Magnetic recoverable MnFe2O4 and MnFe2O4-graphene hybrid as heterogeneous catalysts of peroxymonosulfate activation for efficient degradation of aqueous organic pollutants

Magnetic recoverable MnFe2O4 and MnFe2O4-graphene hybrid as heterogeneous catalysts of peroxymonosulfate activation for efficient degradation of aqueous organic pollutants
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磁性可回收MnFe2O4和MnFe2O4-石墨烯杂化物作为过一硫酸盐活化的多相催化剂,用于有效降解水性有机污染物

DOI:
10.1016/j.jhazmat.2014.01.027
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发表时间:
2014-04-15
影响因子:
13.6
通讯作者:
Wang, Shaobin
Wang, Shaobin
中科院分区:
环境科学与生态学1区
文献类型:
--
作者:
Yao, Yunjin;Cai, Yunmu;Wang, Shaobin

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基于磁铁的材料通常可对许多催化反应有效,并且在施用后可以磁恢复,比其他金属氧化物显示出优势。在目前的工作中,制备了磁性MNFE2O4纳米颗粒和MNFE2O4还原的石墨烯(RGO)杂化,并用作催化剂,以激活过氧甲硫酸盐(PMS)以氧化降解水中的各种有机污染物。从化学沉积和还原过程中,用纳米化的MNFE2O4颗粒(约13.2 nm)生产MNFE2O4-RGO杂交体。发现MNFE2O4或MNFE2O4-RGO在激活PMS以产生硫酸盐自由基以降解有机染料(甲基紫,甲基橙,甲基,甲基蓝,橙色II和Rhodamine B),并且可以用磁铁分离有机染料(甲基紫罗兰色,甲基甲基蓝色,甲基) 。全面研究了反应动力学,不同离子物种(CL-,HCO3-CH3COO-和NO3-)以及CL-强度,反应温度(25-65摄氏度),催化稳定性以及降解机制。 MNFE2O4-RGO(25.7 kJ/mol)上低的活化能证明了比MNFE2O4(31.7 kJ/mol)更高的化学性能,这表明石墨烯在增强染料的降解中起着重要作用。更重要的是,经过准备的MNFE2O4和MNFE2O4-RGO混合动力表现出稳定的性能,可以通过连续的降解实验易于回收和良好的稳定性去除废水中的有机污染物。 (c)2014 Elsevier B.V.保留所有权利。
Magnetic iron based materials are generally effective for many catalytic reactions and can be magnetically recovered after application, showing advantages than other metal oxides. In the present work, magnetic MnFe2O4 nanoparticle and MnFe2O4-reduced graphene oxide (rGO) hybrid were prepared and used as catalysts to activate peroxymonosulfate (PMS) to oxidatively degrade various organic pollutants in water. From a process of chemical deposition and reduction, MnFe2O4-rGO hybrids were produced with nanosized MnFe2O4 particles (ca. 13.2 nm). It was found that MnFe2O4 or MnFe2O4-rGO presented high activity in activating PMS to produce sulfate radicals for degradation of organic dyes (Methyl violet, Methyl orange, Methylene blue, Orange II and Rhodamine B) and could be separated with a magnet without any loss. The reaction kinetics, effect of different ion species (CL-, HCO3- CH3COO- and NO3-) and Cl- strength, reaction temperature (25-65 degrees C), catalytic stability, as well as degradation mechanism were comprehensively studied. The lower activation energy on MnFe2O4-rGO (25.7 kJ/mol) justify the higher chemical performance than that of MnFe2O4 (31.7 kJ/mol), suggesting that graphene plays a significant role in the enhanced degradation of dyes. More importantly, the as-prepared MnFe2O4 and MnFe2O4-rGO hybrid exhibited stable performance to remove the organic pollutants in wastewater with easy recycling and good stability by successive degradation experiments. (C) 2014 Elsevier B.V. All rights reserved.