Identification of by-products and toxicity assessment in aqueous-phase hydrodechlorination of diuron with palladium on activated carbon catalysts

被引:16
作者
Al Bahri, M. [1 ]
Calvo, L. [1 ]
Polo, A. M. [1 ]
Gilarranz, M. A. [1 ]
Mohedano, A. F. [1 ]
Rodriguez, J. J. [1 ]
机构
[1] Univ Autonoma Madrid, Secc Dept Ingn Quim, E-28049 Madrid, Spain
关键词
Hydrodechlorination; Diuron; Activated carbon; Pd catalyst; Ecotoxicity; Biodegradability; BIOLOGICAL TREATMENT; PHOTO-FENTON; WATER; SLUDGE; PD; MINERALIZATION; TEMPERATURE; PESTICIDES; HERBICIDES; OXIDATION;
D O I
10.1016/j.chemosphere.2013.02.065
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
The hydrodechlorination (HDC) of diuron in aqueous phase with hydrogen using two different activated carbon-supported Pd catalysts was studied. A commercial activated carbon and one prepared by chemical activation of grape seeds with phosphoric acid (GS) were evaluated as supports, being the catalysts tested in a wide range of temperature (30-100 degrees C) and space-time (78-311 kg(cat) h mol(-1)). Diuron conversion was above 70% under all the conditions tested. The Pd catalyst supported on GS showed the highest activity in terms of diuron conversion within the temperature range studied, allowing nearly complete conversion above 50 degrees C. However, a gradual loss of activity with time was observed for this catalyst. A complete route of hydrogenation of diuron was elucidated. Two reaction routes one leading to fenuron and another to aniline were identified. As the temperature and space-time were increased, the formation of fenuron (via monuron) was found to be favored. The toxicity of the reaction products was evaluated, being the route to fenuron and monuron, the one giving rise to a significant decrease of ecotoxicity. (C) 2013 Elsevier Ltd. All rights reserved.
引用
收藏
页码:1317 / 1323
页数:7
相关论文
共 37 条
[1]   The effects of different activated carbon supports and support modifications on the properties of Pt/AC catalysts [J].
Aksoylu, AE ;
Madalena, M ;
Freitas, A ;
Pereira, MFR ;
Figueiredo, JL .
CARBON, 2001, 39 (02) :175-185
[2]   Activated carbon from grape seeds upon chemical activation with phosphoric acid: Application to the adsorption of diuron from water [J].
Al Bahri, M. ;
Calvo, L. ;
Gilarranz, M. A. ;
Rodriguez, J. J. .
CHEMICAL ENGINEERING JOURNAL, 2012, 203 :348-356
[3]   Toxicity of 58 substituted anilines and phenols to algae Pseudokirchneriella subcapitata and bacteria Vibrio fischeri: Comparison with published data and QSARs [J].
Aruoja, Villem ;
Sihtmaee, Mariliis ;
Dubourguier, Henri-Charles ;
Kahru, Anne .
CHEMOSPHERE, 2011, 84 (10) :1310-1320
[4]   Use of the ciliated protozoan Tetrahymena pyriformis for the assessment of toxicity and quantitative structure-activity relationships of xenobiotics:: Comparison with the Microtox test [J].
Bogaerts, P ;
Bohatier, J ;
Bonnemoy, F .
ECOTOXICOLOGY AND ENVIRONMENTAL SAFETY, 2001, 49 (03) :293-301
[5]   Piggery wastewater characterisation for biological nitrogen removal process design [J].
Boursier, H ;
Béline, F ;
Paul, E .
BIORESOURCE TECHNOLOGY, 2005, 96 (03) :351-358
[6]   Identification of activated sludge and wastewater characteristics using respirometric batch-experiments [J].
Brouwer, H ;
Klapwijk, A ;
Keesman, KJ .
WATER RESEARCH, 1998, 32 (04) :1240-1254
[7]   Hydrodechlorination of alachlor in water using Pd, Ni and Cu catalysts supported on activated carbon [J].
Calvo, L. ;
Gilarranz, M. A. ;
Casas, J. A. ;
Mohedano, A. F. ;
Rodriguez, J. J. .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2008, 78 (3-4) :259-266
[8]   Hydrodechlorination of 4-chlorophenol in aqueous phase using Pd/AC catalysts prepared with modified active carbon supports [J].
Calvo, L. ;
Gilarranz, M. A. ;
Casas, J. A. ;
Mohedano, A. F. ;
Rodriguez, J. J. .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2006, 67 (1-2) :68-76
[9]   Hydrodechlorination of diuron in aqueous solution with Pd, Cu and Ni on activated carbon catalysts [J].
Calvo, L. ;
Gilarranz, M. A. ;
Casas, J. A. ;
Mohedano, A. F. ;
Rodriguez, J. J. .
CHEMICAL ENGINEERING JOURNAL, 2010, 163 (03) :212-218
[10]   Pesticides in Portuguese surface and ground waters [J].
Cerejeira, MJ ;
Viana, P ;
Batista, S ;
Pereira, T ;
Silva, E ;
Valério, MJ ;
Silva, A ;
Ferreira, M ;
Silva-Fernandes, AM .
WATER RESEARCH, 2003, 37 (05) :1055-1063