氨三乙酸强化零价铁/过一硫酸盐降解橙黄G

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摘要采用氨三乙酸（NTA）强化和改善零价铁/过一硫酸盐（Fe⁰/PMS）体系降解水中偶氮染料的氧化效能，以橙黄G （OG）为目标污染物，研究了NTA强化Fe⁰/PMS （NTA/Fe⁰/PMS）体系中OG的降解效果和NTA的强化作用机制，并考察了NTA、Fe⁰、PMS等主要反应物浓度和水中常见的共存物质对OG降解效能的影响.结果表明，NTA能够强化Fe⁰/PMS体系降解OG的氧化效能，且初始pH值对其强化作用有显著影响.中性（pH=7）和酸性（pH=3）条件下，NTA/Fe⁰/PMS体系去除OG的表观速率常数分别较Fe⁰/PMS体系提高了31.3倍和5.5倍；增加NTA、Fe⁰和PMS浓度有助于OG的降解，但NTA超过8mmol/L或PMS超过1.0mmol/L时出现抑制现象；水质背景中，Cl^-的存在促进了OG的降解，HCO₃^-、H₂PO₄^-和腐殖酸则表现为不同程度的抑制作用；NTA/Fe⁰/PMS体系中，主导的活性物种为Fe⁰界面产生的SO₄^·-和·OH，界面作用和均相作用对OG的降解分别贡献了约83.2%和16.8%；加入NTA后，体系中生成的Fe³⁺/Fe²⁺能与其迅速形成络合物，既缓解了Fe⁰表面钝化层的形成，促进Fe⁰界面对PMS的直接活化，又提高了溶液中溶解性铁的浓度，促进均相作用对PMS的活化分解，使NTA/Fe⁰/PMS体系降解OG的氧化效能得到强化和改善.

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关键词 ：氨三乙酸, 零价铁, 过一硫酸盐, 活性物种, 偶氮染料

Abstract：Nitrilotriacetic acid (NTA) was applied to enhance and improve the oxidation efficiency of azo dyes in Fe⁰/PMS system. Taking Orange G (OG) as the target pollutant, the degradation efficiency of OG, the strengthening role of NTA, the effects of NTA, Fe⁰, PMS and general coexistence substances in water on the degradation of OG were studied in Fe⁰/PMS system enhanced with NTA(NTA/Fe⁰/PMS).The results demonstrated that the introduction of NTA could enhance the degradation of OG by Fe⁰/PMS system, and the initial pH had a significant effect on the enhancement. Under neutral (pH=7) and acidic (pH=3) conditions, the apparent rate constants of OG removal by NTA/Fe⁰/PMS system were 31.3 times and 5.5 times higher than those of Fe⁰/PMS system, respectively. Increasing the concentration of NTA, Fe⁰ and PMS facilitated the degradation of OG, but negative effects were observed when NTA or PMS concentration were over 8mmol/L and 1.0mmol/L, respectively. In the context of water quality, the presence of Cl^- promoted the degradation of OG, while HCO₃^-, H₂PO₄^- and Humic Acid showed different degrees of inhibition. In NTA/Fe⁰/PMS system, SO₄^·- and·OH produced at Fe⁰ interface was confirmed to be the dominant active species responsible for OG degradation, and heterogeneous and homogeneous activation of PMS contributed about 83.2% and 16.8% to the degradation of OG, respectively. When adding NTA to Fe⁰/PMS system, Fe³⁺/Fe²⁺ generated could be complexed rapidly with NTA, which not only alleviated the formation of passive layer and promoting the direct activation of PMS on Fe⁰ interface, but also increased the concentration of soluble iron in system, promoting the activation of PMS by homogeneous interaction. Thus, the degradation effect of OG in Fe⁰/PMS system was enhanced by NTA.

Key words： nitrilotriacetic acid zero valent iron peroxymonosulfate active species azo dyes

收稿日期: 2020-08-24

PACS:

X703.5

基金资助:国家自然科学基金资助项目（51708231）；福建省自然科学基金资助项目（2018J05084）

通讯作者: 邹景,副教授,zoujing@hqu.edu.cn E-mail: zoujing@hqu.edu.cn

作者简介: 马红芳(1969-),女,山西运城人,副教授,在读博士,主要从事高级氧化技术和水污染控制研究.发表论文30余篇.

引用本文:

马红芳, 杨浩宇, 田委民, 伍凌斌, 陈秀峰, 邹景. 氨三乙酸强化零价铁/过一硫酸盐降解橙黄G[J]. 中国环境科学, 2021, 41(4): 1597-1607. MA Hong-fang, YANG Hao-yu, TIAN Wei-min, WU Ling-bin, CHEN Xiu-feng, ZOU Jing. Degradation of Orange G by Fe⁰/peroxymonosulfate with nitrilotriacetic acid enhancement. CHINA ENVIRONMENTAL SCIENCECE, 2021, 41(4): 1597-1607.

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http://www.zghjkx.com.cn/CN/ 或 http://www.zghjkx.com.cn/CN/Y2021/V41/I4/1597

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