A novel heterogeneous system for sulfate radical generation through sulfite activation on a CoFe2O4 nanocatalyst surface

被引:209
作者
Liu, Zizheng [1 ]
Yang, Shaojie [2 ]
Yuan, Yanan [2 ]
Xu, Jing [2 ]
Zhu, Yifan [2 ]
Li, Jinjun [2 ]
Wu, Feng [2 ]
机构
[1] Wuhan Univ, Sch Civil Engn, Wuhan 430072, Peoples R China
[2] Wuhan Univ, Sch Resources & Environm Sci, Dept Environm Sci, Hubei Key Lab Biomass Resource Chem & Environm Bi, Wuhan 430079, Peoples R China
基金
中国国家自然科学基金;
关键词
CoFe2O4; nanocatalyst; Sulfite; Metoprolol; Oxysulfur radical; Alkaline pH; HIGHLY EFFICIENT CATALYSTS; SUPPORTED COBALT OXIDE; ACID ORANGE 7; INDUCED AUTOXIDATION; AQUEOUS-SOLUTION; RATE CONSTANTS; DEGRADATION; OXIDATION; PEROXYMONOSULFATE; MECHANISM;
D O I
10.1016/j.jhazmat.2016.11.029
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Heterogeneous catalytic activation is important for potential application of new sulfate-radical based advanced oxidation process using sulfite as source of sulfate radical. We report herein a heterogeneous system for sulfite activation by CoFe2O4 nanocatalyst for metoprolol removal. Factors that influence metoprolol removal were investigated, including pH and initial concentrations of components. The CoFe2O4 nanocatalyst was characterized by X-ray diffractometry (XRD) and transmission electron microscopy (TEM), and the catalytic stability was tested by consecutive runs. Radicals generated in the CoFe2O4-S(IV)-O-2 system were identified through radical quenching experiments and by electron spin resonance (ESR). The catalytic mechanism was elucidated further by X-ray photoelectron spectroscopy (XPS). The catalytic process was dependent on initial pH, and more than 80% of the metoprolol can be removed at pH 10.0 following the Langmubir-Hinshelwood equation. The generation of Co-OH complexes on the CoFe2O4 surface was crucial for sulfite activation. SO4 center dot- was verified to be the main oxidative species responsible for metoprolol degradation. Other organic pollutants, such as sulfanilamide, sulfasalazine, 2-nitroaniline, sulfapyridine, aniline, azo dye X-3B and 4-chloroaniline, could also be removed in this CoFe2O4 S(IV)-O-2 system. The results suggest that the CoFe2O4 S(IV)-O-2 system has good application prospects in alkaline organic wastewater treatment. (C) 2016 Elsevier B.V. All rights reserved.
引用
收藏
页码:583 / 592
页数:10
相关论文
共 55 条
[1]   Photocatalytic degradation of metoprolol tartrate in suspensions of two TiO2-based photocatalysts with different surface area. Identification of intermediates and proposal of degradation pathways [J].
Abramovic, Biljana ;
Kler, Sanja ;
Sojic, Daniela ;
Lausevic, Mila ;
Radovic, Tanja ;
Vione, Davide .
JOURNAL OF HAZARDOUS MATERIALS, 2011, 198 :123-132
[2]   REACTIONS OF HYDROXYL RADICAL .1. TRANSIENT SPECTRA OF SOME INORGANIC RADICAL-ANIONS [J].
ADAMS, GE ;
BOAG, JW ;
MICHAEL, BD .
TRANSACTIONS OF THE FARADAY SOCIETY, 1965, 61 (512P) :1674-&
[3]   Transition metal/UV-based advanced oxidation technologies for water decontamination [J].
Anipsitakis, GP ;
Dionysiou, DD .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2004, 54 (03) :155-163
[4]   Degradation of organic contaminants in water with sulfate radicals generated by the conjunction of peroxymonosulfate with cobalt [J].
Anipsitakis, GP ;
Dionysiou, DD .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2003, 37 (20) :4790-4797
[5]   Heterogeneous activation of oxone using Co3O4 [J].
Anipsitakis, GP ;
Stathatos, E ;
Dionysiou, DD .
JOURNAL OF PHYSICAL CHEMISTRY B, 2005, 109 (27) :13052-13055
[6]   Radical generation by the interaction of transition metals with common oxidants [J].
Anipsitakis, GP ;
Dionysiou, DD .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2004, 38 (13) :3705-3712
[7]   Degradation of microcystin-LR using sulfate radicals generated through photolysis, thermolysis and e- transfer mechanisms [J].
Antoniou, Maria G. ;
de la Cruz, Armah A. ;
Dionysiou, Dionysios D. .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2010, 96 (3-4) :290-298
[8]   Ultrasound enhanced heterogeneous activation of peroxymonosulfate by a bimetallic Fe-Co/SBA-15 catalyst for the degradation of Orange II in water [J].
Cai, Chun ;
Zhang, Hui ;
Zhong, Xing ;
Hou, Liwei .
JOURNAL OF HAZARDOUS MATERIALS, 2015, 283 :70-79
[9]   Decolorization of Orange II in Aqueous Solution by an Fe(II)/sulfite System: Replacement of Persulfate [J].
Chen, Long ;
Peng, Xinzi ;
Liu, Jihao ;
Li, Jinjun ;
Wu, Feng .
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 2012, 51 (42) :13632-13638
[10]   THE SYNERGISTIC EFFECT OF MANGANESE(II) IN THE SULFITE-INDUCED AUTOXIDATION OF METAL-IONS AND COMPLEXES IN AQUEOUS-SOLUTION [J].
COICHEV, N ;
REDDY, KB ;
VANELDIK, R .
ATMOSPHERIC ENVIRONMENT PART A-GENERAL TOPICS, 1992, 26 (13) :2295-2300