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硫氮共掺杂碳基材料活化过一硫酸盐降解2,4-二氯苯酚的效能及机理
引用本文:杨成海,宁寻安,赖晓君,王逸,吴诗音,李日文.硫氮共掺杂碳基材料活化过一硫酸盐降解2,4-二氯苯酚的效能及机理[J].环境科学学报,2021,41(7):2785-2795.
作者姓名:杨成海  宁寻安  赖晓君  王逸  吴诗音  李日文
作者单位:广东工业大学环境科学与工程学院,广州510006;广东省环境催化与健康风险控制重点实验室,环境健康与污染控制研究院,广州510006
基金项目:广东省"珠江人才计划"本土创新科研团队项目(No.2017BT01Z032)
摘    要:为了解决外源杂原子掺杂到碳基相催化剂过程中掺杂量低和分布不均的问题,本研究通过直接碳化聚吡咯(PPy)和聚噻吩(PTh)混合物制备得到硫氮共掺杂碳基催化材料(CPPy-PTh),并研究其活化过一硫酸盐(PMS)降解水中的2,4-二氯苯酚(2,4-DCP)的性能.结果表明,CPPy-PTh催化PMS可在30 min内降解99%的2,4-DCP.CPPy-PTh的高效催化能力主要是因为其表面被石墨化和氮、硫官能化,这使得PMS更容易在CPPy-PTh表面传递电子.淬灭实验和电子顺磁共振(EPR)结果表明,2,4-DCP的降解过程遵循以单线态氧(1O2)为主导的非自由基氧化途径.CPPy-PTh在宽广的pH范围和干扰离子存在下也同样具备催化能力.这些发现可为水中持久性有机物的降解提供理论指导和技术支持.

关 键 词:2  4-DCP  硫氮共掺杂  过一硫酸盐  单线态氧  催化  降解
收稿时间:2020/10/28 0:00:00
修稿时间:2020/11/27 0:00:00

Degradation efficiency and mechanism of 2, 4-dichlorophenol by activation of peroxymonosulfate with sulfur and nitrogen co-doped carbocatalysts
YANG Chenghai,NING Xun''an,LAI Xiaojun,WANG Yi,WU Shiyin,LI Riwen.Degradation efficiency and mechanism of 2, 4-dichlorophenol by activation of peroxymonosulfate with sulfur and nitrogen co-doped carbocatalysts[J].Acta Scientiae Circumstantiae,2021,41(7):2785-2795.
Authors:YANG Chenghai  NING Xun'an  LAI Xiaojun  WANG Yi  WU Shiyin  LI Riwen
Institution:1. School of Environmental Science and Engineering, Guangdong University of Technology, Guangzhou 510006;2. Guangzhou Key Laboratory of Environmental Catalysis and Pollution Control, Guangdong Key Laboratory of Environmental Catalysis and Health Risk Control, Guangzhou 510006
Abstract:In order to solve the problems of low doping amount and uneven distribution in the process of doping heteroatoms into carbocatalysts, a sulfur and nitrogen co-doped carbocatalysts (CPPy-PTh) was fabricated via facile carbonization of polypyrrole (PPy) and polythiophene (PTh) mixture. The peroxymonosulfate (PMS) catalytic performance of CPPy-PTh were investigated by degradation experiment of 2,4-dichlorophenol (2,4-DCP) in water. The results indicated that the as-fabricated CPPy-PTh revealed an outstanding catalytic capability with almost removal (99%) of 2,4-DCP within 30 min, which was attributed to the its graphitization and nitrogen-sulfur functionalization, causing more efficient for PMS to transfer electrons on its surface. Quenching tests and electron paramagnetic resonance (EPR) studies confirmed that the singlet oxygen(1O2) was the main reactive oxygen species, revealing that 2,4-DCP degradation follows predominantly the nonradical oxidation pathway. CPPy-PTh also showed an excellent catalytic capability in a wide range of pH and the presence of interfering ions. These findings could provide technical support and theoretical guidance for the degradation of persistent organic pollutants in water.
Keywords:2  4-DCP  sulfur-nitrogen co-doped  peroxymonosulfate  singlet oxygen  catalyze  degradation
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