risk. In this study, copper ferrite decorated multi-walled carbon nanotubes magnetic nanoparticles (CuFe2O4/MWCNTs MNPs) were prepared by sol–gel combustion method as catalysts for the degradation of DEP. The catalysts were characterized by scanning electron microscope, transmission electron microscope, Fourier transform infrared spectroscopy, nitrogen gas uptake, X-ray diffraction, and X-ray photoelectron spectroscopy. Catalytic degradation of DEP by persulfate (PS) was investigated with various influencing factors including catalyst loading, PS concentrations, temperature and pH. Furthermore, the CuFe2O4/MWCNTs MNPs showed high catalytic activity, stability and recyclability in DEP removal. Especially, leaching of metal ions from reused CuFe2O4/MWCNTs was negligible (concentration < 0.4%), indicating the resistance to oxidation. The electron paramagnetic resonance analysis confirmed that the addition of CuFe2O4/MWCNTs into PS system can accelerate the generation ofradical dotOH and SO4−radical dot, and the quenching experiments further certified the catalytic reaction was predominated by SO4−radical dot. The degradation intermediates were identified and the pathways were proposed. Overall, this study provides practical knowledge for DEP removal by CuFe2O4/MWCNTs activated PS at ambient temperature.
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