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
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.
文摘用电化学方法制备Ag3PO4/Ni薄膜,以扫描电子显微镜(SEM)、X射线衍射(XRD)和紫外-可见漫反射光谱(UV-Vis DRS)对薄膜的表面形貌、晶相结构、光谱特性及能带结构进行了表征,以罗丹明B为模拟污染物对薄膜的光催化活性和稳定性进行了测定,采用向溶液中加入活性物种捕获剂的方法对薄膜光催化降解机理进行了探索。结果表明:最佳工艺下制备的Ag3PO4/Ni薄膜具有致密的层状表面结构,是由多晶纳米颗粒构成的薄膜。薄膜具有较高的光催化活性和突出的光催化稳定性,可见光下催化作用60 min,薄膜光催化罗丹明B的降解率是多孔P25 Ti O2/ITO纳米薄膜(自制)的2.3倍;在保持薄膜光催化活性基本不变的前提下可循环使用6次。给出了可见光下薄膜光催化降解罗丹明B的反应机理。
文摘采用电化学方法制备Ag3PO4/Ni薄膜,以扫描电镜(SEM)、X射线衍射(XRD)和紫外-可见漫反射光谱(UV-Vis DRS)对薄膜的表面形貌、晶相结构、光谱特性及能带结构进行表征,以罗丹明B为模拟污染物对薄膜的光电催化活性和稳定性进行测定,采用向溶液中加入活性物种捕获剂和通氮除氧方法对薄膜的光催化降解机理进行探索,并提出光电催化降解罗丹明B的反应机理。结果表明:最佳工艺下制备的Ag3PO4/Ni薄膜具有致密的层状表面结构,是由多晶纳米颗粒构成的薄膜。该薄膜具有显著的光电催化活性,在最佳阳极偏压下,光电催化罗丹明B的降解率是多孔P25 Ti O2/ITO薄膜的6.69倍;相对于未加偏压的光催化,降解率提高了5.34倍,并且具有突出的光电协同效应。同时,该薄膜具有优异的光催化和光电催化稳定性。在0.1 V阳极偏压下,可使光催化稳定性提高近一倍。