Hydrodechlorination of chloroorganic compounds in ground water by palladium catalysts - Part 1. Development of polymer-based catalysts and membrane reactor tests

被引:65
作者
Fritsch, D
Kuhr, K
Mackenzie, K
Kopinke, FD
机构
[1] GKSS, Res Ctr, Inst Chem, D-21502 Geesthacht, Germany
[2] UFZ Helmholtz Ctr Environm Res, Dept Remediat Res, D-04318 Leipzig, Germany
关键词
hydrodechlorination; membrane reactor; Pd catalyst; catalysis in water; polymer membrane;
D O I
10.1016/S0920-5861(03)00208-6
中图分类号
O69 [应用化学];
学科分类号
081704 ;
摘要
A polymer-based catalytic membrane reactor was developed and applied for hydrodechlorination of chlorobenzene as a model compound of ground and waste water contaminants. The catalytically active membrane consists of a non-porous, thin film (about 3-7 mum) of poly(dimethylsiloxane) (PDMS) loaded with nano-sized Pd clusters. They were built-in either directly or as nano-sized, supported catalysts. A composite membrane, consisting of porous poly(acrylonitrile) (PAN) support and a Pd-loaded thin PDMS film, was fabricated on a coating machine. Defect-free membrane envelopes of 0.1 m(2) were produced and fitted into a membrane test cell. Gaseous hydrogen as reductant for hydrodechlorination is fed from the membrane's back side directly to the catalyst, embedded in the PDMS layer. The chemical reactions at the Pd surface are accompanied by absorption of chlorobenzene from the water phase into the PDMS layer and desorption of benzene and HCl back to the water phase. The specific activity of supported catalysts decreased only slightly by PDMS incorporation, e.g., from 31 l/g(Pd) min for Pd/Fe on titania to 16 l/g(Pd) min for the same catalyst built-in a 7 mum thick supported PDMS membrane and measured in the membrane test cell. Directly built-in Pd clusters are less active and more difficult to prepare on a larger scale. Some catalyst deactivation was observed and may be balanced by development of more suited nano-sized supported catalysts. (C) 2003 Elsevier B.V. All rights reserved.
引用
收藏
页码:105 / 118
页数:14
相关论文
共 23 条
[1]   Liquid-phase hydrodechlorination of chlorobenzene over palladium-supported catalysts -: Influence of HCl formation and NaOH addition [J].
Aramendía, MA ;
Boráu, V ;
García, IM ;
Jiménez, C ;
Lafont, F ;
Marinas, A ;
Marinas, JM ;
Urbano, FJ .
JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL, 2002, 184 (1-2) :237-245
[2]  
BENGTSON G, UNPUB
[3]   Catalytic dehydrohalogenation of polychlorinated biphenyls - Part II: Studies on a continuous process [J].
Forni, P ;
Prati, L ;
Rossi, M .
APPLIED CATALYSIS B-ENVIRONMENTAL, 1997, 14 (1-2) :49-53
[4]   NOVEL HIGHLY PERMSELECTIVE 6F-POLY(AMIDE-IMIDE)S AS MEMBRANE HOST FOR NANO-SIZED CATALYSTS [J].
FRITSCH, D ;
PEINEMANN, KV .
JOURNAL OF MEMBRANE SCIENCE, 1995, 99 (01) :29-38
[5]   Hydrogen, sulphur and chlorine coadsorption on Pd(111): a theoretical study of poisoning and promotion [J].
Gravil, PA ;
Toulhoat, H .
SURFACE SCIENCE, 1999, 430 (1-3) :176-191
[6]  
Gryaznov V M, 1983, US Patent, Patent No. [4,394,294, 4394294]
[7]  
KOHLER R, 1999, 52000 UFZ
[8]  
KOPINKE FD, 2000, WASSERWIRT WASSERTEC, V7, P58
[9]  
KOPINKE FD, 2002, GRUNDWASSER, V3, P140
[10]   Field application of palladized iron for the dechlorination of trichloroethene [J].
Korte, NE ;
Zutman, JL ;
Schlosser, RM ;
Liang, L ;
Gu, B ;
Fernando, Q .
WASTE MANAGEMENT, 2000, 20 (08) :687-694