Structured catalyst of Pd/ZnO on sintered metal fibers for 2-methyl-3-butyn-2-ol selective hydrogenation

被引:112
作者
Semagina, Natalia
Grasemann, Martin
Xanthopoulos, Nicolas
Renken, Albert
Kiwi-Minsker, Lioubov
机构
[1] Ecole Polytech Fed Lausanne, GGRC, Grp Chem React Engn, CH-1015 Lausanne, Switzerland
[2] EPFL STI IMX LMCH, Met Chem Lab, CH-1015 Lausanne, Switzerland
关键词
palladium; sintered metal fiber; structured catalyst; hydrogenation; acetylene alcohol; 2-methyl-3-butyn-2-ol; quinoline; ultrasonic regeneration;
D O I
10.1016/j.jcat.2007.06.028
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
An innovative structured catalyst based on sintered metal fibers (SMFs) coated by a gram-structured ZnO layer was developed for the selective 3-phase hydrogenation of functionalized alkynes. The catalyst was synthesized by the deposition of Pd-0-sol with 7-nm nanoparticles stabilized by molybdate anions on ZnO/SMF after reduction in hydrogen at 773 K. The crystallites of PdZn alloy (24 nm) were formed by high-temperature treatment in hydrogen and contained partly Pd(0) nanoparticles. Pd/ZnO/SMF (0.2 wt% Pd, 6 wt% ZnO) allowed >95% yield of 2-methyl-3-buten-2-ol (MBE) during 2-methyl-3-butyn-2-ol hydrogenation at 308 K and 5 bar pressure using water as the solvent and adding a small amount of quinoline. The consecutive reaction of MBE hydrogenation was suppressed due to the presence of PdZn in the active phase. The catalyst activity of the catalyst was an order of magnitude higher compared with that of commercial Lindlar catalyst (Pd, Pb/CaCO3), which quickly deactivated in aqueous media due to irreversible chemical transformations of the CaCO3 support. The structured catalyst developed in this study could be reused after ultrasonic regeneration, retaining the original selectivity and most of its initial activity. The catalyst showed high mechanical stability, precluding leaching of its components during the reaction. Due to easy shaping, high permeability, and low pressure drop during the fluid passage, the structured Pd/ZnO/SMF catalyst is suitable for a continuously operated staged bubble column reactor. (c) 2007 Elsevier Inc. All rights reserved.
引用
收藏
页码:213 / 222
页数:10
相关论文
共 77 条
[1]   Kinetic study of the liquid-phase hydrogenation of 1-butyne over a commercial palladium/alumina catalyst [J].
Alves, J. A. ;
Bressa, S. P. ;
Martinez, O. M. ;
Barreto, G. F. .
CHEMICAL ENGINEERING JOURNAL, 2007, 125 (03) :131-138
[2]  
[Anonymous], [No title captured]
[3]   OPTIMIZATION OF THE SELECTIVE SEMIHYDROGENATION OF PHENYLACETYLENE WITH SUPPORTED PALLADIUM SYSTEMS [J].
ARAMENDIA, MA ;
BORAU, V ;
JIMENEZ, C ;
MARINAS, JM ;
SEMPERE, ME ;
URBANO, FJ .
APPLIED CATALYSIS, 1990, 63 (02) :375-389
[4]   Oxidation of FeCrAl alloy: influence of temperature and atmosphere on scale growth rate and mechanism [J].
Badini, C ;
Laurella, F .
SURFACE & COATINGS TECHNOLOGY, 2001, 135 (2-3) :291-298
[5]   Adsorptive and catalytic properties of alumina-supported Pd-Mo catalysts [J].
Baldanza, MAS ;
de Mello, LF ;
Vannice, A ;
Noronha, FB ;
Schmal, M .
JOURNAL OF CATALYSIS, 2000, 192 (01) :64-76
[6]   Supported palladium catalysts for fine chemicals synthesis [J].
Blaser, HU ;
Indolese, A ;
Schnyder, A ;
Steiner, H ;
Studer, M .
JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL, 2001, 173 (1-2) :3-18
[7]   LIQUID-PHASE HYDROGENATION OF UNSATURATED-HYDROCARBONS ON PALLADIUM, PLATINUM AND RHODIUM CATALYSTS .1. KINETIC-STUDY OF 1-BUTENE, 1,3-BUTADIENE AND 1-BUTYNE HYDROGENATION ON PLATINUM [J].
BOITIAUX, JP ;
COSYNS, J ;
ROBERT, E .
APPLIED CATALYSIS, 1987, 32 (1-2) :145-168
[8]   HYDROGENATION OF HIGHLY UNSATURATED-HYDROCARBONS OVER HIGHLY DISPERSED PD CATALYST .2. LIGAND EFFECT OF PIPERIDINE [J].
BOITIAUX, JP ;
COSYNS, J ;
VASUDEVAN, S .
APPLIED CATALYSIS, 1985, 15 (02) :317-326
[9]   Application of heterogeneous colloid catalysts for the preparation of fine chemicals [J].
Bonnemann, H ;
Brijoux, W ;
Tilling, AS ;
Siepen, K .
TOPICS IN CATALYSIS, 1997, 4 (3-4) :217-227
[10]  
BROECKER FJ, 1991, Patent No. 5063194