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

作者：Goltl Florian^*; Michel Carine; Andrikopoulos Prokopis C; Love Alyssa M; Hafner Jurgen; Hermans Iye^*; Sautet Philippe^*

来源：ACS Catalysis, 2016, 6(12): 8404-8409.

DOI：10.1021/acscatal.6b02640

• confinement effects
• methane
• methanol
• zeolites
• density functional theory
• ACFDT-RPA

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.

• 出版日期2016-12