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无金属氮掺杂碳空心球增强吸附及催化过一硫酸盐活化用于水体污染治理

Enhanced adsorption and catalytic peroxymonosulfate activation by metal-free N-doped carbon hollow spheres for water depollution.

作者信息

Li Xuemei, Yan Xinlong, Hu Xiaoyan, Feng Rui, Zhou Min, Wang Liping

机构信息

Key Laboratory of Coal Processing and Efficient Utilization (Ministry of Education), School of Chemical Engineering & Technology, China University of Mining and Technology, Xuzhou 221116, PR China.

Key Laboratory of Coal Processing and Efficient Utilization (Ministry of Education), School of Chemical Engineering & Technology, China University of Mining and Technology, Xuzhou 221116, PR China.

出版信息

J Colloid Interface Sci. 2021 Jun;591:184-192. doi: 10.1016/j.jcis.2021.01.094. Epub 2021 Feb 4.

Abstract

Rational design of metal-free carbon-based heterogeneous catatlyst for wastewater remediation via peroxymonosulfate (PMS) activation is highly desirable. Here, hollow structured porous carbon with abundant N, a high graphitization degree, and a large specific surface area and pore volume (1301 m/g and 1.12 cm/g) was synthesized by the pyrolysis of core-shell structured composites consisting of polystyrene (PS) cores and Zeolitic imidazolate frameworks-8 (ZIF-8) shells. The hollow structured carbon (CPS@ZIF-8) was characterized thoroughly and applied for phenol degradation by the activation of PMS. The effects of operation conditions such as the catalyst and PMS dose, phenol concentration, initial pH, and temperature on phenol removal were investigated comprehensively. Moreover, the main reactive species involved in phenol oxidation were investigated, and a plausible mechanism for the degradation of phenol is proposed. The results show that CPS@ZIF-8 exhibited an excellent phenol adsorption and degradation performance, which can be mainly ascribed to its large surface area, abundance of nitrogen and hollow porous structure. Moreover, both the nonradical pathway (involving O) and the radical pathway (involving SO and O) were found to be involved in the decomposition of phenol.

摘要

通过过一硫酸盐(PMS)活化来合理设计用于废水修复的无金属碳基多相催化剂是非常有必要的。在此,通过热解由聚苯乙烯(PS)核和沸石咪唑酯骨架-8(ZIF-8)壳组成的核壳结构复合材料,合成了具有丰富氮、高石墨化程度、大比表面积和孔体积(1301 m/g和1.12 cm/g)的中空结构多孔碳。对中空结构碳(CPS@ZIF-8)进行了全面表征,并将其应用于通过PMS活化降解苯酚。全面研究了催化剂和PMS剂量、苯酚浓度、初始pH值和温度等操作条件对苯酚去除的影响。此外,研究了苯酚氧化过程中涉及的主要活性物种,并提出了一种合理的苯酚降解机理。结果表明,CPS@ZIF-8表现出优异的苯酚吸附和降解性能,这主要归因于其大表面积、丰富的氮和中空多孔结构。此外,发现非自由基途径(涉及O)和自由基途径(涉及SO和O)均参与了苯酚的分解。

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