The "one-pot" synthesis of 4-methyl-2-pentanone (methyl isobutyl ketone) from acetone over PdCu catalysts prepared from layered double hydroxides

被引:49
作者
Martínez-Ortiz, MD [1 ]
Tichit, D [1 ]
Gonzalez, P [1 ]
Coq, B [1 ]
机构
[1] ENSCM, CNRS, UMR 5618, Lab Mat Catalyt & Catalyse & Chim Organ, F-34296 Montpellier 5, France
关键词
methyl isobutyl ketone; acetone; Pd; Cu; layered double hydroxides; multifunctional catalysis;
D O I
10.1016/S1381-1169(03)00179-1
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
Supported PdCu catalysts prepared from layered double hydroxides (LDHs) as precursors were evaluated in the gas phase reaction of acetone with hydrogen to methyl isobutyl ketone (MIBK). Two series of catalysts containing ca. 0.2 wt.% Pd and various amounts of Cu (Cu/Pd molar ratio of ca. 0.25, 0.5 and 1) were elaborated according to different methods. One series of precursors was obtained by impregnation of calcined Mg(Al)O mixed oxide with heterobinuclear PdxCu1-x acetylacetonates. A second series of precursors was synthesized by coprecipitation of Mg/Pd/Cu/Al LDHs. After calcination, both series were reduced at 473 K. The extends of basic, acid and metal functions were evaluated through microcalorimetric adsorption Of CO2, TPD of NH3 and TPR of H-2. It was found that the multifunctional transformation of acetone to MIBK was rate determined by the basic function. However, the way by which the catalysts were prepared, impregnation or coprecipitation, controls the extend of hydrogenated by-products, isopropyl alcohol and 4-methyl-2-pentanol. The extensive dilution by migrating MgAlOx species onto the metallic particles makes the coprecipitated catalysts highly selective by decreasing selectively the rate of C=O bond hydrogenation. (C) 2003 Elsevier Science B.V. All rights reserved.
引用
收藏
页码:199 / 210
页数:12
相关论文
共 19 条
[1]  
BASILE F, 1996, J CHEM SOC CHEM COMM, P2435
[2]   HYDROGEN-OXYGEN TITRATION METHOD FOR MEASUREMENT OF SUPPORTED PALLADIUM SURFACE-AREAS [J].
BENSON, JE ;
HWANG, HS ;
BOUDART, M .
JOURNAL OF CATALYSIS, 1973, 30 (01) :146-153
[3]  
CHEN G, 1983, APPL CATAL, V8, P3
[4]   One-step synthesis of methyl isobutyl ketone from acetone with calcined Mg/Al hydrotalcite-supported palladium or nickel catalysts [J].
Chen, YZ ;
Hwang, CM ;
Liaw, CW .
APPLIED CATALYSIS A-GENERAL, 1998, 169 (02) :207-214
[5]   One-step synthesis of methyl isobutyl ketone from acetone and hydrogen over Cu-on-MgO catalysts [J].
Chikán, V ;
Molnár, A ;
Balázsik, K .
JOURNAL OF CATALYSIS, 1999, 184 (01) :134-143
[6]   Influence of the metal function in the "one-pot" synthesis of 4-methyl-2-pentanone (methyl isobutyl ketone) from acetone over palladium supported on Mg(Al)O mixed oxides catalysts [J].
Das, N ;
Tichit, D ;
Durand, R ;
Graffin, P ;
Coq, B .
CATALYSIS LETTERS, 2001, 71 (3-4) :181-185
[7]   Alloy formation and stability in Pd-Cu bimetallic catalysts [J].
FernandezGarcia, M ;
Anderson, JA ;
Haller, GL .
JOURNAL OF PHYSICAL CHEMISTRY, 1996, 100 (40) :16247-16254
[8]   METAL SUPPORT INTERACTION - GROUP-VIII METALS AND REDUCIBLE OXIDES [J].
HALLER, GL ;
RESASCO, DE .
ADVANCES IN CATALYSIS, 1989, 36 :173-235
[9]  
LEON Y LEON CA, 1991, APPL CATAL, V69, P291
[10]   DEHYDROGENATION AND HYDROGENATION ACTIVITY OF PALLADIUM-TIN-SILICA AND NICKEL-TIN-SILICA [J].
MASAI, M ;
HONDA, K ;
KUBOTA, A ;
OHNAKA, S ;
NISHIKAWA, Y ;
NAKAHARA, K ;
KISHI, K ;
IKEDA, S .
JOURNAL OF CATALYSIS, 1977, 50 (03) :419-428