Is [FeO]2+ the Active Center Also in Iron Containing Zeolites? A Density Functional Theory Study of Methane Hydroxylation Catalysis by Fe-ZSM-5 Zeolite

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• 作者：Angela Rosa ; Giampaolo Ricciardi ; Evert Jan Baerends
• 刊名：Inorganic Chemistry
• 出版年：2010
• 出版时间：April 19, 2010
• 年：2010
• 卷：49
• 期：8
• 页码：3866-3880
• 全文大小：1158K
• 年卷期：v.49,no.8(April 19, 2010)
• ISSN：1520-510X

文摘

Arguments are put forward that the active α-oxygen site in the Fe-ZSM-5 catalyst consists of the FeO²⁺ moiety. It is demonstrated that this zeolite site for FeO²⁺ indeed obeys the design principles for high reactivity of the FeO²⁺ moiety proposed earlier: a ligand environment consisting of weak equatorial donors (rather oxygen based than nitrogen based) and very weak or absent trans axial donor. The α-oxygen site would then owe its high reactivity to the same electronic structure features that lends FeO²⁺ its high activity in biological systems, as well as in the classical Fenton chemistry.