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单原子Mn-N-C催化活化过一硫酸盐降解2,4-二氯苯酚

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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.
Degradation of 2,4-dichlorophenol by single atom Mn-N-C catalyst activated peroxymonosulfate
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.

single atom catalystperoxymonosulfatesinglet oxygen2,4-dichlorophenoldegradation

唐佳杰、汤岚、陆熙、李杨、朱陆祥、孙铸宇、赵晓祥

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东华大学环境科学与工程学院,上海

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

深圳信息职业技术学院交通与环境学院,广东深圳

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单原子催化剂 过一硫酸盐 单线态氧 2,4-二氯苯酚 降解

国家自然科学基金青年基金上海勘测设计研究院有限公司项目深圳信息职业技术学院博硕科研启动扶持项目

219060162023-8w-0008SZIIT2022KJ073

2024

东华大学学报(自然科学版)
东华大学

东华大学学报(自然科学版)

CSTPCD北大核心
影响因子:0.308
ISSN:1671-0444
年,卷(期):2024.50(2)
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