中国环境科学2024,Vol.44Issue(10) :5630-5638.

氨基羧酸类配体强化Fe2+活化分子氧降解对硝基酚

Effect and mechanism of Fe2+-activated molecular oxygen advanced oxidation of p-nitrophenol enhanced by aminocarboxylic acid chelating agents

辛思怡 张成武 王瑛琪 王德玉 赵薇 秦传玉 任黎明
中国环境科学2024,Vol.44Issue(10) :5630-5638.

氨基羧酸类配体强化Fe2+活化分子氧降解对硝基酚

Effect and mechanism of Fe2+-activated molecular oxygen advanced oxidation of p-nitrophenol enhanced by aminocarboxylic acid chelating agents

辛思怡 1张成武 1王瑛琪 1王德玉 1赵薇 1秦传玉 1任黎明2
扫码查看

作者信息

  • 1. 吉林大学,地下水资源与环境教育部重点实验室,吉林长春 130021;吉林大学,石油化工污染场地控制与修复技术国家地方联合工程实验室,吉林长春 130021;吉林大学,吉林省水资源与环境重点实验室,吉林长春 130021
  • 2. 中石化石油化工科学研究院有限公司,北京 100083
  • 折叠

摘要

本研究构建了 Fe2+/O2/乙二胺四乙酸钠(EDTA)、Fe2+/O2/次氮基三乙酸钠(NTA)、Fe2+/O2/乙二胺二琥珀酸(EDDS)高级氧化体系,选取对硝基酚(PNP)为目标污染物,探究3种体系降解PNP的性能,着重分析Fe2+/O2/EDTA、Fe2+/O2/NTA体系的ROS产生过程及对污染物的降解贡献,阐明氨基羧酸类配体的强化效果及机制.结果表明,Fe2+/O2/EDTA、Fe2+/O2/NTA体系的最佳降解条件均为pH=3、Fe2+与配体物质的量比为1∶1,PNP降解率分别为50.8%、81.2%.Fe2+/O2/EDTA体系生成的ROS为HO·与O2·-,ROS产生途径存在单电子转移(O2→O2·-→H2O2→HO·)、双电子转移(O2→H2O2→HO·)途径,部分PNP被O2·-还原为对氨基酚,大多数PNP及其还原产物被HO·氧化生成对苯二酚和对苯醌,之后氧化开环;Fe2+/O2/NTA体系生成的ROS主要是HO·,体系ROS产生途径主要为双电子转移途径,PNP被HO·直接氧化,生成对苯二酚和对苯醌,之后氧化开环.此外探究了两种配体活化能力的差异及机制.

Abstract

Three advanced oxidation systems,including Fe2+/O2/disodium ethylenediamine tetraacetate(EDTA),Fe2+/O2/trisodium nitrilotriacetate(NTA)and Fe2+/O2/N,N'-Ethylenediamine disuccinic acid(EDDS)systems,were constructed to investigate the effectiveness of the 3 systems focr removing target contaminant p-nitrophenol(PNP).The generation process of reactive free radicals,and their contribution of pollutants degradation as well as the enhancement of aminocarboxylate ligands and its underlying mechanisms were also studied and clarified in the system of Fe2+/O2/EDTA and Fe2+/O2/NTA.The highest PNP degradation efficiency of 50.8%and 81.2%were achieved in the system of Fe2+/O2/EDTA and Fe2+/O2/NTA,respectively,under pH=3 and the molar ratio of Fe2+to ligand of 1∶1.The reactive free radicals generated by Fe2+/O2/EDTA system were HO·and O2,with two generation pathway(one-electron transfer mechanism:O2→O2·-→H2O2→HO·;two-electron transfer mechanism:O2→H2O2→HO·).initial PNP was reduced to p-aminophenol by O2·-;PNP and its reduction products were oxidized by HO to hydroquinone and p-benzoquinone,followed with the ring structure breakage.HO·was the major reactive free radicals generated by Fe2+/O2/NTA system by two-electron transfer mechanism.PNP was directly oxidized by HO·to hydroquinone and p-benzoquinone,followed with the ring structure breakage.The mechanisms of the difference in the activation capacity of the two ligands were studied.

关键词

分子氧活化/活性自由基/乙二胺四乙酸钠/次氮基三乙酸钠/二价铁/对硝基酚

Key words

molecular oxygen activation/reactive free radicals/disodium ethylenediaminetetraacetate(EDTA)/trisodium nitrilotriacetate(NTA)/ferrous iron/p-nitrophenol

引用本文复制引用

基金项目

国家自然科学基金青年基金项目(42107054)

吉林省科技发展计划项目(20230101132JC)

出版年

2024
中国环境科学
中国环境科学学会

中国环境科学

CSTPCDCHSSCD北大核心
影响因子:2.174
ISSN:1000-6923
参考文献量4
段落导航相关论文