Degradation of atrazine by ZnxCu1 - xFe2O4 nanomaterial-catalyzed sulfite under UV-vis light irradiation: Green strategy to generate SO4•-

被引:231
作者
Huang, Ying [1 ]
Han, Changseok [1 ]
Liu, Yiqing [1 ]
Nadagouda, Mallikarjuna N. [2 ]
Machala, Libor [3 ]
O'Shea, Kevin E. [4 ]
Sharma, Virender K. [5 ]
Dionysiou, Dionysios D. [1 ]
机构
[1] Univ Cincinnati, Environm Engn & Sci Program, Cincinnati, OH 45221 USA
[2] Wright State Univ, Ctr Nanoscale Multifunct Mat Mech & Mat Engn, Dayton, OH 45431 USA
[3] Palacky Univ, Fac Sci, Dept Expt Phys, Reg Ctr Adv Technol & Mat, Olomouc 77146, Czech Republic
[4] Florida Int Univ, Dept Chem & Biochem, Miami, FL 33199 USA
[5] Texas A&M Univ, Program Environm & Sustainabil, Dept Environm & Occupat Hlth, Sch Publ Hlth, College Stn, TX 77843 USA
基金
美国国家科学基金会;
关键词
Sulfite; Ferrite; Sulfate radical; Atrazine; UV-vis light; SULFATE RADICALS; VISIBLE-LIGHT; ZINC FERRITE; ORANGE II; PHOTOCATALYTIC DEGRADATION; PEROXYMONOSULFATE OXIDATION; ORGANIC CONTAMINANTS; HYDROGEN-PEROXIDE; HYDROXYL RADICALS; AQUEOUS-SOLUTION;
D O I
10.1016/j.apcatb.2017.09.001
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
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.
引用
收藏
页码:380 / 392
页数:13
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