Characterization of Cu/SiO2 catalysts prepared by ion exchange for methanol dehydrogenation

被引:126
作者
Guerreiro, ED [1 ]
Gorriz, OF [1 ]
Rivarola, JB [1 ]
Arrua, LA [1 ]
机构
[1] UNSL, CONICET, Inst Invest Tecnol Quim, RA-5700 San Luis, Argentina
关键词
dehydrogenation; methanol; methylformate; copper/silica; ion exchange;
D O I
10.1016/S0926-860X(97)00207-X
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
A series of copper on silica catalysts prepared by using the ion exchange methods with copper loadings between 0.45 and 3 wt% have been studied by means of different techniques such as TPR, EPR, XANES, XRD, XRE BET and methanol dehydrogenation reaction. The TPR patterns showed two well-defined peaks with maxima between 250-350 degrees C and 600-650 degrees C. The first one (peak I) corresponds to two contributions: (i) the one step reduction (Cu2+ to Cu-0) of a low interacted species (S-1), and (ii) the partial reduction (Cu2+ to Cu1+) of a highly dispersed and surface interacted species (S-2). The second TPR peak (peak II) observed at a higher temperature corresponds to the second step reduction (Cu1+ to Cu-0) of the S-2 species. In addition, it has been found out that Cu-0 and not Cu2+ is the active site for methanol dehydrogenation to methyl formate. (C) 1997 Elsevier Science B.V.
引用
收藏
页码:259 / 271
页数:13
相关论文
共 43 条
[1]   DEHYDROGENATION OF METHANOL TO METHYL FORMATE OVER COPPER-BASED CATALYSTS [J].
AI, M .
APPLIED CATALYSIS, 1984, 11 (2-3) :259-270
[2]   PREPARATION, SPECTROSCOPIC CHARACTERIZATION AND STABILITY OF SILICA-SUPPORTED COPPER(I) SPECIES [J].
AMARA, M ;
BETTAHAR, M ;
GENGEMBRE, L ;
OLIVIER, D .
APPLIED CATALYSIS, 1987, 35 (01) :153-168
[3]   IMPREGNATION OF ALUMINA WITH COPPER CHLORIDE - EVIDENCE FOR DIFFERENTLY IMMOBILIZED COPPER SPECIES [J].
BAIKER, A ;
MONTI, D ;
WOKAUN, A .
APPLIED CATALYSIS, 1986, 23 (02) :425-436
[4]   POLYNUCLEAR METAL-COMPLEXES AS MODEL MIXED-OXIDE CATALYSTS - AN ION-EXCHANGE SUPPORT INTERACTION [J].
BECKLER, RK ;
WHITE, MG .
JOURNAL OF CATALYSIS, 1986, 102 (01) :252-256
[5]   AN IMPROVED PROCEDURE FOR ESTIMATING THE METAL-SURFACE AREA OF SUPPORTED COPPER-CATALYSTS [J].
BOND, GC ;
NAMIJO, SN .
JOURNAL OF CATALYSIS, 1989, 118 (02) :507-510
[6]   NATURE OF ACTIVE SPECIES IN COPPER-BASED CATALYSTS AND THEIR CHEMISTRY OF TRANSFORMATION OF NITROGEN-OXIDES [J].
CENTI, G ;
PERATHONER, S .
APPLIED CATALYSIS A-GENERAL, 1995, 132 (02) :179-259
[7]   THE MEASUREMENT OF COPPER SURFACE-AREAS BY REACTIVE FRONTAL CHROMATOGRAPHY [J].
CHINCHEN, GC ;
HAY, CM ;
VANDERVELL, HD ;
WAUGH, KC .
JOURNAL OF CATALYSIS, 1987, 103 (01) :79-86
[8]  
Cvetanovic R.J., 1967, ADV CATAL, V17, P103, DOI [DOI 10.1016/S0360-0564(08)60686-0, 10.1016/S0360-0564, DOI 10.1016/S0360-0564]
[9]   Amorphous alloy catalysis .8. A new activation of an amorphous Cu41Zr59 alloy in the transformation of methyl alcohol to methyl formate [J].
Domokos, L ;
Katona, T ;
Molnar, A ;
Lovas, A .
APPLIED CATALYSIS A-GENERAL, 1996, 142 (01) :151-158
[10]  
DVORAK B, 1970, J CATAL, V18, P108