The effect of AuAg-MCF and AuAg-NbMCF catalysts pretreatment on the gold-silver alloy formation and the catalytic behavior in selective methanol oxidation with oxygen

被引:23
作者
Sobczak, Izabela [1 ]
Dembowiak, Ewa [1 ]
机构
[1] Adam Mickiewicz Univ, Fac Chem, PL-61614 Poznan, Poland
关键词
NbMCF; MCF; Au-Ag system; Methanol oxidation; Formaldehyde; MESOSTRUCTURED CELLULAR FOAMS; MESOPOROUS MATERIALS; CO OXIDATION; OXIDE CATALYSTS; ACTIVE-SITES; AG; NANOPARTICLES; NB; NIOBIUM; PHASE;
D O I
10.1016/j.molcata.2015.08.017
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
MCF (mesostructured cellular foams) and NbMCF were used as supports for gold and silver. Bimetallic (Au-Ag) catalysts were prepared by metals loading (Au/Ag atomic ratio= 0.5 and 2) on 3-aminopropyltrimethoxysilane grafted supports and reduction by NaBH4 before calcination at 773 K. The prepared samples were then activated in inert gas at 623 K or reduced with hydrogen at 723 K. The catalysts treated in these ways were fully characterized by XRD, TEM, UV-vis and XPS techniques. Au-Ag alloy was identified on the surface of AuAg-MCF and AuAg-NbMCF catalysts. The composition of Au-Ag alloy was found to be sensitive to the catalyst pretreatment conditions. The reduction of Au-Ag containing materials with NaBH4 led to the formation of alloy with low silver content. The Au-Ag alloy was enriched in silver partially by the activation in argon flow and to a substantial degree by the reduction with hydrogen. The conditions of catalysts treatment also determined the alloy particle size. Catalytic activity of Au-Ag catalysts was tested in the oxidation of methanol in the gas phase. The results showed that the presence of gold-silver alloy on MCF surface was responsible for high activity of the catalysts as a result of synergetic interactions between Au and Ag species. Niobium in MCF support influenced both the activity of the catalysts and the selectivity to formaldehyde. (C) 2015 Elsevier B.V. All rights reserved.
引用
收藏
页码:137 / 148
页数:12
相关论文
共 48 条
[31]   REPORTING PHYSISORPTION DATA FOR GAS SOLID SYSTEMS WITH SPECIAL REFERENCE TO THE DETERMINATION OF SURFACE-AREA AND POROSITY (RECOMMENDATIONS 1984) [J].
SING, KSW ;
EVERETT, DH ;
HAUL, RAW ;
MOSCOU, L ;
PIEROTTI, RA ;
ROUQUEROL, J ;
SIEMIENIEWSKA, T .
PURE AND APPLIED CHEMISTRY, 1985, 57 (04) :603-619
[32]   Au containing mesostructured cellular foams NbMCF and ZrMCF in selective oxidation of methanol to formaldehyde [J].
Sobczak, Izabela ;
Kozlowska, Marta ;
Ziolek, Maria .
JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL, 2014, 390 :114-124
[33]   CuxCryOz mixed oxide as a promising support for gold - The effect of Au loading method on the effectiveness in oxidation reactions [J].
Sobczak, Izabela ;
Szrama, Katarzyna ;
Wojcieszak, Robert ;
Gaigneaux, Eric M. ;
Ziolek, Maria .
CATALYSIS TODAY, 2012, 187 (01) :48-55
[34]   Glycerol oxidation on gold catalysts supported on group five metal oxides-A comparative study with other metal oxides and carbon based catalysts [J].
Sobczak, Izabela ;
Jagodzinska, Katarzyna ;
Ziolek, Maria .
CATALYSIS TODAY, 2010, 158 (1-2) :121-129
[35]   Methanol oxidation as a catalytic surface probe [J].
Tatibouet, JM .
APPLIED CATALYSIS A-GENERAL, 1997, 148 (02) :213-252
[36]   Niobium rich SBA-15 materials - preparation, characterisation and catalytic activity [J].
Trejda, M. ;
Tuel, A. ;
Kujawa, J. ;
Kilos, B. ;
Ziolek, M. .
MICROPOROUS AND MESOPOROUS MATERIALS, 2008, 110 (2-3) :271-278
[37]   New Nb and Ta-FAU zeolites-Direct synthesis, characterisation and surface properties [J].
Trejda, M. ;
Wojtaszek, A. ;
Floch, A. ;
Wojcieszak, R. ;
Gaigneaux, E. M. ;
Ziolek, M. .
CATALYSIS TODAY, 2010, 158 (1-2) :170-177
[38]   The radical species and impurities present in mesoporous silicas as oxidation active centres [J].
Trejda, M. ;
Ziolek, M. ;
Decyk, P. ;
Duczmal, D. .
MICROPOROUS AND MESOPOROUS MATERIALS, 2009, 120 (03) :214-220
[39]   Nb-containing mesoporous materials of MCF type-Acidic and oxidative properties [J].
Trejda, Madej ;
Kujawa, Jolanta ;
Ziolek, Maria ;
Mrowiec-Bialon, Julita .
CATALYSIS TODAY, 2008, 139 (03) :196-201
[40]   Understanding the synergistic effects of gold bimetallic catalysts [J].
Wang, Aiqin ;
Liu, Xiao Yan ;
Mou, Chung-Yuan ;
Zhang, Tao .
JOURNAL OF CATALYSIS, 2013, 308 :258-271