Ascorbic acid promoted magnetite Fenton degradation of alachlor: Mechanistic insights and kinetic modeling

被引:142
作者
Sun, Hongwei [1 ,2 ,3 ]
Xie, Guihong [1 ]
He, Di [4 ]
Zhang, Lizhi [1 ]
机构
[1] Cent China Normal Univ, Inst Environm & Appl Chem, Key Lab Pesticide & Chem Biol, Minist Educ,Coll Chem, Wuhan 430079, Peoples R China
[2] Pohang Univ Sci & Technol POSTECH, Dept Chem Engn, Pohang 37673, South Korea
[3] Pohang Univ Sci & Technol POSTECH, Div Environm Sci & Engn, Pohang 37673, South Korea
[4] Guangdong Univ Technol, Inst Environm & Ecol Engn, Guangdong Key Lab Environm Catalysis & Hlth Risk, Guangzhou 510006, Peoples R China
基金
中国国家自然科学基金; 中国博士后科学基金;
关键词
Ascorbic acid; Surface Fenton; Magnetite; Iron redox cycle; Kinetics; REDUCTIVE DISSOLUTION; RADICAL GENERATION; HYDROXYL RADICALS; RATE CONSTANTS; XPS SPECTRA; IRON-OXIDES; OXIDATION; CATALYSTS; SIMULATION; ANIONS;
D O I
10.1016/j.apcatb.2019.118383
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
In this study we constructed a heterogeneous Fenton system with ascorbic acid (AA), magnetite (Fe3O4) and H2O2 for the alachlor degradation, aiming to clarify the heterogeneous Fenton mechanism. The addition of AA could significantly accelerate the Fenton reaction by promoting the surface Fe(III)/Fe(II) redox cycle (iron cycle) of Fe3O4. A kinetic model was successfully developed to quantitatively describe the complicated reactions in the Fe3O4/AA/H2O2 system. We thus employed this model to identify the individual contributions of surface and homogeneous Fenton reactions to the overall alachlor degradation in the Fe3O4/AA/H2O2 system, and found the surface Fenton reaction was mainly responsible for the alachlor degradation with more than 62.6% of contribution. This work offers a new strategy to improve the heterogeneous Fenton activity via promoting surface Fenton reaction, and sheds light on the possibility to quantitatively describe and predict the heterogeneous Fenton processes with first principle kinetic models.
引用
收藏
页数:10
相关论文
共 39 条
[1]  
AFONSO MD, 1990, J COLLOID INTERF SCI, V138, P74
[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]   Oxidation reduction potential of ascorbic acid (Vitamin C) [J].
Borsook, H ;
Keighley, G .
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 1933, 19 :875-878
[4]   Electro-Fenton Process and Related Electrochemical Technologies Based on Fenton's Reaction Chemistry [J].
Brillas, Enric ;
Sires, Ignasi ;
Oturan, Mehmet A. .
CHEMICAL REVIEWS, 2009, 109 (12) :6570-6631
[5]   Antioxidant perturbations in the olfactory mucosa of alachlor-treated rats [J].
Burman, DM ;
Shertzer, HG ;
Senft, AP ;
Dalton, TP ;
Genter, MB .
BIOCHEMICAL PHARMACOLOGY, 2003, 66 (09) :1707-1715
[6]   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
[7]   Photochemistry of Hydrochar: Reactive Oxygen Species Generation and Sulfadimidine Degradation [J].
Chen, Na ;
Huang, Yahui ;
Hou, Xiaojing ;
Ai, Zhihui ;
Zhang, Lizhi .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2017, 51 (19) :11278-11287
[8]   Use of XPS in the determination of chemical environment and oxidation state of iron and sulfur samples: constitution of a data basis in binding energies for Fe and S reference compounds and applications to the evidence of surface species of an oxidized pyrite in a carbonate medium [J].
Descostes, M ;
Mercier, F ;
Thromat, N ;
Beaucaire, C ;
Gautier-Soyer, M .
APPLIED SURFACE SCIENCE, 2000, 165 (04) :288-302
[9]   pH Effects on Iron-Catalyzed Oxidation using Fenton's Reagent [J].
Duesterberg, Christopher K. ;
Mylon, Steven E. ;
Waite, T. David .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2008, 42 (22) :8522-8527
[10]   Process optimization of Fenton oxidation using kinetic modeling [J].
Duesterberg, Christopher K. ;
Waite, T. David .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2006, 40 (13) :4189-4195