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[氧化石墨烯固定化纳米零价铁耦合弱磁场增强铬(Ⅵ)去除特性及机制(GO-nFe/WMF)]

[Enhanced Chromate (Ⅵ) Removal Characteristics and Mechanism Using Graphene Oxide Immobilized Nanoscale Zero-Valent Iron Coupled with a Weak Magnetic Field (GO-nFe/WMF)].

作者信息

Ji Meng, Bao Jian-Guo, Zhu Xiao-Wei, Du Jiang-Kun, Zheng Han

机构信息

Hubei Laboratory of Special Wastewater Treatment, School of Environmental Studies, China University of Geosciences, Wuhan 430074, China.

出版信息

Huan Jing Ke Xue. 2020 Jul 8;41(7):3326-3336. doi: 10.13227/j.hjkx.201912265.

DOI:10.13227/j.hjkx.201912265
PMID:32608906
Abstract

A green, high-efficiency mesoporous magnetic material with strong reusability and oxidation resistance, named graphene oxide immobilized nanoscale zero-valent iron (GO-nFe), was prepared by a co-precipitation method. The structure, appearance, surface elements, and valence of GO-nFe were characterized via FESEM, TEM, FTIR, BET, XRD, and XPS. The characteristics and mechanism of Cr(Ⅵ) treatment in water using a weak magnetic field (WMF) coupled with GO-nFe (GO-nFe/WMF) were studied. Batch experiments established that when the load mass ratio of GO to nFe was 1:10 under 20 mT weak magnetic field strength, the GO-nFe/WMF system could completely remove the 10 mg·L of Cr(Ⅵ) solution in 30 min, consistent with first-order dynamics. With a decrease in initial pH value and an increase in material dosage, the removal efficiency of Cr(Ⅵ) increased significantly by enhancing the release rate of Fe. ClO had no effect on the reaction, Cl could encourage corrosion and promote the corrosion of nFe to release Fe, CO restrained the reaction through an increase in initial pH of the solution, and SO could promote the dissolution of the nFe surface passivation film to accelerate the reaction process. The GO-nFe/WMF system can maintain high activity after five reuses and 30 days of exposure to air. XRD, XPS, and 1,10-phenanthroline shielding experiments proved that its great conductivity allowed GO to provide electron transfer sites to accelerate the transfer of electrons, and nFe could quickly release Fe. WMF generated a magnetic gradient force () that pushed the paramagnetic Fe ions in the diffusion boundary layer concentrated on the two poles of GO-nFe, where the most magnetic intensity was present, to exposed active sites on both sides. The high removal rate ability of GO-nFe to release Fe continuously was maintained.

摘要

通过共沉淀法制备了一种具有强可重复使用性和抗氧化性的绿色高效介孔磁性材料,命名为氧化石墨烯固定化纳米零价铁(GO-nFe)。通过场发射扫描电子显微镜(FESEM)、透射电子显微镜(TEM)、傅里叶变换红外光谱仪(FTIR)、比表面积分析仪(BET)、X射线衍射仪(XRD)和X射线光电子能谱仪(XPS)对GO-nFe的结构、外观、表面元素和价态进行了表征。研究了弱磁场(WMF)耦合GO-nFe(GO-nFe/WMF)处理水中Cr(Ⅵ)的特性和机理。批次实验表明,在20 mT弱磁场强度下,当GO与nFe的负载质量比为1:10时,GO-nFe/WMF体系能在30分钟内完全去除10 mg·L的Cr(Ⅵ)溶液,符合一级动力学。随着初始pH值的降低和材料用量的增加,通过提高Fe的释放速率,Cr(Ⅵ)的去除效率显著提高。ClO对反应无影响,Cl能促进腐蚀并促进nFe腐蚀以释放Fe,CO通过提高溶液初始pH值抑制反应,SO能促进nFe表面钝化膜的溶解以加速反应过程。GO-nFe/WMF体系在重复使用五次和暴露于空气中30天后仍能保持高活性。XRD、XPS和邻菲罗啉屏蔽实验证明,其良好的导电性使GO能够提供电子转移位点以加速电子转移,nFe能快速释放Fe。WMF产生磁梯度力(),将扩散边界层中的顺磁性Fe离子推至GO-nFe两极,此处磁强度最大,使两侧的活性位点暴露。GO-nFe持续释放Fe的高去除率能力得以保持。

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