The selectivity of a catalyst in ethylene epoxidation reaction was addressed using quantum mechanical computer simulations. We found that the catalyst's selectivity in the reaction of oxametallacycle to form ethylene epoxide (EO) rather than the competing acetaldehyde (Ac) is determined in part by the differential bonding affinity of the catalyst toward the O and C atoms of the oxametallacycle. This interplay between O- and C-metal bond strength is due to the different structures of the two transition states. Based on this finding, we introduce a new indicator that determines the difference between the EO and Ac activation energies in the oxametallacycle reaction remarkably well for a number of different materials.

What determines the catalyst's selectivity in the ethylene epoxidation reaction / Kokalj, A.; Gava, P.; de Gironcoli, S.; Baroni, S.. - In: JOURNAL OF CATALYSIS. - ISSN 0021-9517. - 254:2(2008), pp. 304-309. [10.1016/j.jcat.2008.01.008]

What determines the catalyst's selectivity in the ethylene epoxidation reaction

Kokalj, A.;Gava, P.;de Gironcoli, S.;Baroni, S.
2008-01-01

Abstract

The selectivity of a catalyst in ethylene epoxidation reaction was addressed using quantum mechanical computer simulations. We found that the catalyst's selectivity in the reaction of oxametallacycle to form ethylene epoxide (EO) rather than the competing acetaldehyde (Ac) is determined in part by the differential bonding affinity of the catalyst toward the O and C atoms of the oxametallacycle. This interplay between O- and C-metal bond strength is due to the different structures of the two transition states. Based on this finding, we introduce a new indicator that determines the difference between the EO and Ac activation energies in the oxametallacycle reaction remarkably well for a number of different materials.
2008
254
2
304
309
https://www.sciencedirect.com/science/article/pii/S0021951708000134?via%3Dihub
Kokalj, A.; Gava, P.; de Gironcoli, S.; Baroni, S.
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Utilizza questo identificativo per citare o creare un link a questo documento: https://hdl.handle.net/20.500.11767/14033
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