OMS-2活化过硫酸盐降解有机污染物  

Degradation of organic contaminants by OMS-2 activated persulfate

作　　者：沈悦 曹鸿健 刘晓恬 廖用开 蔡超[1] SHEN Yue;CAO Hong-jian;LIU Xiao-tian;LIAO Yong-kai;CAI Chao(State Key Laboratory of Urban Environment and Health,Institute of Urban Environment,Chinese Academy of Sciences,Xiamen 361021,China;University of Chinese Academy of Sciences,Beijing 100049,China)

机构地区：[1]中国科学院城市环境研究所城市环境与健康重点实验室,福建厦门361021 [2]中国科学院大学,北京100049

出　　处：《中国环境科学》2025年第4期1939-1950,共12页China Environmental Science

基　　金：国家重点研发计划基金资助项目(2023YFC3709700);福建省科技计划引导性项目基金资助项目(2022Y0073)。

摘　　要：以过硫酸钾和乙酸锰为原料,采用固相法制备了氧化锰八面体分子筛(OMS-2_(PS)),采用X射线衍射仪(XRD),傅里叶变换红外光谱仪(FT-IR),X射线光电子能谱仪(XPS)等手段对OMS-2_(PS)进行表征,考察了OMS-2_(PS)活化过硫酸盐(PS)降解有机污染物的性能,研究了催化剂投加量,PS浓度和初始pH值等反应条件对目标污染物去除效果的影响,探究了OMS-2_(PS)活化PS的作用机制.结果表明,采用固相法成功制备出OMS-2_(PS),且呈纳米棒状结构.OMS-2_(PS)可有效活化PS降解水中有机污染物,当酸性橙7(AO7)浓度为50mg/L,催化剂投加量为1.0g/L,PS浓度为2.0mmol/L时,60min内AO7的去除率和矿化率分别为97.4%和50.1%.离子共存实验结果表明,Cl^(-),NO_(3)^(-)和CO_(3)^(2-)对AO7的去除具有显著的抑制作用,而HA对AO7的去除几乎没有影响.自由基淬灭实验和电子顺磁共振(EPR)分析结果表明,OMS-2_(PS)/PS体系中主要活性物种为·OH和SO_(4)^(·-),且其中·OH对AO7的去除起主导作用.XPS分析结果表明,OMS-2_(PS)表面的Mn(Ⅳ)和晶格氧是活化PS的主要活性位点.结合实验结果,分析OMS-2_(PS)活化PS的机制可能是PS先通过OMS-2_(PS)表面-OH和OMS-2_(PS)结合,进而PS与OMS-2_(PS)表面的活性位点反应产生活性物种.此外,将OMS-2_(PS)/PS体系用于不同水体及其他有机污染物(双酚A,萘,四环素)的降解,也展现出良好的降解效果,表明该体系在环境污染治理领域具有广阔的应用前景.In the present study,Manganese oxide octahedral molecular sieve(OMS-2_(PS))was synthesized using K2S2O8 and(CH3COO)2Mn·4H2O via a solid-phase method.The physicochemical properties of OMS-2_(PS)were analyzed via X-ray diffraction(XRD),Fourier-transform infrared spectroscopy(FT-IR),and X-ray photoelectron spectroscopy(XPS).The performance of persulfate activation by OMS-2_(PS)for degrading organic contaminants was examined.This study also investigated the effect of various parameters,including dosage of OMS-2_(PS),PS concentration,and initial pH,on AO7 removal efficiency.Moreover,the mechanism of PS activation by OMS-2_(PS)was explored.The results showed OMS-2_(PS)was successfully synthesized via a solid-phase method,which exhibits a nanorod structure.OMS-2_(PS)could activate PS to degrade organic contaminants.The use of 50mg/L AO7,1.0g/L OMS-2_(PS),and 2.0mmol/L PS led to the AO7 removal and mineralization rates of 97.4%and 50.1%,respectively.Ion coexistence experiments demonstrated that AO7 removal was considerably inhibited by Cl^(-),NO_(3)^(-),and CO_(3)^(2-),while HA had almost no effect on it.The free radical quenching experiments and electron paramagnetic resonance(EPR)analysis indicated·OH and SO_(4)^(·-)were the primary active oxygen species in the OMS-2_(PS)/PS system,and·OH played the dominant role in the AO7 degradation.XPS analysis revealed Mn(IV)and lattice oxygen on the surface of OMS-2_(PS)were the main active sites for PS activation.Based on experiment results,a potential activation mechanism of PS by OMS-2_(PS)was proposed that PS combined with OMS-2_(PS)through the hydroxyl groups on the surface of OMS-2_(PS),and then PS reacted with the active sites on the surface of OMS-2_(PS)to produce active oxygen species.In addition,The OMS-2_(PS)/PS system effectively removed AO7 from different water bodies,and also degraded efficiently other pollutants including bisphenol A,naphthalene,and tetracycline,indicating that the OMS-2_(PS)/PS system have a bright application prospect in environmental polluti

关 键 词：OMS-2 催化活化 过硫酸盐 有机污染物 

分 类 号：X703.5[环境科学与工程—环境工程]