单原子Mn-N-C催化活化过一硫酸盐降解2,4-二氯苯酚
Degradation of 2,4-dichlorophenol by single atom Mn-N-C catalyst activated peroxymonosulfate
唐佳杰 1汤岚 1陆熙 2李杨 3朱陆祥 1孙铸宇 1赵晓祥1
作者信息
- 1. 东华大学环境科学与工程学院,上海
- 2. 三峡智慧水务科技有限公司,上海;上海勘测设计研究院有限公司,上海
- 3. 深圳信息职业技术学院交通与环境学院,广东深圳
- 折叠
摘要
针对2,4-二氯苯酚(2,4-Dichlorophenol,2,4-DCP)对环境污染的危害,急需开发一种清洁高效的处理方式.研究采用模板蚀刻法制备了锚定在氮掺杂碳上的Mn单原子催化剂(Mn-N-C),Mn原子以Mn—Nx的形式均匀地稳定在载体上,该结构增强了 Mn-N-C材料的极化和电子传递.当Mn-N-C和PMS的投加量分别为50 mg/L和0.8 mmol/L时,在温度为25 ℃,pH=7.0的条件下,2,4-DCP在60 min内降解率为99.6％,拟一级反应速率常数kobs=0.078 6 min-1.通过分析计算,Mn-N-C中Mn—Nx和N—(C)3结构活化PMS产生1O2和·O2-,而后2,4-DCP主要由通过羟基化、脱氯和开环反应降解,降解产物的毒性大幅降低.试验结果表明:Mn-N-C在活化PMS降解2,4-DCP显现出优异的催化活性;Mn-N-C/PMS体系具有一定抗干扰能力、优异的稳定性和可重复使用性,为实际废水中2,4-DCP的处理提供了一种有效方法.
Abstract
Aiming at the harm of 2,4-Dichlorophenol(2,4-DCP)to environmental pollution,it is urgent to develop a clean and efficient treatment method.Study synthesized a Mn-single atom catalyst(Mn-N-C)anchored on nitrogen doped carbon substrate by template etching method.Mn atoms were uniformly stabilized on the support in the form of Mn-Nx,which enhanced the polarization and electron transfer of Mn-N-C.When the addition of Mn-N-C and PMS were 50 mg/L and 0.8 mmol/L respectively,the degradation rate of 2,4-DCP was 99.6％within 60 min at the temperature of 25 ℃ and pH of 7.0,and the pseudo-first-order reaction rate constant kobs=0.078 6 m in-1.Through analysis and calculation,Mn—Nx and N—(C)3 structures in Mn-N-C activated PMS to produce 1 O2 and·O-,then 2,4-DCP was mainly degraded by 1 O2 via three dominant pathways,namely hydroxylation,dechlorination and ring-opening reaction,which significantly reduced the toxicity of the degradation products.The experimental results indicated that Mn-N-C shows excellent catalytic activity in activating PMS to degrade 2,4-DCP;Mn-N-C/PMS system has certain anti-interference ability,excellent stability and reusability,which provides an effective method for the treatment of 2,4-DCP in real wastewaters.
关键词
单原子催化剂/过一硫酸盐/单线态氧/2,4-二氯苯酚/降解Key words
single atom catalyst/peroxymonosulfate/singlet oxygen/2,4-dichlorophenol/degradation引用本文复制引用
基金项目
国家自然科学基金青年基金(21906016)
上海勘测设计研究院有限公司项目(2023-8w-0008)
深圳信息职业技术学院博硕科研启动扶持项目(SZIIT2022KJ073)
出版年
2024
NETL
NSTL
维普
万方数据