Hydrogenolysis of glycerol over carbon-supported Ru and Pt catalysts

被引:495
作者
Maris, Erin P. [1 ]
Davis, Robert J. [1 ]
机构
[1] Univ Virginia, Dept Chem Engn, Charlottesville, VA 22904 USA
基金
美国国家科学基金会;
关键词
glycerol hydrogenolysis; ruthenium; platinum; retro-aldol; hydrogenation; ethylene glycol; propylene glycol; lactic acid;
D O I
10.1016/j.jcat.2007.05.008
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
Commercial carbon -supported Ru and Pt catalysts were evaluated in the batchwise hydrogenolysis of glycerol in aqueous solution at 473 K and 40 bar H-2, with and without added base. At neutral pH, Ru was more active than Pt at converting glycerol to glycols. However, Ru favored the production of ethylene glycol over propylene glycol and also catalyzed methane formation. Although less active, Pt catalyzed propylene glycol formation with high selectivity. Addition of base enhanced the reactivity of Pt to a greater extent than Ru, but lactate formation was significant at high pH in the presence of either Pt or Ru. The cleavage of C-C bonds leading to the formation of ethylene glycol from glycerol is proposed to occur primarily through a metal-catalyzed reaction on Ru, whereas this cleavage is thought to occur through a base-catalyzed reaction in the presence of Pt. An overall reaction network for glycerol hydrogenolysis is presented. (C) 2007 Published by Elsevier Inc.
引用
收藏
页码:328 / 337
页数:10
相关论文
共 40 条
[1]  
ALTAF M, 2007, J APPL MICROBIOL
[2]  
[Anonymous], 1994, US Pat, Patent No. [5276181, 5,276,181]
[3]  
Augustine R.L., 1996, HETEROGENEOUS CATALY
[4]   The solubility of lime in aqueous solutions of sugar and of glycerol [J].
Cameron, FK ;
Patten, HE .
JOURNAL OF PHYSICAL CHEMISTRY, 1911, 15 (01) :67-72
[5]   Glycerol hydrogenolysis on heterogeneous catalysts [J].
Chaminand, J ;
Djakovitch, L ;
Gallezot, P ;
Marion, P ;
Pinel, C ;
Rosier, C .
GREEN CHEMISTRY, 2004, 6 (08) :359-361
[6]   Removal of residual catalyst from simulated biodiesel's crude glycerol for glycerol hydrogenolysis to propylene glycol [J].
Chiu, CW ;
Dasari, MA ;
Sutterlin, WR ;
Suppes, GJ .
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 2006, 45 (02) :791-795
[7]   HYDROGENOLYSIS OF SORBITOL [J].
CLARK, IT .
INDUSTRIAL AND ENGINEERING CHEMISTRY, 1958, 50 (08) :1125-1126
[8]   Ethane hydrogenolysis over platinum - Selection and estimation of kinetic parameters [J].
Cortright, RD ;
Watwe, RM ;
Dumesic, JA .
JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL, 2000, 163 (1-2) :91-103
[9]   'Greening' the chemical industry: research and development priorities for biobased industrial products [J].
Dale, BE .
JOURNAL OF CHEMICAL TECHNOLOGY AND BIOTECHNOLOGY, 2003, 78 (10) :1093-1103
[10]   Low-pressure hydrogenolysis of glycerol to propylene glycol [J].
Dasari, MA ;
Kiatsimkul, PP ;
Sutterlin, WR ;
Suppes, GJ .
APPLIED CATALYSIS A-GENERAL, 2005, 281 (1-2) :225-231