The Role of Rhenium in the Conversion of Glycerol to Synthesis Gas Over Carbon Supported Platinum-Rhenium Catalysts

Journal Article · Tue Jan 01 00:00:00 EST 2008 · Journal of Catalysis

DOI:https://doi.org/10.1016/j.jcat.2008.09.027· OSTI ID:980641

Kunkes, E; Simonetti, D; Dumesic, J; Pyrz, W; Chen, J

Reaction kinetics measurements were carried out to study the conversion of aqueous solutions of glycerol (30 and 80 wt%) over carbon-supported Pt and Pt-Re catalysts at temperatures from 483 to 523 K. The results of these studies show that the turnover frequencies for production of H2, CO, CO2, and light alkanes (primarily methane) all increase upon the addition of Re to Pt/C catalysts. The molar ratio of H2/CO increases, while the CO/CO2 ratio decreases with Re addition, indicating increased rate of water-gas shift. For glycerol conversion over a Pt-Re/C catalyst with an atomic Pt:Re ratio of 1:1, increasing pressure or decreasing temperature leads to an increase in the production of alkanes and light oxygenated hydrocarbons (ethanol, methanol, propanediols, and acetone) at the expense of CO and CO2. Temperature-programmed desorption studies and microcalorimetric measurements indicate that addition of Re to Pt modifies the interaction of CO with surface sites. X-ray absorption spectroscopy and transmission electron microscopy studies provide evidence indicating that Pt-Re/C catalysts consist primarily of bimetallic nanoparticles with sizes below 2 nm, and Re inhibits the sintering of these nanoparticles during reaction conditions for glycerol conversion. The results of these reaction kinetic studies and characterization studies indicate that the performance of Pt-Re/C catalysts for glycerol conversion is related to the formation of Pt-Re nanoparticles, for which Re promotes the overall rate of glycerol reforming by reducing the binding energy of CO to Pt, thereby leading to less extensive blocking of surface sites by reaction intermediates and/or products. In addition, the presence of Re facilitates water-gas shift and Csingle bondO bond cleavage reactions.

• Research Organization: Brookhaven National Lab. (BNL), Upton, NY (United States). National Synchrotron Light Source
• Sponsoring Organization: Doe - Office Of Science
• DOE Contract Number: DE-AC02-98CH10886
• OSTI ID: 980641
• Report Number(s): BNL-93559-2010-JA; JCTLA5; TRN: US201015%%2026
• Journal Information: Journal of Catalysis, Vol. 260; ISSN 0021-9517
• Country of Publication: United States
• Language: English

Related Subjects

37 INORGANIC
ORGANIC
PHYSICAL AND ANALYTICAL CHEMISTRY
ABSORPTION SPECTROSCOPY
AQUEOUS SOLUTIONS
BINDING ENERGY
CARBON
CATALYSTS
CONVERSION
GLYCEROL
REACTION INTERMEDIATES
REACTION KINETICS
RHENIUM
SYNTHESIS GAS
TRANSMISSION ELECTRON MICROSCOPY
VISIBLE RADIATION
WATER GAS
national synchrotron light source