Immobilized hybrids between nitrogen-doped carbon and stainless steel derived Fe3O4 used as a heterogeneous activator of persulfate during the treatment of aqueous carbamazepine

水溶液 过硫酸盐 化学 X射线光电子能谱 催化作用 电子顺磁共振 核化学 无机化学 化学工程 有机化学 核磁共振 物理 工程类
作者
Lu Huang,Tao Zeng,Xuyang Xu,Zhiqiao He,Jianmeng Chen,Shuang Song
出处
期刊:Chemical Engineering Journal [Elsevier]
卷期号:372: 862-872 被引量:73
标识
DOI:10.1016/j.cej.2019.04.208
摘要

Immobilized activators of persulfate (PS) with high activity and stability are highly desirable from an industrial and environmental point of view. In this work, nitrogen-doped carbon (CNx) was successfully hybridized with stainless steel (SS) derived Fe3O4 to construct a SS supported CNx/Fe3O4 heterogeneous catalyst (CNx/Fe3O4/SS). When used in a sulfate radical (SO4−)-based advanced oxidation process (SR-AOP), CNx/Fe3O4/SS displayed significantly higher activity towards the degradation of aqueous carbamazepine (CBZ) when compared to the single Fe3O4 and CNx activators. The removal of CBZ had the most rapid progression, with an initial pH of 3.5, a temperature of 35 °C, an initially added PS concentration of 250 mg L−1 and an added amount of CNx/Fe3O4/SS of 0.30 g. The removal efficiency of CBZ was ∼100% after 35 min of SR-AOPs. In addition, the CNx/Fe3O4/SS catalyst was stable, as demonstrated by six successive cycling experiments. The results obtained from the electron paramagnetic resonance (EPR) spectra and radical quenching experiments indicated that both SO4− and HO contributed to the CBZ oxidation process. On the basis of X-ray photoelectron spectroscopy (XPS) and Fermi level analyses, it can be concluded that SO4− and HO originated from the Fe3O4 catalyzed decomposition of aqueous PS. CNx facilitated the redox cycle of Fe(III)/Fe(II) in Fe3O4. This study demonstrated the potential application of SR-AOPs to efficiently degrade organic contaminants.
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