Hydrodechlorination of alachlor in water using Pd, Ni and Cu catalysts supported on activated carbon

被引:47
作者
Calvo, L. [1 ]
Gilarranz, M. A. [1 ]
Casas, J. A. [1 ]
Mohedano, A. F. [1 ]
Rodriguez, J. J. [1 ]
机构
[1] Univ Autonoma Madrid, Fac Ciencias, Secc Ingn Quim, E-28049 Madrid, Spain
关键词
hydrodechlorination; alachlor; ecotoxicity; activated carbon supported catalysts; palladium; nickel; copper; leaching;
D O I
10.1016/j.apcatb.2007.09.028
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
The hydrodechlorination of alachlor with hydrogen in aqueous phase was studied in a trickle bed reactor using different activated carbon-supported catalysts. The reactor was continuously fed with a 50 mg/L solution of alachlor in water and a H-2/N-2 gas stream. The variables studied were space-time (44.8-448.3 kg(cat) h/mol), H-2:N-2 volumetric ratio in the gas phase (1:1-1:4), temperature (308-373 K) and pressure (0.24-0.6 MPa). The results of the hydrodechlorination experiments were evaluated in terms of alachlor conversion and ecotoxicity of the exit stream. High conversion values and important reductions of ecotoxicity were obtained working under mild conditions of temperature (323-348 K) and pressure (0.24 MPa). Palladium catalysts supported on activated carbon were found as the most active in the hydrodechlorination of alachlor, although copper and nickel catalysts led also to high conversions in the 80-93% range. The hydrodechlorination of alachlor was performed successfully with metal loads between 0.5 and 2.5 wt.% on the catalysts. A significant metal leaching was observed from the nickel and copper catalysts, which negatively affected the ecotoxicity of the final effluents. Oxidative treatment of the activated carbon supports with nitric acid previous to the impregnation with the metal precursor improved the anchorage of the active phase and reduced leaching dramatically. Likewise, the activity was not influenced by the oxidation of the supports and reductions of ecotoxicity by more than 90% were observed. (c) 2007 Elsevier B.V. All rights reserved.
引用
收藏
页码:259 / 266
页数:8
相关论文
共 30 条
[1]  
*APHA, 1979, STAND METH EX WAT WA, P198
[2]  
*APHA, 1979, STAND METH EX WAT WA, P233
[3]   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
[4]   Effects of support surface composition on the activity and selectivity of Pd/C catalysts in aqueous-phase hydrodechlorination reactions [J].
Calvo, L ;
Gilarranz, MA ;
Casas, JA ;
Mohedano, AF ;
Rodríguez, JJ .
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 2005, 44 (17) :6661-6667
[5]   Treatment of chlorophenols-bearing wastewaters through hydrodechlorination using Pd/activated carbon catalysts [J].
Calvo, L ;
Mohedano, AF ;
Casas, JA ;
Gilarranz, MA ;
Rodríguez, JJ .
CARBON, 2004, 42 (07) :1377-1381
[6]   Dehalogenative oligomerization of dichlorodifluoromethane catalyzed by activated carbon-supported Pt-Cu catalysts: effect of Cu to Pt atomic ratio [J].
Chakraborty, D ;
Kulkarni, PP ;
Kovalchuk, VI ;
d'Itri, JL .
CATALYSIS TODAY, 2004, 88 (3-4) :169-181
[7]  
DURAES L, 2004, BIOTECHNOLOGY, V64, P712
[8]   Degradation of some biorecalcitrant pesticides by homogeneous and heterogeneous photocatalytic ozonation [J].
Farré, MJ ;
Franch, MI ;
Malato, S ;
Ayllón, JA ;
Peral, J ;
Doménech, X .
CHEMOSPHERE, 2005, 58 (08) :1127-1133
[9]   Three-step catalytic detoxification process of wastewater containing chlorinated aromatic compounds: Experimental results and modeling issues [J].
Felis, V ;
Fouilloux, P ;
De Bellefon, C ;
Schweich, D .
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 1999, 38 (11) :4213-4219
[10]   Modification of the surface chemistry of activated carbons [J].
Figueiredo, JL ;
Pereira, MFR ;
Freitas, MMA ;
Orfao, JJM .
CARBON, 1999, 37 (09) :1379-1389