Ruthenium Nanoparticles Supported on Carbon: An Active Catalyst for the Hydrogenation of Lactic Acid to 1,2-Propanediol

被引:95
作者
Iqbal, Sarwat [1 ]
Kondrat, Simon A. [1 ]
Jones, Daniel R. [1 ]
Schoenmakers, Daniel C. [1 ]
Edwards, Jennifer K. [1 ]
Lu, Li
Yeo, Benjamin R. [1 ]
Wells, Peter P. [3 ,4 ]
Gibson, Emma K. [3 ,4 ]
Morgan, David J. [1 ]
Kiely, Christopher J. [2 ]
Hutchings, Graham J. [1 ]
机构
[1] Cardiff Univ, Sch Chem, Cardiff Catalysis Inst, Main Bldg,Pk Pl, Cardiff CF10 3AT, S Glam, Wales
[2] Lehigh Univ, Dept Mat Sci & Engn, Bethlehem, PA 18015 USA
[3] UK Catalysis Hub, Harwell OX11 0FA, Oxon, England
[4] UCL, Dept Chem, London WC1H 0AJ, England
基金
英国工程与自然科学研究理事会; 欧洲研究理事会;
关键词
Catalytic hydrogenation; lactic acid; Ru/C; catalyst reuse; propane diol; propylene glycol; AQUEOUS-PHASE HYDROGENATION; ION-EXCHANGE-RESIN; ETHYL LACTATE; BIOMASS; HYDROGENOLYSIS; GLYCEROL; SURFACE; RU; CONVERSION; REDUCTION;
D O I
10.1021/acscatal.5b00625
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
The hydrogenation of lactic acid to form 1,2-propanediol has been investigated using Ru nanoparticles supported on carbon as a catalyst. Two series of catalysts which were prepared by wet impregnation and sol-immobilization were investigated. Their activity was contrasted with that of a standard commercial Ru/C catalyst (all catalysts comprise 5 wt % Ru). The catalyst prepared using sol-immobilization was found to be more active than the wet impregnation materials. In addition, the catalyst made by sol-immobilization was initially more active than the standard commercial catalyst. However, when reacted for an extended time or with successive reuse cycles, the sol-immobilized catalyst became less active, whereas the standard commercial catalyst became steadily more active. Furthermore, both catalysts exhibited an induction period during the first 1000 s of reaction. Detailed scanning transmission electron microscopy, X-ray photoelectron spectroscopy and X-ray absorption fine structure analysis data, when correlated with the catalytic performance results, showed that the high activity can be ascribed to highly dispersed Ru nanoparticles. Although the sol-immobilization method achieved these optimal discrete Ru nanoparticles immediately, as can be expected from this preparation methodology, the materials were unstable upon reuse. In addition, surface lactide species were detected on these particles using X-ray photoelectron spectroscopy, which could contribute to their deactivation. The commercial Ru/C catalysts, on the other hand, required treatment under reaction conditions to change from raft-like morphologies to the desired small nanoparticle morphology, during which time the catalytic performance progressively improved.
引用
收藏
页码:5047 / 5059
页数:13
相关论文
共 36 条
[1]   EFFECT OF RATIO OF CATALYST AND OTHER FACTORS UPON THE RATE OF HYDROGENATION [J].
ADKINS, H ;
BILLICA, HR .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1948, 70 (09) :3118-3120
[2]   PREPARATION AND CHARACTERIZATION OF CHLORINE-FREE RUTHENIUM CATALYSTS AND THE PROMOTER EFFECT IN AMMONIA-SYNTHESIS .3. A MAGNESIA-SUPPORTED RUTHENIUM CATALYST [J].
AIKA, K ;
TAKANO, T ;
MURATA, S .
JOURNAL OF CATALYSIS, 1992, 136 (01) :126-140
[3]   Incorporation of RuO2 nanoparticles into MFI-type zeolites [J].
Altwasser, S ;
Gläser, R ;
Lo, AS ;
Liu, PH ;
Chao, KJ ;
Weitkamp, J .
MICROPOROUS AND MESOPOROUS MATERIALS, 2006, 89 (1-3) :109-122
[4]   Understanding the structural deactivation of ruthenium catalysts on an atomic scale under both oxidizing and reducing conditions [J].
Assmann, J ;
Crihan, D ;
Knapp, M ;
Lundgren, E ;
Löffler, E ;
Muhler, M ;
Narkhede, V ;
Over, H ;
Schmid, M ;
Seitsonen, AP ;
Varga, P .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2005, 44 (06) :917-920
[5]  
Beamson G., 1992, High Resolution XPS of Organic Polymers: The Scienta ESCA300 Database, V1st ed., P136
[6]   RHENIUM AND ITS COMPOUNDS AS HYDROGENATION CATALYSTS .3. RHENIUM HEPTOXIDE [J].
BROADBENT, HS ;
CAMPBELL, GC ;
BARTLEY, WJ ;
JOHNSON, JH .
JOURNAL OF ORGANIC CHEMISTRY, 1959, 24 (12) :1847-1854
[7]   High-pressure oxidation of ruthenium as probed by surface-enhanced Raman and X-ray photoelectron spectroscopies [J].
Chan, HYH ;
Takoudis, CC ;
Weaver, MJ .
JOURNAL OF CATALYSIS, 1997, 172 (02) :336-345
[8]   Acid/base-treated activated carbons: Characterization of functional groups and metal adsorptive properties [J].
Chen, JP ;
Wu, SN .
LANGMUIR, 2004, 20 (06) :2233-2242
[9]   Kinetics of aqueous-phase hydrogenation of organic acids and their mixtures over carbon supported ruthenium catalyst [J].
Chen, Yuqing ;
Miller, Dennis J. ;
Jackson, James E. .
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 2007, 46 (10) :3334-3340
[10]   Effect of Reduction Temperature on the Preparation and Characterization of Pt-Ru Nanoparticles on Multiwalled Carbon Nanotubes [J].
Chetty, Raghuram ;
Xia, Wei ;
Kundu, Shankhamala ;
Bron, Michael ;
Reinecke, Thomas ;
Schuhmann, Wolfgang ;
Muhler, Martin .
LANGMUIR, 2009, 25 (06) :3853-3860