Adsorption and catalytic oxidation of pharmaceuticals by nitrogen-doped reduced graphene oxide/Fe3O4 nanocomposite

Adsorption and catalytic oxidation of pharmaceuticals by nitrogen-doped reduced graphene oxide/Fe3O4 nanocomposite
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DOI:
10.1016/j.cej.2018.02.064
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发表时间:
2018-06-01
影响因子:
15.1
通讯作者:
Yu, Gang
Yu, Gang
中科院分区:
工程技术1区
文献类型:
--
作者:
Peng, Guilong;Zhang, Menghan;Yu, Gang

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采用水解法制备了一种具有吸附和催化降解水中药物功能的新型纳米复合材料(N-RGO/Fe 3 O 4)。磁性Fe 3 O 4纳米粒子修饰的氮改性还原氧化石墨烯(N-RGO)可提高其吸附和催化活性,并使其具有磁性分离性。N-RGO/Fe_3O_4对诺氟沙星(NOR)和酮洛芬(KP)具有较快的吸附,最大吸附量分别为158.1 mg/g和468.0 mg/g。N-RGO/Fe_3O_4复合材料可活化过硫酸盐(PS)产生活性自由基。研究了N-RGO/Fe_3O_4/PS体系对NOR的降解动力学和降解途径。投加10 mmol/LS 2 O 82-和100 mg/L N-RGO/Fe 3 O 4,在210 min内可完全去除20 mg/L的NOR,总有机碳(TOC)去除率为89%。电子自旋共振(ESR)测试表明,N-RGO/Fe_3O_4/PS体系在催化氧化过程中同时产生了中心点OH和SO_4-中心点,其中中心点OH起着重要作用。
A novel nanocomposites (N-RGO/Fe3O4) with the function of adsorption and catalytic degradation of pharmaceuticals in water was successfully synthesized through a facile hydrolysis process. The nitrogen modified reduced graphene oxide (N-RGO) incorporated with magnetic Fe(3)O(4 )nanoparticles could enhance its adsorption and catalytic activity, and allowed the magnetic separability. The as-prepared N-RGO/Fe3O4 exhibited relatively fast adsorption for norfloxacin (NOR) and ketoprofen (KP), and the maximum adsorption capacity on the NRGO/Fe3O4 was 158.1 mg/g for NOR and 468.0 mg/g for KP according to the Langmuir fitting. The N-RGO/Fe3O4 composite could activate persulfate (PS) to generate active radicals. NOR degradation kinetics and pathway by N-RGO/Fe3O4/PS system were also investigated. A complete removal of NOR (20 mg/L) was achieved within 210 min with the addition of 10 mmol/LS2O82- and 100 mg/L N-RGO/Fe3O4, and the removal efficiency of total organic carbon (TOC) was 89%. Electron spin resonance (ESR) tests verified that both center dot OH and SO4-center dot were produced in the catalytic oxidation process, and center dot OH played a significant role in the N-RGO/Fe3O4/PS system.