Degradation efficiency of atrazine by Fe(VI)/Na2SO3 system
SUN Shao-fang1,2, LI Jia-long1,2, QIU Qi3, QIU Li-ping1,2, MA Jun4, LIU Cai-hong5
1. School of Civil Engineering and Architecture, University of Jinan, Jinan 250022, China; 2. Shandong Province Engineering Technology Research Center for Water Purification Functional Material, Jinan 250022, China; 3. School of Conservancy and Environment, University of Jinan, Jinan 250022, China; 4. School of Environment, Harbin Institute of Technology, Harbin 150090, China; 5. College of Environment and Ecology, Chongqing University, Chongqing 400044, China
Abstract:The degradation efficiency of atrazine (ATZ) by Na2SO3 activated with potassium ferrate (K2FeO4) was studied. The primary reactive species formed in Fe(VI)/sulfite system were identified. In addition, the influences of dosages of sulfite, solution pH as well as water background matrices including humic acid (HA), Cl-, and CO32- on the transformation efficiency of ATZ in Fe(VI)/sulfite process were evaluated. The results showed that 74.4% of ATZ was transformed by the combination of 50μmol/L Fe(VI) and 200μmol/L Na2SO3 at 10s, while only 10.2% and 7.5% of ATZ was removed at 60s by individual Fe(VI) and Na2SO3, respectively, under similar conditions. Sulfate radicals (SO4·-) was responsible for the degradation of ATZ based on the results of radical probe compound and dissolved oxygen experiments. In the presence of 50μmol/L Fe(VI) and at pH=8, the degradation efficacy of ATZ firstly increased, then decreased with increasing the dosage of Na2SO3, in which the optimal concentration of Na2SO3 was 150~200μmol/L. The enhanced degradation of ATZ by Fe(Ⅵ)/Na2SO3 system was observed in the pH range of 7~10. The removal of ATZ in natural water by Fe(VI)/sulfite process was also confirmed, but with lower efficiency compared to synthetic water, mainly resulting from the competition of SO4·- by water background matrix.
杨梅,林忠胜,姚子伟,等.三嗪类除草剂莠去津的研究进展[J]. 农药科学与管理, 2006,27(11):31-37. Yang Mei, Lin Zhongsheng, Yao Ziwei, et al. Research progress of the herbicide atrazine[J]. Journal of Pesticide Science and Management, 2006,27(11):31-37.
[2]
GB3838-2002地表水环境质量标准[S]. GB3838-2002 Environmental quality standards for surface water[S].
[3]
杨晓燕.固定化阿特拉津降解菌-藻体系的构建及去除水体中阿特拉津的研究[D]. 北京:中国农业科学院, 2018. Yang Xiaoyan. Construction of immobilized atrazine-degrading bacteria-algae system and study on removal of atrazine in water[D]. Beijing:Chinese Academy of Agricultural Sciences, 2018.
[4]
Chen H, Bramanti E, Longo I, et al. Oxidative decomposition of atrazine in water in the presence of hydrogen peroxide using an innovative microwave photochemical reactor[J]. Journal of Hazardous Materials, 2011,186(2/3):1808-1817.
[5]
Yin L, Warne M, Lim P. Toxicity and bioavailability of atrazine and molinate to the freshwater fish (melanotenia fluviatilis) under laboratory and simulated field conditions[J]. Science of the Total Environment, 2006,356(1/3):86-99.
[6]
史伟,李香菊,张宏军.除草剂莠去津对环境的污染及治理[J]. 农药科学与管理, 2009,30(8):30-35. Shi Wei, Li Xiangju, Zhang Hongjun. Environment and contamination of atrazine[J]. Journal of Pesticide Science and Management, 2009,30(8):30-35.
[7]
Tugba H, Idil A. Comparison of sulfate and hydroxyl radical based advanced oxidation of phenol[J]. Chemical Engineering Journal, 2013,224:10-16.
[8]
Lutze H, Bircher S, Rapp I, et al. Degradation of chlorotriazine pesticides by sulfate radicals and the influence of organic matter[J]. Environmental Science & Technology, 2015,49:1673-1680.
[9]
Hong Y, Peng J, Zhao X, et al. Efficient degradation of atrazine by CoMgAl layered double oxides catalyzed peroxymonosulfate:Optimization, degradation pathways and mechanism[J]. Chemical Engineering Journal, 2019,370:354-363.
[10]
Yang Y, Jiang J, Lv X, et al. Production of sulfate radical and hydroxyl radical by reaction of ozone with peroxymonosulfate:a novel advanced oxidation process[J]. Environmental Science & Technology, 2015,49(12):7330-7339.
[11]
Xie P, Zhang L, Chen J, et al. Enhanced degradation of organic contaminants by zero-valent iron/sulfite process under simulated sunlight irradiation[J]. Water Research, 2019,149:169-178.
[12]
Zhou D, Yuan Y, Yang S, et al. Roles of oxysulfur radicals in the oxidation of acid orange 7in the Fe(III)-sulfite system[J]. Journal of Sulfur Chemistry, 2015,36(4):373-384.
[13]
Thompson W, Ockerman T, Schreyer M. Preparation and purification of potassium ferrate(VI)[J]. Journal of the American Chemical Society, 1951,73(3):1379-1381.
[14]
Sun S, Pang S, Jiang J, et al. The combination of ferrate(VI) and sulfite as a novel advanced oxidation process for enhanced degradation of organic contaminants[J], Chemical Engineering Journal, 2018,333:11-19.
[15]
Gao Y, Zhou Y, Pang S, et al. Quantitative evaluation of relative contribution of high-valent iron species and sulfate radical in Fe(VI) enhanced oxidation processes via sulfur reducing agents activation[J]. Chemical Engineering Journal, 2020,387:124077.
[16]
Shao B, Dong H, Feng L, et al. Influence of[sulfite]/[Fe(VI)] molar ratio on the active oxidants generation in Fe(VI)/sulfite process[J]. Journal of Hazardous Materials, 2019,384:121303.
[17]
Zou J, Ma J, Chen L, et al. Rapid acceleration of ferrous iron/peroxymonosulfate oxidation of organic pollutants by promoting Fe(III)/Fe(II) cycle with hydroxylamine[J]. Environmental Science & Technology, 2013,47(20):11685-11693.
[18]
Ranguelova K, Rice B, Khajo A, et al.Formation of reactive sulfitederived free radicals by the activation of human neutrophils:an ESR study[J]. Free Radical Biology and Medicine, 2012,52(8):1264-1271.
[19]
Luo C, Jiang J, Ma J, et al. Oxidation of the odorous compound 2,4,6-trichloroanisole by UV activated persulfate:Kinetics, products, and pathways[J] Water Research, 2016,96:12-21.