Immobilized hybrids between nitrogen-doped carbon and stainless steel derived Fe3O4 used as a heterogeneous activator of persulfate during the treatment of aqueous carbamazepine
Immobilized hybrids between nitrogen-doped carbon and stainless steel derived Fe3O4 used as a heterogeneous activator of persulfate during the treatment of aqueous carbamazepine
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DOI：
10.1016/j.cej.2019.04.208
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发表时间：
2019-09
影响因子：
15.1
通讯作者：
Lu Huang;T. Zeng;Xuyang Xu;Zhiqiao He;Jianmeng Chen;Shuang Song
中科院分区：
文献类型：
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作者：
Lu Huang;T. Zeng;Xuyang Xu;Zhiqiao He;Jianmeng Chen;Shuang Song
从工业和环境的角度来看，具有高活性和高稳定性的固定化过硫酸盐（PS）活化剂是非常需要的。本工作将氮掺杂碳（CNx）与不锈钢（SS）衍生的Fe 3 O 4杂化，制备了不锈钢负载的CNx/Fe 3 O 4多相催化剂（CNx/Fe 3 O 4/SS）。当用于基于硫酸根（SO 4 radical dot−）的高级氧化工艺（SR-AOP）时，CNx/Fe 3 O 4/SS对卡马西平水溶液（CBZ）的降解活性显著高于单一的Fe 3 O 4和CNx活化剂。CBZ的去除进展最快，初始pH为3.5，温度为35 °C，初始加入的PS浓度为250 mg L-1，CNx/Fe 3 O 4/SS的加入量为0.30 g。SR-AOPs对CBZ的去除率在35 min后可达100%以上。此外，CNx/Fe 3 O 4/SS催化剂是稳定的，通过六个连续的循环实验证明。电子顺磁共振（EPR）谱和自由基猝灭实验结果表明，SO 4自由基dot−和HO自由基dot −均参与了CBZ的氧化过程. X射线光电子能谱（XPS）和费米能级分析表明，Fe_3O_4催化PS水溶液分解产生了SO_4自由基点−和HO自由基点. CNx促进了Fe 3 O 4中Fe（III）/Fe（II）的氧化还原循环。本研究表明SR-AOPs在高效降解有机污染物方面具有潜在的应用价值。
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 Fe3O4to construct a SS supported CNx/Fe3O4heterogeneous catalyst (CNx/Fe3O4/SS). When used in a sulfate radical (SO4radical dot−)-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 Fe3O4and 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−1and 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 SO4radical dot−and HOradical dotcontributed to the CBZ oxidation process. On the basis of X-ray photoelectron spectroscopy (XPS) and Fermi level analyses, it can be concluded that SO4radical dot−and HOradical dotoriginated from the Fe3O4catalyzed 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.