A simple direct mechanism for methane-to-methanol conversion has been investigated by first principles on a series of oxygen-precovered transition-metal surfaces. Energy barriers and reaction paths have been determined for three competing elementary processes by the nudged elastic band algorithm. Indicators of reactivity toward each elementary step have been identified, providing significant insight into a rational search for a suitable catalyst. The effect of chemical environment, local geometry, strain, and coadsorption have been addressed, and general guidelines have been identified. On the basis of this analysis, we suggest that upon suitable conditions O-dosed Ag surfaces could display considerable reactivity toward direct methane-to-methanol conversion.
Direct methane-to-methanol conversion: Insight from first-principles calculations
de Gironcoli S
2007
Abstract
A simple direct mechanism for methane-to-methanol conversion has been investigated by first principles on a series of oxygen-precovered transition-metal surfaces. Energy barriers and reaction paths have been determined for three competing elementary processes by the nudged elastic band algorithm. Indicators of reactivity toward each elementary step have been identified, providing significant insight into a rational search for a suitable catalyst. The effect of chemical environment, local geometry, strain, and coadsorption have been addressed, and general guidelines have been identified. On the basis of this analysis, we suggest that upon suitable conditions O-dosed Ag surfaces could display considerable reactivity toward direct methane-to-methanol conversion.I documenti in IRIS sono protetti da copyright e tutti i diritti sono riservati, salvo diversa indicazione.
