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

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• 作者：Florian Göltl ; Carine Michel ; Prokopis C. Andrikopoulos ; Alyssa M. Love ; Jürgen Hafner ; Ive Hermans ; Philippe Sautet
• 刊名：ACS Catalysis
• 出版年：2016
• 出版时间：December 2, 2016
• 年：2016
• 卷：6
• 期：12
• 页码：8404-8409
• 全文大小：418K
• ISSN：2155-5435

文摘

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.