Reaction kinetics of ethylene glycol reforming over platinum in the vapor versus aqueous phases

Journal Article · Thu Aug 12 00:00:00 EDT 2010 · Journal of Physical Chemistry. C

DOI:https://doi.org/10.1021/jp104136s· OSTI ID:1065669

Kandoi, Shampa ^[1]; Greeley, Jeff ^[2]; Simonetti, Dante ^[1]; Shabaker, John ^[1]; Dumesic, James A. ^[1]; Mavrikakis, Manos ^[1]

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1. Univ. of Wisconsin, Madison, WI (United States). Dept. of Chemical and Biological Engineering.
2. Univ. of Wisconsin, Madison, WI (United States). Dept. of Chemical and Biological Engineering; Argonne National Lab. (ANL), Argonne, IL (United States). Center for Nanoscale Materials.

First-principles, periodic, density functional theory (DFT) calculations are carried out on Pt(111) to investigate the structure and energetics of dehydrogenated ethylene glycol species and transition states for the cleavage of C–H/O–H and C–C bonds. Additionally, reaction kinetics studies are carried out for the vapor phase reforming of ethylene glycol (C₂H₆O₂) over Pt/Al₂O₃ at various temperatures, pressures, and feed concentrations. These results are compared to data for aqueous phase reforming of ethylene glycol on this Pt catalyst, as reported in a previous publication (Shabaker, J. W.; et al. J. Catal. 2003, 215, 344). Microkinetic models were developed to describe the reaction kinetics data obtained for both the vapor-phase and aqueous-phase reforming processes. The results suggest that C–C bond scission in ethylene glycol occurs at an intermediate value of x (3 or 4) in C₂H_xO₂. It is also found that similar values of kinetic parameters can be used to describe the vapor and aqueous phase reforming data, suggesting that the vapor phase chemistry of this reaction over platinum is similar to that in the aqueous phase over platinum.

• Research Organization: Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Oak Ridge Leadership Computing Facility (OLCF); Energy Frontier Research Centers (EFRC) (United States). Institute for Atom-efficient Chemical Transformations (IACT)
• Sponsoring Organization: USDOE Office of Science (SC), Basic Energy Sciences (BES)
• DOE Contract Number: AC02-06CH11357; AC05-00OR22725; AC02-05CH11231
• OSTI ID: 1065669
• Journal Information: Journal of Physical Chemistry. C, Vol. 115, Issue 4; Related Information: IACT partners with Argonne National Laboratory (lead); Brookhaven National Laboratory; Northwestern University; Purdue University; University of Wisconsin at Madison; ISSN 1932-7447
• Publisher: American Chemical Society
• Country of Publication: United States
• Language: English

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