Computational Investigation of Thermochemistry and Kinetics of Steam Methane Reforming on Ni(111) under Realistic Conditions

Autor:	D. Wayne Blaylock, Teppei Ogura, William H. Green, Gregory J. O. Beran
Rok vydání:	2009
Předmět:	Chemistry Kinetics Thermodynamics Reaction intermediate Surfaces Coatings and Films Electronic Optical and Magnetic Materials Catalysis Steam reforming General Energy Adsorption Thermochemistry Physical chemistry Density functional theory Physical and Theoretical Chemistry Bar (unit)
Zdroj:	The Journal of Physical Chemistry C. 113:4898-4908
ISSN:	1932-7455 1932-7447
DOI:	10.1021/jp806527q
Popis:	The reaction pathways and kinetics of steam methane reforming (SMR) over Ni(111) are investigated using plane wave density functional theory. The thermochemical data are used to develop a microkinetic model of SMR that allows for the investigation of reforming pathways and the most abundant reaction intermediates on the catalyst surface at industrially relevant temperatures and pressures. Pairing the kinetic model with a statistical thermodynamic treatment, surface behavior under a wide range of temperatures, pressures, and initial concentrations can be examined. We present our results at T = 800 °C and P = 10 bar with an initial H2O/CH4 ratio of 2.5:1. Sensitivity analysis is used to provide information about rate-limiting steps in the reaction network. The reaction intermediate CH* is found to be the most important carbon-containing intermediate. CH4(g) adsorption as well as the reactions CH* + O* → CHO* and CH* + OH* → CHOH* are found to be the most sensitive reactions in the mechanism. Consistent acco...
Databáze:	OpenAIRE
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