Magnetic Cu^0/Fe3O4 submicron composites were prepared using a hydrothermal method and used as heterogeneous catalysts for the activation of peroxymonosulfate（PMS） and the degradation of organic pollutants.The as-pr...Magnetic Cu^0/Fe3O4 submicron composites were prepared using a hydrothermal method and used as heterogeneous catalysts for the activation of peroxymonosulfate（PMS） and the degradation of organic pollutants.The as-prepared magnetic Cu^0/Fe3O4 submicron composites were composed of Cu^0 and Fe3O4 crystals and had an average size of approximately 220 nm.The Cu^0/Fe3O4 composites could efficiently catalyze the activation of PMS to generate singlet oxygen,and thus induced the rapid degradation of rhodamine B,methylene blue,orange Ⅱ,phenol and 4-chlorophenol.The use of0.1 g/L of the Cu^0/Fe3O4 composites induced the complete removal of rhodamine B（20 μmol/L） in15 min,methylene blue（20 μmol/L） in 5 min,orange Ⅱ（20 μmol/L） in 10 min,phenol（0.1mmol/L） in 30 min and 4-chlorophenol（0.1 mmol/L） in 15 min with an initial pH value of 7.0 and a PMS concentration of 0.5 mmol/L.The total organic carbon（TOC） removal higher than 85%for all of these five pollutants was obtained in 30 min when the PMS concentration was 2.5 mmol/L.The rate of degradation was considerably higher than that obtained with Cu^0 or Fe3O4 particles alone.The enhanced catalytic activity of the Cu^0/Fe3O4 composites in the activation of PMS was attributed to the synergistic effect of the Cu^0 and Fe3O4 crystals in the composites.Singlet oxygen was identified as the primary reactive oxygen species responsible for pollutant degradation by electron spin resonance and radical quenching experiments.A possible mechanism for the activation of PMS by Cu^0/Fe3O4 composites is proposed as electron transfer from the organic pollutants to PMS induces the activation of PMS to generate ^1O2,which induces the degradation of the organic pollutants.As a magnetic catalyst,the Cu^0/Fe3O4 composites were easily recovered by magnetic separation,and exhibited excellent stability over five successive degradation cycles.The present study provides a facile and green heterogeneous catalysis method for the oxidative removal of organic pollutants.展开更多
以PEG4000和(NH_4)2SO_4为双水相体系、二异丙胺为沉淀剂,对共沉淀法进行改进,合成了四氧化三铁(Fe_3O_4)纳米粒子。采用XRD、TEM、VSM、FT-IR等对Fe_3O_4进行性能表征,证明所合成的Fe_3O_4粒子为具有反尖晶石结构、稳定性和分散性良好...以PEG4000和(NH_4)2SO_4为双水相体系、二异丙胺为沉淀剂,对共沉淀法进行改进,合成了四氧化三铁(Fe_3O_4)纳米粒子。采用XRD、TEM、VSM、FT-IR等对Fe_3O_4进行性能表征,证明所合成的Fe_3O_4粒子为具有反尖晶石结构、稳定性和分散性良好、尺寸均一、粒径大小为11 nm左右的球形纳米粒子,具备优异的超顺磁性和高磁化强度等特性。同时对反应温度及铁离子浓度比、PEG4000/(NH_4)2SO_4的质量浓度对双水相体系的形成进行条件探索,确定了最优工艺方案为n(Fe2+)∶n(Fe3+)=2∶3、1.0 g Fe Cl2·4H2O、1.2 g Fe Cl3、10 m L二异丙胺,PEG4000/(NH_4)2SO_4双水相体系中PEG4000的质量分数为18%、(NH_4)2SO_4的质量分数为25%,反应温度为60℃,反应时间为1 h。展开更多
基金supported by the National Natural Science Foundation of China (21377169, 21507168)the Fundamental Research Funds for the Central Universities (CZW15078)the Natural Science Foundation of Hubei Province of China (2014CFC1119, 2015CFB505)~~
文摘Magnetic Cu^0/Fe3O4 submicron composites were prepared using a hydrothermal method and used as heterogeneous catalysts for the activation of peroxymonosulfate（PMS） and the degradation of organic pollutants.The as-prepared magnetic Cu^0/Fe3O4 submicron composites were composed of Cu^0 and Fe3O4 crystals and had an average size of approximately 220 nm.The Cu^0/Fe3O4 composites could efficiently catalyze the activation of PMS to generate singlet oxygen,and thus induced the rapid degradation of rhodamine B,methylene blue,orange Ⅱ,phenol and 4-chlorophenol.The use of0.1 g/L of the Cu^0/Fe3O4 composites induced the complete removal of rhodamine B（20 μmol/L） in15 min,methylene blue（20 μmol/L） in 5 min,orange Ⅱ（20 μmol/L） in 10 min,phenol（0.1mmol/L） in 30 min and 4-chlorophenol（0.1 mmol/L） in 15 min with an initial pH value of 7.0 and a PMS concentration of 0.5 mmol/L.The total organic carbon（TOC） removal higher than 85%for all of these five pollutants was obtained in 30 min when the PMS concentration was 2.5 mmol/L.The rate of degradation was considerably higher than that obtained with Cu^0 or Fe3O4 particles alone.The enhanced catalytic activity of the Cu^0/Fe3O4 composites in the activation of PMS was attributed to the synergistic effect of the Cu^0 and Fe3O4 crystals in the composites.Singlet oxygen was identified as the primary reactive oxygen species responsible for pollutant degradation by electron spin resonance and radical quenching experiments.A possible mechanism for the activation of PMS by Cu^0/Fe3O4 composites is proposed as electron transfer from the organic pollutants to PMS induces the activation of PMS to generate ^1O2,which induces the degradation of the organic pollutants.As a magnetic catalyst,the Cu^0/Fe3O4 composites were easily recovered by magnetic separation,and exhibited excellent stability over five successive degradation cycles.The present study provides a facile and green heterogeneous catalysis method for the oxidative removal of organic pollutants.
基金supported by National 863 Program Emphasis Project (Nanometer Biology Ware Study, No.2007AA0222006)National Natural Science Foundation of P.R. China(No.30740062 and No.30872970)High School Doctor Subjec Special-purpose Scientific Research Foundation(No.20070286042)
文摘以PEG4000和(NH_4)2SO_4为双水相体系、二异丙胺为沉淀剂,对共沉淀法进行改进,合成了四氧化三铁(Fe_3O_4)纳米粒子。采用XRD、TEM、VSM、FT-IR等对Fe_3O_4进行性能表征,证明所合成的Fe_3O_4粒子为具有反尖晶石结构、稳定性和分散性良好、尺寸均一、粒径大小为11 nm左右的球形纳米粒子,具备优异的超顺磁性和高磁化强度等特性。同时对反应温度及铁离子浓度比、PEG4000/(NH_4)2SO_4的质量浓度对双水相体系的形成进行条件探索,确定了最优工艺方案为n(Fe2+)∶n(Fe3+)=2∶3、1.0 g Fe Cl2·4H2O、1.2 g Fe Cl3、10 m L二异丙胺,PEG4000/(NH_4)2SO_4双水相体系中PEG4000的质量分数为18%、(NH_4)2SO_4的质量分数为25%,反应温度为60℃,反应时间为1 h。
