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经胺强化Fe(Ⅲ)-NTA络合物活化过二硫酸盐降解磺胺甲恶唑

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针对 Fe(Ⅱ)/过二硫酸盐(Peroxydisulfate,PDS)高级氧化技术存在的pH值应用范围窄、铁泥产量大等缺陷,研究构建 Fe(Ⅲ)-氨三乙酸(Nitrilotriacetic Acid,NTA)/经胺(Hydroxylamine,HAm)/PDS体系,以在中性条件下高效降解水中新污染物磺胺甲恶唑(Sulfamethoxazole,SMX)。研究结果显示,Fe(Ⅲ)-NTA/HAm/PDS体系在pH=7条件下对SMX的降解率可达91%,该体系降解SMX的主要活性物种为·SO4-和。OH。SMX 在 Fe(Ⅲ)-NTA/HAm/PDS 体系中的降解效率随溶液pH值的升高而降低,且增加Fe(Ⅲ)、PDS的用量会加速SMX降解。NTA的引入可将Fe(Ⅱ)/PDS体系的pH值应用范围由酸性拓展至弱碱性,与此同时,向体系内加入HAm可有效减少铁泥的产量。根据检测到的降解产物,提出SMX在Fe(Ⅲ)-NTA/HAm/PDS体系中可能的降解途径包括断键反应、羟基化反应、氨基氧化反应。双酚AF、双氯芬酸、土霉素等其他新污染物也能在Fe(Ⅲ)-NTA/HAm/PDS体系中被高效去除,表明该体系在新污染物的降解领域有较大的应用潜力。
Hydroxylamine promoted degradation of sulfamethoxazole by Fe(Ⅲ)-NTA complexes activated peroxydisulfate
To overcome the shortcomings of Fe(Ⅱ)/peroxydisulfate(PDS)advanced oxidation technology such as narrow working pH range and large iron sludge production,Fe(Ⅲ)-nitrilotriacetic acid(NTA)/hydroxylamine(HAm)/PDS system was established in this work to effectively degrade sulfamethoxazole(SMX),an emerging contaminant,under neutral condition.Fe(Ⅲ)-NTA/HAm/PDS system was proved to exhibit a significant advantage over Fe(Ⅱ)/PDS system on the degradation of SMX.Firstly,the introduction of NTA could extend the working pH range of Fe(Ⅱ)/PDS system from acidic to weakly alkaline,which is more beneficial for the practical application of this technology.In addition,the introduction of HAm into this system could effectively drive the cycle of Fe(Ⅱ)/Fe(Ⅲ)and reduce the production of iron sludge,which will reduce the risk of secondary pollution.The result shows that the degradation efficiency of SMX in Fe(Ⅲ)-NTA/HAm/PDS system could reach 91%at pH 7.It was speculated that both·SO4-and·OH were responsible for the degradation of SMX in this system based on the results of the radical scavenging experiment.The effects of solution pH,Fe(Ⅲ)concentration,and PDS dose on the degradation of SMX were also systematically investigated.It is observed that the degradation of SMX in Fe(Ⅲ)-NTA/HAm/PDS system was obviously suppressed with increasing solution pH due to the change in the complexes formed between Fe(Ⅲ)and NTA.In contrast,the degradation of SMX in this system could be promoted by increasing the dosage of Fe(Ⅲ)and PDS.Six degradation products of SMX were detected in Fe(Ⅲ)-NTA/HAm/PDS system and three possible degradation pathways of SMX in this system were accordingly proposed,including bond cleavage,hydroxylation,and amino oxidation.Three different emerging contaminants(i.e.,bisphenol AF,diclofenac,and oxytetracycline)could also be effectively degraded in Fe(Ⅲ)-NTA/HAm/PDS system,suggesting that this system has a huge potential to be applied in the field of emerging contaminants degradation.

environmental engineeringsulfamethoxazolehydroxylamineFe(Ⅲ)-NTA complexesperoxydisulfate

王真然、彭藴斓、刘义青、付永胜

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西南交通大学地球科学与环境工程学院,成都 611756

环境工程学 磺胺甲恶唑 羟胺 Fe(Ⅲ)-NTA络合物 过二硫酸盐

四川省科技厅应用基础研究项目

2021YJ0385

2024

安全与环境学报
北京理工大学 中国环境科学学会 中国职业安全健康协会

安全与环境学报

CSTPCD北大核心
影响因子:0.943
ISSN:1009-6094
年,卷(期):2024.24(3)
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