Fe(Ⅵ)@PMS双氧化体系降解废水中的尼泊金甲酯  

Fe(Ⅵ)@PMS double oxidation system for degradation of methylparaben from wastewater

作　　者：赵文博 苏冰琴 张霞玲 宋鑫峂 林嘉伟 卫月星 ZHAO Wen-bo;SU Bing-qin;ZHANG Xia-ling;SONG Xin-tong;LIN Jia-wei;WEI Yue-xing(College of Civil Engineering,Taiyuan University of Technology,Taiyuan 030024,China;Shanxi Municipal Engineering Graduate Education Innovation Center,Jinzhong 030600,China;College of Environment and Ecology,Taiyuan University of Technology,Jinzhong 030600,China)

机构地区：[1]太原理工大学土木工程学院,山西太原030024 [2]山西省市政工程研究生教育创新中心,山西晋中030600 [3]太原理工大学环境与生态学院,山西晋中030600

出　　处：《中国环境科学》2024年第12期6921-6934,共14页China Environmental Science

基　　金：国家自然科学基金资助项目(22206149);山西省自然科学基金资助项目(202403021211189);山西省专利转化计划项目(202406023)。

摘　　要：采用高铁酸钾活化过一硫酸盐(Fe(Ⅵ)@PMS体系)降解废水中的尼泊金甲酯(MeP).考察了不同Fe(Ⅵ)投加量,PMS浓度,初始pH值,反应温度,MeP初始浓度和共存离子对Me P降解性能的影响.基于Box-Behnken实验设计进行了多因素实验,拟合了Me P降解率与Fe(Ⅵ)投加量,PMS浓度和初始pH值之间的关系,优化了反应条件.结果表明,在Fe(Ⅵ)投加量为0.92g/L,PMS浓度为1.08mol/L,初始pH值为6.83,反应温度25℃的条件下,反应60min MeP的降解率可达99.03%,与模型预测Me P最大降解率99.17%相近,表明该响应面模型具有较好的模拟和预测能力.Cl^(-),NO_(3)^(-),HCO_(3)^(-)和SO_(4)^(2-)对Me P的降解均没有显著影响.活性氧化物种鉴定实验证明,MeP的降解由自由基(·OH和SO_(4)^(-)·)和非自由基( ^(1)O_(2) )氧化共同完成,其中^(1)O_(2)发挥主要作用.液相色谱-质谱联用(LC-MS)分析显示,MeP降解的主要途径包括羟基化和脱羧反应.ECOSAR毒性分析显示,Fe(Ⅵ)@PMS体系可以显著降低Me P的毒性,最终将Me P分解为无毒无害的产物.Ferrate-activated peroxymonosulfate(Fe(Ⅵ)@PMS system) was used to degrade methylparaben(MeP) in wastewater.The degradation performance of MeP with different Fe(Ⅵ) dosage,PMS concentration,initial pH value,reaction temperature,initial MeP concentration and coexisting ions was investigated.Based on the Box-Behnken experimental design,a multifactorial experiment was conducted to fit the relationship between the degradation rate of MeP and Fe(Ⅵ) dosage,PMS concentration and initial pH to optimize the reaction conditions.The results showed that the MeP degradation rate was 99.03% under the conditions of Fe(Ⅵ) dosage of 0.92g/L,PMS concentration of 1.08mmol/L,initial pH of 6.83,and temperature of 25°C,which was similar to the model prediction of the maximum degradation rate of 99.17% for MeP,indicating that the response surface model has a better simulation and prediction ability.Cl~-,NO_(3)~-,HCO_(3)~-and SO_(4)^(2-)had no significant effect on the degradation of MeP.The free radical identification experiments proved that the degradation of MeP was accomplished by a combination of free radicals(·OH and SO_(4)~-·) and non-radical( ~1O_(2) ) oxidation,with ~1O_(2) playing a major role.Liquid chromatography-mass spectrometry(LC-MS) analysis showed that the main pathways of MeP degradation included hydroxylation and decarboxylation reactions.ECOSAR toxicity analysis showed that the toxicity of MeP could be significantly reduced into non-toxic and harmless in Fe(Ⅵ)@PMS system.

关 键 词：高铁酸盐Fe(Ⅵ) 过一硫酸盐(PMS) 双氧化体系 尼泊金甲酯(MeP) 响应面分析 降解机制 

分 类 号：X703.5[环境科学与工程—环境工程]