Theoretical studies of the decomposition of methanol on Ni(100)

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Abstract
The formation energies for a number of possible intermediates in the decomposition of methanol on Ni(100) have been calculated from first principles, using a 20‐atom model for bulk Ni. The formation of a methoxy species is shown to be a favorable first step (ΔH = −67 kcal/mol) but cleavage of the CO bond is shown to be thermodynamically preferred (ΔH = −109 kcal/mol). Decomposition of the methoxy species is postulated to proceed via formation of a strongly bound CH2O species and subsequently, a CHO radical with an enthalpy change for both steps in the range 16–24 kcal/mol. The calculational procedure (generalized valence bond and configuration interaction) is shown to produce analogous data for gas phase decompositions that are accurate to ±2 kcal/mol. The implications of these results for other transition metal systems are also discussed.

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