Fenton回收铁砂对水体中盐酸四环素降解性能及机制研究  

Research Degradation Performance and Mechanism of Tetracycline Hydrochloride by Fenton Recycled Iron Sand in Water

作　　者：蒙李杰 黄闻宇 周磊 高宇凡 韦子深 董怡武 梁琛 MENG Lijie;HUANG Wenyu;ZHOU Lei;GAO Yufan;WEI Zishen;DONG Yiwu;LIANG Chen(School of Resources,Environment and Materials,Guangxi University,Nanning 530004,China;School of Resources and Environmental Engineering,East China University of Science and Technology,Shanghai 200237,China)

机构地区：[1]广西大学资源环境与材料学院,广西南宁530004 [2]华东理工大学资源与环境工程学院,上海200237

出　　处：《环境科学研究》2023年第12期2355-2368,共14页Research of Environmental Sciences

基　　金：南宁市重点研发计划项目(No.20225060);南宁“邕江计划”项目(No.2021001)。

摘　　要：Fenton法作为一种成熟的高级氧化技术,在工业废水深度处理中得到了广泛应用,然而,该方法同时会产生大量含铁固体废弃物,影响污水处理效果并增加运行成本.为了探索一种更直接的Fenton固废资源化利用方式,本研究收集了来自新型废水处理Fenton塔的铁砂和传统Fenton池的铁泥,并将它们作为催化剂在非均相Fenton体系中去除盐酸四环素(TC)的效率和机制进行了对比.结果表明:(1)新型废水处理Fenton塔的铁砂和传统Fenton池的铁泥在外观、微观结构和组成上都有明显区别,铁砂偏黄、铁泥偏红,铁砂具有介孔结构和相对简单的成分,比表面积为144.818 m^(2)/g,平均孔径为3.061 nm.(2)铁砂中Fe的质量分数远高于铁泥,且以不定型FeOOH的形式存在.铁砂中还含有S元素以及微量的其他金属元素,铁泥则缺乏S元素.(3)作为催化剂,铁砂和铁泥对TC的去除率分别为87.40%和29.83%.(4)铁砂对TC的吸附过程符合伪二级吸附动力学模型,在铁砂-H_(2)O_(2)体系中可以达到良好的降解效果.C1^(-)、NO_(3)^(-)、SO_(4)^(2-)对TC降解的影响较小,而HCO_(3)^(-)、H_(2)PO_(4)^(-)的存在会抑制TC的降解反应.机理探究试验表明,·OH、·O_(2)^(-)和^(1)O_(2)是反应过程中的主要活性基团,·O_(2)影响更大,·OH和^(1)O_(2)贡献相当,·OH和^(1)O_(2)起直接进攻作用,·O_(2)^(-)影响·OH和^(1)O_(2)的生成过程.铁砂-H_(2)O_(2)体系中的反应具有均相和非均相作用,主要以均相作用为主.研究显示,铁砂具备发生氧化还原反应的潜力,在直接应用于TC降解方面具有明显优势.Fenton method,as a well-known advanced oxidation technology,has been widely used in the advanced treatment of industrial wastewater.However,it generates a large amount of iron-containing solid waste,which affects the efficiency of sewage treatment and increases operating costs.In order to explore a more direct utilization of Fenton solid waste,this study collected iron sand from a novel wastewater treatment Fenton tower and iron sludge from traditional Fenton ponds,and compared their effectiveness as catalysts for the degradation of tetracycline hydrochloride(TC)in a heterogeneous Fenton system.(1)Iron sand and iron sludge have obvious differences in appearance,microstructure and composition.Iron sand is yellow,iron sludge is reddish,iron sand has a mesoporous structure with relatively simple composition,with a specific surface area of 144.818 m^(2)/g,and an average pore size of 3.061 nm.(2)The mass fraction of Fe in the iron sand is as high as 61%,which is significantly higher than that of the iron sludge,and exists in the form of indeterminate FeOOH.In addition,iron sand contains sulfur(S)and trace amounts of other metal elements,whereas iron sludge lacks sulfur(S).(3)Furthermore,iron sand and iron sludge have been used as catalysts for the removal of TC,and the removal of TC has been proven to be a important factor in the removal of TC.As catalysts,the removal of tetracycline hydrochloride by iron sand and iron sludge was 87.40%and 29.83%,respectively.(4)The adsorption process of TC on iron sand follows the pseudo-second-order kinetic model,and the iron sand-H_(2)O_(2)system has good degradation performance.The effects of Cl^(-),NO_(3)and SO_(4)^(2-)on the degradation of TC were relatively small,while the presence of HCO_(3)^(-)and H_(2)PO_(4)inhibited the degradation of TC.Mechanistic studies indicated that·OH,·O2^(-)and^(1)O_(2)were the main active radicals in the reaction process,with·O_(2)^(-)contributing the most,followed by·OH and^(1)O_(2)in comparable amounts.·OH and^(1)O_(2)act as direct attackers

关 键 词：Fenton铁砂 催化剂 非均相Fenton体系 盐酸四环素(TC) 机制研究 

分 类 号：X793[环境科学与工程—环境工程]