Hydrodechlorination of CCl2F2 (CFC-12) over silica-supported palladium-gold catalysts

被引:82
作者
Bonarowska, M [1 ]
Malinowski, A [1 ]
Juszczyk, W [1 ]
Karpinski, Z [1 ]
机构
[1] Polish Acad Sci, Inst Phys Chem, Dept Catalysis Met, PL-01224 Warsaw, Poland
关键词
CCl2F2; hydrodechlorination; Pd-Au/SiO2; selectivity for CH2F2; alloy homogeneity;
D O I
10.1016/S0926-3373(00)00231-9
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
Two series of well-mixed Pd-Au/SiO2 catalysts prepared by direct redox method were tested in the reaction of CCl2F2 (CFC-12) hydrodechlorination. A moderate selectivity for CH2F2 exhibited by monometallic Pd/SiO2 (similar to 40%) is significantly increased, up to similar to 95%, with Au addition. Proper Pd-Au alloying is essential to obtain such a selectivity enhancement. Poorly mixed Pd-Au/SiO2 catalysts show the catalytic behaviour not very much different from that of Pd/SiO2, producing a lot of methane. Changes in the apparent activation energy are also associated with the degree of Pd-Au alloying. After reaction, the Pd/SiO2 and Pd-Au/SiO2 catalysts contain dissolved carbon. Hydrogen treatment of carbonized Pd-Au/SiO2 catalysts removes this carbon. XRD study of the regenerated samples shows no change in the structure and composition of Pd-Au phase, compared to freshly prereduced bimetallic catalysts. (C) 2001 Elsevier Science B.V. All rights reserved.
引用
收藏
页码:187 / 193
页数:7
相关论文
共 29 条
[1]  
Ainbinder Z., 1997, HDB HETEROGENEOUS CA, V4, P1677
[2]   PREPARATION OF PLATINUM GOLD BIMETALLIC CATALYSTS BY REDOX REACTIONS [J].
BARBIER, J ;
MARECOT, P ;
DELANGEL, G ;
BOSCH, P ;
BOITIAUX, JP ;
DIDILLON, B ;
DOMINGUEZ, JM ;
SCHIFTER, I ;
ESPINOSA, G .
APPLIED CATALYSIS A-GENERAL, 1994, 116 (1-2) :179-186
[3]  
Barbier J., 1997, Handbook of Heterogeneous Catalysis, V1, P257
[4]   Characterization of Pd-Au/SiO2 catalysts by X-ray diffraction, temperature-programmed hydride decomposition, and catalytic probes [J].
Bonarowska, M ;
Pielaszek, J ;
Juszczyk, W ;
Karpinski, Z .
JOURNAL OF CATALYSIS, 2000, 195 (02) :304-315
[5]   CONVERSION UNDER HYDROGEN OF DICHLORODIFLUOROMETHANE OVER BIMETALLIC PALLADIUM CATALYSTS [J].
COQ, B ;
HUB, S ;
FIGUERAS, F ;
TOURNIGANT, D .
APPLIED CATALYSIS A-GENERAL, 1993, 101 (01) :41-50
[6]   EFFECT OF THE METAL-SUPPORT INTERACTION ON THE CATALYTIC PROPERTIES OF PALLADIUM FOR THE CONVERSION OF DIFLUORODICHLOROMETHANE WITH HYDROGEN - COMPARISON OF OXIDES AND FLUORIDES AS SUPPORTS [J].
COQ, B ;
FIGUERAS, F ;
HUB, S ;
TOURNIGANT, D .
JOURNAL OF PHYSICAL CHEMISTRY, 1995, 99 (28) :11159-11166
[7]   CONVERSION UNDER HYDROGEN OF DICHLORODIFLUOROMETHANE OVER SUPPORTED PALLADIUM CATALYSTS [J].
COQ, B ;
COGNION, JM ;
FIGUERAS, F ;
TOURNIGANT, D .
JOURNAL OF CATALYSIS, 1993, 141 (01) :21-33
[8]   Transient kinetics investigations of reaction intermediates involved in CF2Cl2 hydrodechlorination [J].
Deshmukh, S ;
d'Itri, JL .
CATALYSIS TODAY, 1998, 40 (04) :377-385
[9]   Hydrodechlorination of 1,1-dichlorotetrafluoroethane and dichlorodifluoromethane catalyzed by Pd on fluorinated aluminas: The role of support material [J].
Early, K ;
Kovalchuk, VI ;
Lonyi, F ;
Deshmukh, S ;
d'Itri, JL .
JOURNAL OF CATALYSIS, 1999, 182 (01) :219-227
[10]   THE ADSORPTION AND REACTION OF CO AND O-2 ON PD-AU ALLOY WIRES [J].
ELEY, DD ;
MOORE, PB .
SURFACE SCIENCE, 1981, 111 (02) :325-343