Dramatically Enhanced Aerobic Atrazine Degradation with Fe@Fe2O3 Core-Shell Nanowires by Tetrapolyphosphate

被引:184
作者
Wang, Li [1 ]
Cao, Menghua [1 ]
Ai, Zhihui [1 ]
Zhang, Lizhi [1 ]
机构
[1] Cent China Normal Univ, Inst Environm Chem, Minist Educ, Key Lab Pesticide & Chem Biol, Wuhan 430079, Peoples R China
基金
美国国家科学基金会;
关键词
ZERO-VALENT IRON; PHOSPHATE ADSORPTION; HYDROGEN-PEROXIDE; HYDROXYL RADICALS; ATR-FTIR; AQUEOUS-SOLUTION; OXYGEN; OXIDATION; TIO2; GENERATION;
D O I
10.1021/es404741x
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
In this study, the effects of an inorganic ligand tetrapolyphosphate on the molecular oxygen activation and the subsequent aerobic atrazine degradation by Fe@Fe2O3 core-shell nanowires were investigated systematically at a circum-neutral to alkaline pH range (pH 6.0-9.0). We interestingly found that the addition of tetrapolyphosphate could enhance the aerobic atrazine degradation rate 955 times, which was even 10 times that of the traditional organic ligand ethylenediamine tetraacetate. This tetrapolyphosphate induced dramatic aerobic atrazine degradation enhancement could be attributed to two factors. One was that the presence of tetrapolyphosphate strongly suppressed hydrogen evolution from the reduction of proton by Fe@Fe2O3 core shell nanowires through proton confinement, leaving over more electrons for the reduction of Fe(III) to Fe(II) and the subsequent molecular oxygen activation. The other was that the complexation of tetrapolyphosphate with ferrous ions not only guaranteed enough soluble Fe(II) for Fenton reaction, but also provided another route to produce more center dot OH in the solution via the single-electron molecular oxygen reduction pathway. We employed gas chromatography-mass spectrometry and liquid chromatography-mass spectrometry to identify the atrazine degradation intermediates and proposed a possible aerobic atrazine degradation pathway. This study not only sheds light on the promotion effects of ligands on the molecular oxygen activation by nanoscale zerovalent iron, but also offers a facile and green iron-based method for the oxidative atrazine removal.
引用
收藏
页码:3354 / 3362
页数:9
相关论文
共 46 条
[1]   Polyphosphate - an ancient energy source and active metabolic regulator [J].
Achbergerova, Lucia ;
Nahalka, Jozef .
MICROBIAL CELL FACTORIES, 2011, 10
[2]   Reduction of nitro aromatic compounds by zero-valent iron metal [J].
Agrawal, A ;
Tratnyek, PG .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 1996, 30 (01) :153-160
[3]   Core-Shell Structure Dependent Reactivity of Fe@Fe2O3 Nanowires on Aerobic Degradation of 4-Chlorophenol [J].
Ai, Zhihui ;
Gao, Zhiting ;
Zhang, Lizhi ;
He, Weiwei ;
Yin, Jun Jie .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2013, 47 (10) :5344-5352
[4]   ATR-FTIR spectroscopic investigation on phosphate adsorption mechanisms at the ferrihydrite-water interface [J].
Arai, Y ;
Sparks, DL .
JOURNAL OF COLLOID AND INTERFACE SCIENCE, 2001, 241 (02) :317-326
[5]   DEGRADATION OF ATRAZINE BY FENTONS REAGENT - CONDITION OPTIMIZATION AND PRODUCT QUANTIFICATION [J].
ARNOLD, SM ;
HICKEY, WJ ;
HARRIS, RF .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 1995, 29 (08) :2083-2089
[6]   The generation of hydroxyl radicals in the reaction of molecular oxygen with polyphosphate complexes of ferrous ion [J].
Biaglow, JE ;
Kachur, AV .
RADIATION RESEARCH, 1997, 148 (02) :181-187
[7]   Degradation of Atrazine by Electrochemical Advanced Oxidation Processes Using a Boron-Doped Diamond Anode [J].
Borras, Nuria ;
Oliver, Ramon ;
Arias, Conchita ;
Brillas, Enric .
JOURNAL OF PHYSICAL CHEMISTRY A, 2010, 114 (24) :6613-6621
[8]   Phenol degradation using hydroxyl radicals generated from zero-valent iron and hydrogen peroxide [J].
Bremner, DH ;
Burgess, AE ;
Houllemare, D ;
Namkung, KC .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2006, 63 (1-2) :15-19
[9]   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
[10]   Multiple Proton Confinement in the M2 Channel from the Influenza A Virus [J].
Carnevale, Vincenzo ;
Fiorin, Giacomo ;
Levine, Benjamin G. ;
DeGrado, William F. ;
Klein, Michael L. .
JOURNAL OF PHYSICAL CHEMISTRY C, 2010, 114 (48) :20856-20863