Degradation of atrazine by ZnxCu1 - xFe2O4 nanomaterial-catalyzed sulfite under UV-vis light irradiation: Green strategy to generate SO4•-
Degradation of atrazine by ZnxCu1 - xFe2O4 nanomaterial-catalyzed sulfite under UV-vis light irradiation: Green strategy to generate SO4•-
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DOI：
10.1016/j.apcatb.2017.09.001
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发表时间：
2018-02-01
影响因子：
22.1
通讯作者：
Dionysiou, Dionysios D.
中科院分区：
文献类型：
--
作者：
Huang, Ying;Han, Changseok;Dionysiou, Dionysios D.
以ZnxCu 1-xFe 2 O 4为光催化剂，研究了紫外可见光照射下，ZnxCu 1-xFe 2 O 4光催化氧化硫酸根（SO 4中心点（-））前体亚硫酸根（SO 4）降解除草剂阿特拉津的新工艺。采用溶胶-凝胶燃烧法合成了不同Zn/Cu比的ZnxCu 1-xFe 2 O 4粉体，并用X射线粉末衍射仪、扫描电子显微镜、透射电子显微镜、孔隙率仪、紫外-可见漫反射光谱仪、振动样品磁强计和穆斯堡尔谱仪对粉体进行了表征。在本实验条件下，Zn0.8Cu0.2Fe2O4催化亚硫酸盐降解阿特拉津的能力最强。通过自由基猝灭实验和两个重要副产物（莠去津-去乙基和莠去津-去异丙基）的测定，确定了紫外可见光/Zn0.8Cu0.2Fe2O4/亚硫酸盐体系中产生的硫酸根自由基为主要反应物种。对新鲜和使用过的催化剂的XPS谱进行了分析，以进一步阐明反应机理。产生SO 4中心点（-）的可能途径有两种：光生空穴氧化亚硫酸盐和Zn_（0.8）Cu_（0.2）Fe_2 O_4表面的金属-硫化物络合物（Fe（III）-sulfito和Cu（II）-sulfito）的加速分解。根据检测到的副产物，提出了紫外可见光/Zn0.8Cu0.2Fe2O4/亚硫酸盐对阿特拉津的转化途径。在阿特拉津完全分解后，使用的催化剂可以使用磁铁磁性回收，并且没有亚硫酸盐残留在系统中。结果表明，紫外可见光/Zn 0. 8 Cu 0. 2Fe 2 O 4/亚硫酸盐体系是一种“绿色”的高级氧化技术，在废水处理中具有广阔的应用前景。
Degradation of atrazine, a widely-used herbicide, by a novel advanced oxidation process was investigated through photo-catalyzing sulfite, the precursor of sulfate radical (SO4 center dot(-)) in this study, by zinc-copper ferrites (ZnxCu1 - xFe2O4) under UV-vis light irradiation. The ZnxCu1 - xFe2O4 with different ratios of Zn to Cu was synthesized through a facile sol-gel combustion method, and characterized by X-ray powder diffractometry, scanning electron microscopy, transmission electron microscopy, porosimetry, and UV-vis diffuse reflectance spectroscopy, and by a vibrating sample magnetometer and Mossbauer spectrometer. The Zn0.8Cu0.2Fe2O4 demonstrated the highest photocatalytic ability to activate sulfite for the degradation of atrazine under current experimental conditions. The sulfate radical generated in the UV-vis light/Zn0.8Cu0.2Fe2O4/qulfite system was identified as the main reactive species through radical quenching experiments and measuring two important byproducts (atrazine-desethyl and atrazine-desisopropyl). The XPS spectra of fresh and used catalysts were analyzed to further elucidate the reaction mechanisms. There are two possible approaches to produce SO4 center dot(-): the oxidation of sulfite by photo-generated holes and the accelerated decomposition of metal-sulfito complexes (Fe (III)-sulfito and Cu(II)-sulfito) on the surface of Zn0.8Cu0.2Fe2O4. Based on the detected byproducts, the transformation pathways of atrazine by UV-vis light/Zn0.8Cu0.2Fe2O4/sulfite were proposed as well. After the complete decomposition of atrazine, the used catalysts could be magnetically recovered using a magnet and no sulfite remained in the system. The results suggest that the UV-vis light/Zn0.8Cu0.2Fe2O4/sulfite system is a "green" advanced oxidation technology for future application in wastewater treatment.