Computationally Exploring Confinement Effects in the Methane-to-Methanol Conversion over Iron-Oxo Centers in Zeolites

Florian Göltl; Carine Michel; Prokopis C. Andrikopoulos; Alyssa M. Love; Jürgen Hafner; Ive Hermans; Philippe Sautet

doi:10.1021/acscatal.6b02640

Computationally Exploring Confinement Effects in the Methane-to-Methanol Conversion over Iron-Oxo Centers in Zeolites

Florian Göltl, Carine Michel, Prokopis C. Andrikopoulos, Alyssa M. Love, Jürgen Hafner, Ive Hermans, Philippe Sautet

Research output: Contribution to journal › Article › peer-review

91 Scopus citations

Abstract

Transition metal-oxo centers in zeolites are known to be active in the conversion of methane to methanol. Here, we study this reaction over Fe-oxo sites in the zeolite SSZ-13. By comparing calculations for the fully periodic structure and a cluster for two different methods - the standard van der Waals corrected semilocal density functional PBE-D2 and ACFDT-RPA, which is a method where correlation is calculated fully nonlocally - we find that it is actually the confining environment in the zeolite that reduces the barrier for this reaction, by more than 50%, and we find that the two applied methods lead to qualitatively different results. (Figure Presented).

Original language	English (US)
Pages (from-to)	8404-8409
Number of pages	6
Journal	ACS Catalysis
Volume	6
Issue number	12
DOIs	https://doi.org/10.1021/acscatal.6b02640
State	Published - Dec 2 2016
Externally published	Yes

Keywords

ACFDT-RPA
confinement effects
density functional theory
methane
methanol
zeolites

ASJC Scopus subject areas

Catalysis
General Chemistry

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10.1021/acscatal.6b02640

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title = "Computationally Exploring Confinement Effects in the Methane-to-Methanol Conversion over Iron-Oxo Centers in Zeolites",

abstract = "Transition metal-oxo centers in zeolites are known to be active in the conversion of methane to methanol. Here, we study this reaction over Fe-oxo sites in the zeolite SSZ-13. By comparing calculations for the fully periodic structure and a cluster for two different methods - the standard van der Waals corrected semilocal density functional PBE-D2 and ACFDT-RPA, which is a method where correlation is calculated fully nonlocally - we find that it is actually the confining environment in the zeolite that reduces the barrier for this reaction, by more than 50%, and we find that the two applied methods lead to qualitatively different results. (Figure Presented).",

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T1 - Computationally Exploring Confinement Effects in the Methane-to-Methanol Conversion over Iron-Oxo Centers in Zeolites

AU - Göltl, Florian

AU - Michel, Carine

AU - Andrikopoulos, Prokopis C.

AU - Love, Alyssa M.

AU - Hafner, Jürgen

AU - Hermans, Ive

AU - Sautet, Philippe

PY - 2016/12/2

Y1 - 2016/12/2

N2 - Transition metal-oxo centers in zeolites are known to be active in the conversion of methane to methanol. Here, we study this reaction over Fe-oxo sites in the zeolite SSZ-13. By comparing calculations for the fully periodic structure and a cluster for two different methods - the standard van der Waals corrected semilocal density functional PBE-D2 and ACFDT-RPA, which is a method where correlation is calculated fully nonlocally - we find that it is actually the confining environment in the zeolite that reduces the barrier for this reaction, by more than 50%, and we find that the two applied methods lead to qualitatively different results. (Figure Presented).

AB - Transition metal-oxo centers in zeolites are known to be active in the conversion of methane to methanol. Here, we study this reaction over Fe-oxo sites in the zeolite SSZ-13. By comparing calculations for the fully periodic structure and a cluster for two different methods - the standard van der Waals corrected semilocal density functional PBE-D2 and ACFDT-RPA, which is a method where correlation is calculated fully nonlocally - we find that it is actually the confining environment in the zeolite that reduces the barrier for this reaction, by more than 50%, and we find that the two applied methods lead to qualitatively different results. (Figure Presented).

KW - ACFDT-RPA

KW - confinement effects

KW - density functional theory

KW - methane

KW - methanol

KW - zeolites

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Computationally Exploring Confinement Effects in the Methane-to-Methanol Conversion over Iron-Oxo Centers in Zeolites

Abstract

Keywords

ASJC Scopus subject areas

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