On the Heterogeneity of Iron‐Oxo Species in Zeolites for the Oxidation of Methane to Methanol by Nitrous Oxide: A Theoretical Perspective DOI
Shuo Wang, Chenchen Li, Chong Liu

et al.

ChemCatChem, Journal Year: 2024, Volume and Issue: unknown

Published: Sept. 16, 2024

Abstract The conversion of methane to methanol (MTM) represents a pivotal objective in the C1 chemical industry. Transition metals, such as iron, exchanged zeolites are one category most active catalysts for direct MTM. One important topic understanding mechanism Fe‐zeolite catalyzed MTM is how heterogeneity catalytic (Fe) sites influences system stability and reactivity. Employing DFT calculations machine learning method, we herein studied stability–reactivity relationship cycle with N 2 O oxidant over Fe‐exchanged zeolites. Fe was introduced by using CHA FER looking at number related species (Fe II , FeO, FeOH). A strong correlation observed between species, which primarily determined formation energy trend remains consistent throughout cycle. reactivity analysis then demonstrated that less stable may exhibit higher reactivities when situated specific sites. Further validated significant relevance activation barriers reaction energies decomposition step not sufficiently captured traditional one‐dimensional Brønsted–Evans–Polanyi (BEP) relationship.

Language: Английский

On the Heterogeneity of Iron‐Oxo Species in Zeolites for the Oxidation of Methane to Methanol by Nitrous Oxide: A Theoretical Perspective DOI
Shuo Wang, Chenchen Li, Chong Liu

et al.

ChemCatChem, Journal Year: 2024, Volume and Issue: unknown

Published: Sept. 16, 2024

Abstract The conversion of methane to methanol (MTM) represents a pivotal objective in the C1 chemical industry. Transition metals, such as iron, exchanged zeolites are one category most active catalysts for direct MTM. One important topic understanding mechanism Fe‐zeolite catalyzed MTM is how heterogeneity catalytic (Fe) sites influences system stability and reactivity. Employing DFT calculations machine learning method, we herein studied stability–reactivity relationship cycle with N 2 O oxidant over Fe‐exchanged zeolites. Fe was introduced by using CHA FER looking at number related species (Fe II , FeO, FeOH). A strong correlation observed between species, which primarily determined formation energy trend remains consistent throughout cycle. reactivity analysis then demonstrated that less stable may exhibit higher reactivities when situated specific sites. Further validated significant relevance activation barriers reaction energies decomposition step not sufficiently captured traditional one‐dimensional Brønsted–Evans–Polanyi (BEP) relationship.

Language: Английский

Citations

0