Efficient degradation of atrazine by magnetic porous copper ferrite catalyzed peroxymonosulfate oxidation via the formation of hydroxyl and sulfate radicals

被引:951
作者
Guan, Ying-Hong [1 ,3 ]
Ma, Jun [1 ]
Ren, Yue-Ming [2 ]
Liu, Yu-Lei [1 ]
Xiao, Jia-Yue [1 ]
Lin, Ling-qiang [2 ]
Zhang, Chen [2 ]
机构
[1] Harbin Inst Technol, State Key Lab Urban Water Resource & Environm, Harbin 150090, Peoples R China
[2] Harbin Engn Univ, Key Lab Superlight Mat & Surface Technol, Minist Educ, Coll Mat Sci & Chem Engn, Harbin 150008, Peoples R China
[3] Northeast Agr Univ, Sch Water Conservancy & Construct, Harbin 150030, Peoples R China
关键词
Sulfate radical; Hydroxyl radical; Peroxymonosulfate; Copper ferrite; Atrazine; Oxone; HYDROGEN-PEROXIDE; RATE CONSTANTS; ACTIVATION; OZONATION; DECOMPOSITION; PERSULFATE; KINETICS; ACID; PH; MECHANISMS;
D O I
10.1016/j.watres.2013.06.023
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Magnetic porous copper ferrite (CuFe2O4) showed a notable catalytic activity to peroxymonosulfate (PMS). More than 98% of atrazine was degraded within 15 min at 1 mM PMS and 0.1 g/L CuFe2O4. In contrast, CuFe2O4 exhibited no obvious catalytic activity to peroxodisulfate or H2O2. Several factors affecting the catalytic performance of PMS/CuFe2O4 were investigated. Results showed that the catalytic degradation efficiency of atrazine increased with PMS and CuFe2O4 doses, but decreased with the increase of natural organic matters concentration. The catalytic oxidation also showed a dependence on initial pH. The presence of bicarbonate stimulated atrazine degradation by PMS/CuFe2O4 at low concentrations but inhibited the degradation at high concentrations. Furthermore, the reactive species for atrazine degradation in PMS/CuFe2O4 system were identified as hydroxyl radical (HO center dot) and sulfate radical (SO4 center dot-) through competition reactions of atrazine and nitrobenzene, instead of commonly used alcohol scavenging, which was not a reliable method in metal oxide catalyzed oxidation. Surface hydroxyl groups of CuFe2O4 were a critical part in radical generation and the copper on CuFe2O4 surface was an active site to catalyze PMS. The catalytic degradation of atrazine by PMS/CuFe2O4 was also effective under the background of actual waters. (C) 2013 Elsevier Ltd. All rights reserved.
引用
收藏
页码:5431 / 5438
页数:8
相关论文
共 39 条
[1]   Degradation kinetics of atrazine and its degradation products with ozone and OH radicals: A predictive tool for drinking water treatment [J].
Acero, JL ;
Stemmler, K ;
Von Gunten, U .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2000, 34 (04) :591-597
[2]   Radical generation by the interaction of transition metals with common oxidants [J].
Anipsitakis, GP ;
Dionysiou, DD .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2004, 38 (13) :3705-3712
[3]   Degradation of atrazine in aqueous medium by electrocatalytically generated hydroxyl radicals. A kinetic and mechanistic study [J].
Balci, Beytul ;
Oturan, Nihal ;
Cherrier, Richard ;
Oturan, Mehmet A. .
WATER RESEARCH, 2009, 43 (07) :1924-1934
[4]   Decolorization of synthetic dyes by hydrogen peroxide with heterogeneous catalysis by mixed iron oxides [J].
Baldrian, Petr ;
Merhautová, Vera ;
Gabriel, Jirí ;
Nerud, Frantisek ;
Stopka, Pavel ;
Hruby, Martin ;
Benes, Milan J. .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2006, 66 (3-4) :258-264
[5]   A KINETIC AND ISOTOPIC STUDY OF DECOMPOSITION OF MONOPEROXYPHTHALIC ACID [J].
BALL, RE ;
EDWARDS, JO ;
HAGGETT, ML ;
JONES, P .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1967, 89 (10) :2331-&
[6]   ATR-FTIR spectroscopic characterization of coexisting carbonate surface complexes on hematite [J].
Bargar, JR ;
Kubicki, JD ;
Reitmeyer, R ;
Davis, JA .
GEOCHIMICA ET COSMOCHIMICA ACTA, 2005, 69 (06) :1527-1542
[7]   CRITICAL-REVIEW OF RATE CONSTANTS FOR REACTIONS OF HYDRATED ELECTRONS, HYDROGEN-ATOMS AND HYDROXYL RADICALS (.OH/.O-) IN AQUEOUS-SOLUTION [J].
BUXTON, GV ;
GREENSTOCK, CL ;
HELMAN, WP ;
ROSS, AB .
JOURNAL OF PHYSICAL AND CHEMICAL REFERENCE DATA, 1988, 17 (02) :513-886
[8]   Degradation of atrazine by cobalt-mediated activation of peroxymonosulfate: Different cobalt counteranions in homogenous process and cobalt oxide catalysts in photolytic heterogeneous process [J].
Chan, K. H. ;
Chu, W. .
WATER RESEARCH, 2009, 43 (09) :2513-2521
[9]   Reduction potentials of SO3•-, SO5•-, and S4O6•3- radicals in aqueous solution [J].
Das, TN ;
Huie, RE ;
Neta, P .
JOURNAL OF PHYSICAL CHEMISTRY A, 1999, 103 (18) :3581-3588
[10]   Comparative study of the oxidation of atrazine and acetone by H2O2/UV, Fe(III)/UV, Fe(III)/H2O2/UV and Fe(II) or Fe(III)/H2O2 [J].
De Laat, J ;
Gallard, H ;
Ancelin, S ;
Legube, B .
CHEMOSPHERE, 1999, 39 (15) :2693-2706