多活性位点的磁性氮掺杂石墨烯活化过一硫酸盐研究

杨柳; 刘丹; 刘世昂; 吴西林; 陈建荣

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中国环境科学 ›› 2021, Vol. 41 ›› Issue (9) : 4127-4134.

水污染与控制

多活性位点的磁性氮掺杂石墨烯活化过一硫酸盐研究

杨柳, 刘丹, 刘世昂, 吴西林, 陈建荣

作者信息 +

Magnetic N-doped graphene with multiple catalytic sites for efficient activiation of peroxymonosulfate

YANG liu, LIU Dan, LIU Shi-ang, WU Xi-lin, CHEN Jian-rong

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摘要

通过简单的一锅法制备Fe₂O₃、Fe₃N、单原子Fe（SA-Fe）和N掺杂的磁性石墨烯材料（Fe-MNG）应用于催化活化过一硫酸盐（PMS）.结果表明，Fe-MNG/PMS体系可在宽的pH范围（3-10）氧化降解磺胺异恶唑（SIZ），降解率均达到99%以上.经过五次循环使用其对SIZ的降解率仍保持在95%以上.Fe-MNG中的SA-Fe、N等活性位点可高效催化活化PMS产生各种活性氧物种（ROS）.淬灭实验和电子顺磁共振波谱分析表明Fe-MNG/PMS体系中产生多种ROS，包括硫酸根自由基（SO₄·^-）、羟基自由基（HO·）和单线态氧（¹O₂），证明存在自由基和非自由基两种氧化过程.此外，Fe-MNG具有大的比表面积（446.18m²/g），能将水中有机微污染物吸附富集到材料表面，同时在Fe-MNG表面催化PMS产生大量ROS，实现对有机微污染物的原位、高效氧化去除.Fe-MNG还具有磁性，易于分离和回收，具有潜在的应用前景.

Abstract

The Fe₂O₃, Fe₃N, single-atom Fe (SA-Fe) and N-doped magnetic graphene (Fe-MNG) were prepared by a facile one-pot method and applied for the activation of perpxymonosulfate (PMS). The results show that Fe-MNG/PMS system was efficient for the oxidative degradation of sulfisoxazole (SIZ) over a wide pH range (3~10) with the removal percentages over 99%. After five cycles, degradation percentages of SIZ maintain over 95% by using the recycled Fe-MNG catalyst. The multiple catalytic sites such as SA-Fe and N of Fe-MNG can effectively activate PMS for the generation of various reactive oxygen species (ROS). Quenching experiment and electron paramagnetic resonance spectroscopy showed that SO₄^·-, HO· and ¹O₂ were produced in the Fe-MNG/PMS system, demonstrating the co-existence of free radicals and non-radicals processes. In addition, the Fe-MNG possesses large surface area (446.18m²/g), which can pre-concentrate organic micropollutants onto its surface by adsorption, simultaneously producing a large amount of ROS via PMS activation, leading to the in-situ and high-efficiency oxidation and removal of organic micropollutants. The Fe-MNG also possesses magnetic properties which can be easily recycled, indicating its great application potential.

导出引用

杨柳, 刘丹, 刘世昂, 吴西林, 陈建荣. 多活性位点的磁性氮掺杂石墨烯活化过一硫酸盐研究[J]. 中国环境科学. 2021, 41(9): 4127-4134

YANG liu, LIU Dan, LIU Shi-ang, WU Xi-lin, CHEN Jian-rong. Magnetic N-doped graphene with multiple catalytic sites for efficient activiation of peroxymonosulfate[J]. China Environmental Science. 2021, 41(9): 4127-4134

中图分类号： X703.5

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