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铁修饰共价有机框架作为活化过二硫酸盐降解2,4-二氯苯酚的高效催化剂:性能与机理洞察

Iron-decorated covalent organic framework as efficient catalyst for activating peroxydisulfate to degrade 2,4-dichlorophenol: Performance and mechanism insight.

作者信息

Han Yuhang, Tai Meng, Yao Yuxin, Li Jingyang, Wu Yuanyuan, Hu Bo, Ma Yunchao, Liu Chunbo

机构信息

Key Laboratory of Preparation and Application of Environmental Friendly Materials (Jilin Normal University), Ministry of Education, Changchun, 130103, China; College of Chemistry, Jilin Normal University, Siping, 136000, China.

Key Laboratory of Preparation and Application of Environmental Friendly Materials (Jilin Normal University), Ministry of Education, Changchun, 130103, China.

出版信息

J Colloid Interface Sci. 2024 Jun;663:238-250. doi: 10.1016/j.jcis.2024.02.165. Epub 2024 Feb 21.

Abstract

Herein, a novel two-dimensional double-pore covalent organic framework (JLNU-305) was synthesized using N,N,N',N'-tetrakis(4-aminophenyl)-1,4-phenylenediamine (TAPD) and 2,2'-bipyridine-5,5'-dicarboxaldehyde (BPDA). The extended π-π conjugated structure and nitrogen-riched pyridine in JLNU-305 (JLNU = Jilin Normal University) provide abundant binding sites for Fe doping. The obtained JLNU-305-Fe exhibited high and recycled catalytic efficiency for peroxydisulfate (PDS) activation to completely degrade 10 mg/L 2,4-dichlorophenol (2,4-DCP) within 8 min. The JLNU-305-Fe/PDS system showed excellent catalytic activity and cyclic stability. The capture experiments and electron paramagnetic resonance (ESR) analysis indicated that the catalytic behavior of JLNU-305-Fe/PDS is contributed to the synergistic effect between free radicals and non-free radicals. It is the first time to activate PDS for covalent organic frameworks (COFs) being used to degrade 2,4-DCP, which has a great potential for development and practical application in related water environment remediation.

摘要

在此,使用N,N,N',N'-四(4-氨基苯基)-1,4-苯二胺(TAPD)和2,2'-联吡啶-5,5'-二甲醛(BPDA)合成了一种新型二维双孔共价有机框架(JLNU-305)。JLNU-305(JLNU =吉林师范大学)中扩展的π-π共轭结构和富含氮的吡啶为铁掺杂提供了丰富的结合位点。所得的JLNU-305-Fe对过二硫酸盐(PDS)活化表现出高且可循环的催化效率,能在8分钟内完全降解10mg/L的2,4-二氯苯酚(2,4-DCP)。JLNU-305-Fe/PDS体系表现出优异的催化活性和循环稳定性。捕获实验和电子顺磁共振(ESR)分析表明,JLNU-305-Fe/PDS的催化行为归因于自由基和非自由基之间的协同作用。这是首次将用于降解2,4-DCP的共价有机框架(COF)活化PDS,在相关水环境修复中具有巨大的发展潜力和实际应用价值。

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