TY - JOUR
T1 - Theoretical insights into catalytic oxidation of methane and light hydrocarbons
AU - Neurock, Matthew
AU - Buda, Corneliu
AU - Qian, Qiang
AU - Chin, Cathy
AU - Iglesia, Enrique
AU - Vajda, Stefan
PY - 2011
Y1 - 2011
N2 - The catalytic conversion of methane and light alkanes into energy, liquid fuels and chemicals via reforming, dehydrogenation, partial oxidation and combustion processes occur through similar elementary C-H and O2 bond activation steps which differ only in the nature of the active sites and the surface coverages that result under operating conditions. The prevailing chemistry is ultimately controlled by the nature of the metal, the as well as the surface coverage and reactivity of chemisorbed oxygen. Experimental results for the partial oxidation of methane over supported metal clusters, for example, reveal the presence of different kinetic regimes which can be described by unique rate expressions that result for the conversion over bare and oxygen-covered metal surfaces. First-principle density functional theoretical calculations and kinetic Monte Carlo simulation are used here to elucidate the elementary C-H and O2 activation steps at different surface sites and to establish the influence of surface coverage on the catalytic activity and selectivity for the over different transition metal surfaces. The results are used to understand the partial oxidation of methane and dehydrogenation of propane and cyclohexane on transition metal particles.
AB - The catalytic conversion of methane and light alkanes into energy, liquid fuels and chemicals via reforming, dehydrogenation, partial oxidation and combustion processes occur through similar elementary C-H and O2 bond activation steps which differ only in the nature of the active sites and the surface coverages that result under operating conditions. The prevailing chemistry is ultimately controlled by the nature of the metal, the as well as the surface coverage and reactivity of chemisorbed oxygen. Experimental results for the partial oxidation of methane over supported metal clusters, for example, reveal the presence of different kinetic regimes which can be described by unique rate expressions that result for the conversion over bare and oxygen-covered metal surfaces. First-principle density functional theoretical calculations and kinetic Monte Carlo simulation are used here to elucidate the elementary C-H and O2 activation steps at different surface sites and to establish the influence of surface coverage on the catalytic activity and selectivity for the over different transition metal surfaces. The results are used to understand the partial oxidation of methane and dehydrogenation of propane and cyclohexane on transition metal particles.
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M3 - Conference article
AN - SCOPUS:80051885840
SN - 0065-7727
JO - ACS National Meeting Book of Abstracts
JF - ACS National Meeting Book of Abstracts
T2 - 241st ACS National Meeting and Exposition
Y2 - 27 March 2011 through 31 March 2011
ER -