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氨三乙酸强化零价铁/过一硫酸盐降解橙黄G
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.
作者姓名:马红芳  杨浩宇  田委民  伍凌斌  陈秀峰  邹景
作者单位:1. 华侨大学土木工程学院市政工程系, 福建 厦门 361021;2. 华侨大学化工学院, 福建 厦门 361021
基金项目: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)
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.

关 键 词:氨三乙酸  零价铁  过一硫酸盐  活性物种  偶氮染料  
收稿时间:2020-08-24

Degradation of Orange G by Fe0/peroxymonosulfate with nitrilotriacetic acid enhancement
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[J].China Environmental Science,2021,41(4):1597-1607.
Authors:MA Hong-fang  YANG Hao-yu  TIAN Wei-min  WU Ling-bin  CHEN Xiu-feng  ZOU Jing
Institution:1. Department of Municipal Engineering, College of Civil Engineering, Huaqiao University, Xiamen 361021, China;2. College of Chemical Engineering, Huaqiao University, Xiamen 361021, China
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.
Keywords:nitrilotriacetic acid  zero valent iron  peroxymonosulfate  active species  azo dyes  
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