Organic contaminants degradation from the S(IV) autoxidation process catalyzed by ferrous-manganous ions: A noticeable Mn(III) oxidation process

被引:69
作者
Zhang, Jiaming [1 ]
Ma, Jun [1 ]
Song, Haoran [1 ]
Sun, Shaofang [1 ]
Zhang, Zhongxiang [1 ]
Yang, Tao [1 ]
机构
[1] Harbin Inst Technol, State Key Lab Urban Water Resource & Environm, Harbin 150090, Heilongjiang, Peoples R China
基金
中国国家自然科学基金;
关键词
Fe2+-Mn2+ catalysis process; Mn(III) oxidation; Sulfur radicals; Atrazine; Acetylation degradation pathway; DISSOLVED SULFUR-DIOXIDE; ELECTRON REDOX REACTIONS; AQUEOUS-SOLUTION; SPECTROPHOTOMETRIC DETERMINATION; FENTONS REAGENT; INORGANIC-IONS; KINETICS; MECHANISM; ATRAZINE; SULFITE;
D O I
10.1016/j.watres.2018.01.039
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Remarkable atrazine degradation in the S(IV) autoxidation process catalyzed by Fe2+-Mn2+ (Fe2+/Mn2+/sulfite) was demonstrated in this study. Competitive kinetic experiments, alcohol inhibiting methods and electron spin resonance (ESR) experiments proved that sulfur radicals were not the major oxidation species. Mn(III) was demonstrated to be the primary active species in the Fe2+/Mn(2+/)sulfite process based on the comparison of oxidation selectivity. Moreover, the inhibiting effect of the Mn(III) hydrolysis and the S(IV) autoxidation in the presence of organic contaminants indicated the existence of three Mn(III) consumption routes in the Fe2+/Mn2+/sulfite process. The absence of hydroxyl radical and sulfate radical was interpreted by the competitive dynamics method. The oxidation capacity of the Fe2+/Mn2+/sulfite was independent of the initial pH (4.0-6.0) because the fast decay of S(IV) decreased initial pH below 4.0 rapidly. The rate of ATZ degradation was independent of the dissolved oxygen (DO) because that the major DO consumption process was not the rate determining step during the production of SO5 center dot-. Phosphate and bicarbonate were confirmed to have greater inhibitory effects than other environmental factors because of their strong pH buffering capacity and complexing capacity for Fe3+. The proposed acetylation degradation pathway of ATZ showed the application of the Fe2+/Mn2+/sulfite process in the research of contaminants degradation pathways. This work investigated the characteristics of the Fe2+/Mn2+/sulfite process in the presence of organic contaminants, which might promote the development of Mn(III) oxidation technology. (C) 2018 Published by Elsevier Ltd.
引用
收藏
页码:227 / 235
页数:9
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]   Sulfate radical anion oxidation of diclofenac and sulfamethoxazole for water decontamination [J].
Ahmed, Moussa Mahdi ;
Barbati, Stephane ;
Doumenq, Pierre ;
Chiron, Serge .
CHEMICAL ENGINEERING JOURNAL, 2012, 197 :440-447
[3]   KINETICS AND MECHANISM FOR MANGANESE-CATALYZED OXIDATION OF SULFUR(IV) BY OXYGEN IN AQUEOUS-SOLUTION [J].
BERGLUND, J ;
FRONAEUS, S ;
ELDING, LI .
INORGANIC CHEMISTRY, 1993, 32 (21) :4527-4538
[4]   MANGANESE-CATALYZED AUTOXIDATION OF DISSOLVED SULFUR-DIOXIDE IN THE ATMOSPHERIC AQUEOUS-PHASE [J].
BERGLUND, J ;
ELDING, LI .
ATMOSPHERIC ENVIRONMENT, 1995, 29 (12) :1379-1391
[5]  
Biedermann G., 1978, ACTA CHEM SCAND A, V32
[6]   KINETICS AND MECHANISM OF THE IRON(III)-CATALYZED AUTOXIDATION OF SULFUR(IV) OXIDES IN AQUEOUS-SOLUTION - EVIDENCE FOR THE REDOX CYCLING OF IRON IN THE PRESENCE OF OXYGEN AND MODELING OF THE OVERALL REACTION-MECHANISM [J].
BRANDT, C ;
FABIAN, I ;
VANELDIK, R .
INORGANIC CHEMISTRY, 1994, 33 (04) :687-701
[7]   Kinetics and mechanism of the oxidation of HSO3- by O-2 .2. The manganese(II)-catalyzed reaction [J].
Connick, RE ;
Zhang, YX .
INORGANIC CHEMISTRY, 1996, 35 (16) :4613-4621
[8]   Iron-manganese redox processes and synergism in the mechanism for manganese-catalyzed autoxidation of hydrogen sulfite [J].
Fronaeus, S ;
Berglund, J ;
Elding, LI .
INORGANIC CHEMISTRY, 1998, 37 (19) :4939-4944
[9]   Unrecognized role of bisulfite as Mn(III) stabilizing agent in activating permanganate (Mn(VII)) for enhanced degradation of organic contaminants [J].
Gao, Yuan ;
Jiang, Jin ;
Zhou, Yang ;
Pang, Su-Yan ;
Ma, Jun ;
Jiang, Chengchun ;
Wang, Zhen ;
Wang, Pan-Xin ;
Wang, Li-Hong ;
Li, Juan .
CHEMICAL ENGINEERING JOURNAL, 2017, 327 :418-422
[10]   AQUEOUS S(IV) OXIDATION .1. CATALYTIC EFFECTS OF SOME METAL-IONS [J].
GRGIC, I ;
HUDNIK, V ;
BIZJAK, M ;
LEVEC, J .
ATMOSPHERIC ENVIRONMENT PART A-GENERAL TOPICS, 1991, 25 (08) :1591-1597