Carbon nanotube supported ruthenium catalysts for the treatment of high strength wastewater with aniline using wet air oxidation

被引:115
作者
Garcia, J.
Gomes, H. T.
Serf, Ph.
Kalck, Ph.
Figueiredo, J. L.
Faria, J. L.
机构
[1] Univ Porto, Fac Engn, Lab Catalise & Mat, Dept Engn Quim, P-4200465 Oporto, Portugal
[2] Univ Complutense Madrid, Fac Ciencia, Dept Ingn Quim, E-28040 Madrid, Spain
[3] Inst Politecn Braganca, Escola Super Tecnol & Gestao, Dept Tecnol Quim, P-5300857 Braganca, Portugal
[4] Ecole Natl Super Ingn Arts Chim & Technol, Lab Catalyse Chim Fine & Polymeres, F-31077 Toulouse 4, France
关键词
carbon nanotubes; catalyst support; transmission electron microscopy; catalytic properties; oxidation;
D O I
10.1016/j.carbon.2006.05.035
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
Multi-walled carbon nanotubes (MWCNT) can be efficiently used as support of ruthenium catalysts for the catalytic wet air oxidation of high strength wastewater containing aniline. Catalysts were prepared using different ruthenium precursors, Ruthenocene [Ru(eta(5)-C5H5)(2)], Ruthenium (1,5-cyclooctadiene, 1,3,5-cyclooctatriene) [Ru(cod)(cot)] and Ruthenium trichloride (RuCl3 center dot xH(2)O), different impregnation methods (excess solution and incipient wetness impregnation) and different MWCNT support surface chemistry (nitric acid oxidized MWCNT-COOH and Na2CO3 ion exchanged MWCNT-COONa). The efficiency of the aniline removal obtained with the catalysts prepared with different precursors decreases in the order [Ru(cod)(cot)] > RuCl3 center dot xH(2)O > [Ru(eta(5)-C5H5)(2)], 100% aniline conversion being obtained after 45 min of reaction with the catalyst prepared with [Ru(cod)(cot)]. The influence of the impregnation technique was found to be negligible, while the use of the MWCNT-COONa support led to increased catalyst performances when compared to that obtained with catalysts prepared with the MWCNT-COOH support. Leaching of ruthenium was observed in all cases, but the use of the precursor [Ru(cod)(cot)] and of the support MWCNT-COONa in the preparation of the catalysts seems to improve their stability. A direct relationship between metal load and catalyst stability was found and attributed to the strength of metal-support interactions. (c) 2006 Elsevier Ltd. All rights reserved.
引用
收藏
页码:2384 / 2391
页数:8
相关论文
共 31 条
[1]   Nanotubes from carbon [J].
Ajayan, PM .
CHEMICAL REVIEWS, 1999, 99 (07) :1787-1799
[2]   SOME ASPECTS OF THE SURFACE-CHEMISTRY OF CARBON-BLACKS AND OTHER CARBONS [J].
BOEHM, HP .
CARBON, 1994, 32 (05) :759-769
[3]   Further insights into the Ru nanoparticles-carbon interactions and their role in the catalytic properties [J].
Cerro-Alarcón, M ;
Maroto-Valiente, A ;
Rodríguez-Ramos, I ;
Guerrero-Ruiz, A .
CARBON, 2005, 43 (13) :2711-2722
[4]  
Chambers A, 1998, POWER ENG, V102, P12
[5]   Novel multi-walled nanotubes-supported and alkali-promoted Ru catalysts for ammonia synthesis under atmospheric pressure [J].
Chen, HB ;
Lin, JD ;
Cai, Y ;
Wang, XY ;
Yi, J ;
Wang, J ;
Wei, G ;
Lin, YZ ;
Liao, DW .
APPLIED SURFACE SCIENCE, 2001, 180 (3-4) :328-335
[6]   Nanotubes, nanoscience, and nanotechnology [J].
Cohen, ML .
MATERIALS SCIENCE & ENGINEERING C-BIOMIMETIC AND SUPRAMOLECULAR SYSTEMS, 2001, 15 (1-2) :1-11
[7]   Catalytic wet air oxidation of phenol over platinum and ruthenium catalysts [J].
Cybulski, A ;
Trawczynski, J .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2004, 47 (01) :1-13
[8]   Removal of aniline from aqueous solution in a mixed flow reactor using emulsion liquid membrane [J].
Datta, S ;
Bhattacharya, PK ;
Verma, N .
JOURNAL OF MEMBRANE SCIENCE, 2003, 226 (1-2) :185-201
[9]   Decoration of carbon nanotubes [J].
Ebbesen, TW ;
Hiura, H ;
Bisher, ME ;
Treacy, MMJ ;
ShreeveKeyer, JL ;
Haushalter, RC .
ADVANCED MATERIALS, 1996, 8 (02) :155-&
[10]   Platinum catalysts supported on MWNT for catalytic wet air oxidation of nitrogen containing compounds [J].
Garcia, J ;
Gomes, HT ;
Serp, P ;
Kalck, P ;
Figueiredo, JL ;
Faria, JL .
CATALYSIS TODAY, 2005, 102 :101-109