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用改性磁性碳的可回收纳米复合材料 g-CN 活化过一硫酸盐降解酸性橙 7。

Degradation of Acid Orange 7 by peroxymonosulfate activated with the recyclable nanocomposites of g-CN modified magnetic carbon.

机构信息

School of Chemistry and Chemical Engineering, Wuhan Textile University, Wuhan, 430200, China.

Engineering Research Centre for Cleaner Production of Textile Printing and Dyeing, Ministry of Education, Wuhan, 430200, China.

出版信息

Chemosphere. 2018 Aug;205:297-307. doi: 10.1016/j.chemosphere.2018.04.139. Epub 2018 Apr 23.

Abstract

Carbon-based catalysts have attracted high attention since they are greener and cheaper, while magnetic nanomaterials are very useful in environmental application because of the easy recovery and operation given by the magnetic separability. Therefore, graphitic carbon nitride modified magnetic carbon nanocomposites FeO@C/g-CN was prepared herein for the first time as a new carbon-based catalyst for the activation of peroxymonosulfate (PMS). The catalytic properties of FeO@C/g-CN in activating PMS for the degradation of Acid Orange 7 (AO 7), a model organic pollutant, were investigated. AO 7 degradation efficiency was significantly enhanced after modification of FeO@C with g-CN, and the composite FeO@C/g-CN from loading of 5 wt% g-CN and calcined at 300 °C for 30 min exhibited the best performance. AO 7 could be efficiently decolorized using the "FeO@C/CN (5%) + PSM" system within the pH range of 2-6, and 97% of AO 7 could be removed in 20 min without pH adjustment (pH = 4). Radical quenching and EPR studies confirmed that both sulfate and hydroxyl radicals produced from PMS activation were the active species responsible for the oxidation of AO 7. The degradation mechanism was suggested based on the experimental results and XPS analyses. It was proposed that the CO groups on the carbon surface of FeO@C rather than the CO in g-CN played a key role as the active sites for PMS activation. The catalyst was magnetically separable and displayed good stability and reusability, thus providing a potentially green catalyst for sustainable remediation of organic pollutants.

摘要

碳基催化剂因其绿色环保和价格低廉而受到高度关注,而磁性纳米材料由于其易于回收和操作的磁性分离性能,在环境应用中非常有用。因此,本文首次制备了石墨相氮化碳修饰的磁性碳纳米复合材料 FeO@C/g-CN,作为一种新型的过一硫酸盐(PMS)活化用碳基催化剂。研究了 FeO@C/g-CN 活化 PMS 降解酸性橙 7(AO 7)模型有机污染物的催化性能。通过在 FeO@C 上负载 5wt%g-CN 并在 300°C 下煅烧 30min,改性后的 FeO@C/g-CN 的催化性能得到显著提高。在 pH 值为 2-6 的范围内,使用“FeO@C/CN(5%)+PSM”体系可以有效地对 AO 7 进行脱色,在不进行 pH 调节(pH=4)的情况下,20min 内可以去除 97%的 AO 7。自由基猝灭和 EPR 研究证实,PMS 活化产生的硫酸盐和羟基自由基都是氧化 AO 7 的活性物质。根据实验结果和 XPS 分析,提出了降解机制。研究表明,FeO@C 碳表面上的 CO 基团而不是 g-CN 中的 CO 基团作为 PMS 活化的活性位点发挥了关键作用。该催化剂具有磁性分离性能,表现出良好的稳定性和可重复使用性,为可持续修复有机污染物提供了一种潜在的绿色催化剂。

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