Rapid Destruction of Tetrabromobisphenol A by Iron(III)-Tetraamidomacrocyclic Ligand/Layered Double Hydroxide Composite/H2O2 System

被引:66
作者
Wang, Chao [1 ]
Gao, Juan [2 ]
Gu, Cheng [1 ]
机构
[1] Nanjing Univ, Sch Environm, State Key Lab Pollut Control & Resource Reuse, Nanjing 210023, Jiangsu, Peoples R China
[2] Chinese Acad Sci, Inst Soil Sci, Key Lab Soil Environm & Pollut Remediat, Nanjing 210008, Jiangsu, Peoples R China
基金
美国国家科学基金会;
关键词
LAYERED DOUBLE HYDROXIDES; BROMINATED FLAME RETARDANTS; OXIDATIVE-DEGRADATION; TOXICITY; KINETICS; TBBPA; IMMOBILIZATION; CATALYST; PRODUCTS; DESIGN;
D O I
10.1021/acs.est.6b04294
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Iron(III)-tetraamidomacrocyclic ligand (Fe(III)-TAIVIL) activators have received widespread attentions for their abilities to activate hydrogen peroxide to oxidize many organic pollutants. In this study, Fe(III)-TAML/layered double hydroxide (LDH) composite was developed by intercalating Fe(III)-TAML into the interlayer of LDH. Electrostatic interaction and hydrogen bonding might account for the adsorption of Fe(III)-TAML on LDH. The newly synthesized Fe(III)-TAML/LDH composite showed superior reactivity as indicated by efficient decomposition of tetrabromobisphenol A (TBBPA) in the presence of hydrogen peroxide, which can be fully degraded within 20 s and the degradation rate increased up to 8 times compared to free Fe(III)-TAML. In addition, the toxicity of the system was significantly reduced after the reaction. The higher reactivity of Fe(III)-TAML/LDH system is attributed to the enhanced adsorption of TBBPA on LDH, which could increase the contact possibility between Fe(III)-TAML and TBBPA. On the basis of the analysis of reaction intermediates, beta-scission at the middle carbon atom and C-Br bond cleavage in phenyl ring of TBBPA were involved in the degradation process. Furthermore, our results demonstrated that the Fe(III)-TAME/LDH composite can be reused several times, which could lower the overall cost for environmental implication and render Fe(III)-TAML/LDH as the potential environmentally friendly catalyst for future wastewater treatment under mild reaction conditions.
引用
收藏
页码:488 / 496
页数:9
相关论文
共 64 条
[1]   An overview of commercially used brominated flame retardants, their applications, their use patterns in different countries/regions and possible modes of release [J].
Alaee, M ;
Arias, P ;
Sjödin, A ;
Bergman, Å .
ENVIRONMENT INTERNATIONAL, 2003, 29 (06) :683-689
[2]   DENSITY-FUNCTIONAL THERMOCHEMISTRY .3. THE ROLE OF EXACT EXCHANGE [J].
BECKE, AD .
JOURNAL OF CHEMICAL PHYSICS, 1993, 98 (07) :5648-5652
[3]   Brominated flame retardants: Cause for concern? [J].
Birnbaum, LS ;
Staskal, DF .
ENVIRONMENTAL HEALTH PERSPECTIVES, 2004, 112 (01) :9-17
[4]   Effect of solute concentration on sorption of polyaromatic hydrocarbons in soil: Uptake rates [J].
Braida, WJ ;
White, JC ;
Ferrandino, FJ ;
Pignatello, JJ .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2001, 35 (13) :2765-2772
[5]   New multiresidue analytical method dedicated to trace level measurement of brominated flame retardants in human biological matrices [J].
Cariou, R ;
Antignac, JP ;
Marchand, P ;
Berrebi, A ;
Zalko, D ;
Andre, F ;
Le Bizec, B .
JOURNAL OF CHROMATOGRAPHY A, 2005, 1100 (02) :144-152
[6]   FeIII-TAML-catalyzed green oxidative degradation of the azo dye Orange II by H2O2 and organic peroxides:: products, toxicity, kinetics, and mechanisms [J].
Chahbane, Naima ;
Popescu, Delia-Laura ;
Mitchell, Douglas A. ;
Chanda, Arani ;
Lenoir, Dieter ;
Ryabov, Alexander D. ;
Schramm, Karl-Werner ;
Collins, Terrence J. .
GREEN CHEMISTRY, 2007, 9 (01) :49-57
[7]   Total degradation of fenitrothion and other organophosphorus pesticides by catalytic oxidation employing Fe-TAML peroxide activators [J].
Chanda, Arani ;
Khetan, Sushil K. ;
Banerjee, Deboshri ;
Ghosh, Anindya ;
Collins, Terrence J. .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2006, 128 (37) :12058-12059
[8]   Probing the surface acidity of lithium aluminium and magnesium aluminium layered double hydroxides [J].
Chisem, IC ;
Jones, W ;
Martin, I ;
Martin, C ;
Rives, V .
JOURNAL OF MATERIALS CHEMISTRY, 1998, 8 (08) :1917-1925
[9]   BASIC PROPERTIES OF MG1-X(2+)ALX(3+) LAYERED DOUBLE HYDROXIDES INTERCALATED BY CARBONATE, HYDROXIDE CHLORIDE AND SULFATE ANIONS [J].
CONSTANTINO, VRL ;
PINNAVAIA, TJ .
INORGANIC CHEMISTRY, 1995, 34 (04) :883-892
[10]   Analytical and environmental aspects of the flame retardant tetrabromobisphenol-A and its derivatives [J].
Covaci, Adrian ;
Voorspoels, Stefan ;
Abdallah, Mohamed Abou-Elwafa ;
Geens, Tinne ;
Harrad, Stuart ;
Law, Robin J. .
JOURNAL OF CHROMATOGRAPHY A, 2009, 1216 (03) :346-363