Local Electric Field Effect of TMI (Fe, Co, Cu)-BEA on N2O Direct Dissociation

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• 作者：Ning Liu ; Runduo Zhang ; Yaping Li ; Biaohua Chen
• 刊名：Journal of Physical Chemistry C
• 出版年：2014
• 出版时间：May 22, 2014
• 年：2014
• 卷：118
• 期：20
• 页码：10944-10956
• 全文大小：693K
• 年卷期：v.118,no.20(May 22, 2014)
• ISSN：1932-7455

文摘

Zeolite catalyst consists of an infinite network of TO₄ tetrahedra (T = Si, Al, etc.) having various physic-chemical properties, among which the electric field effect (EFE) constituting one of the most important properties plays a major role in the heterogeneously catalytic reactions. However, up to now few works have been devoted to establishing the relationship between EFE and related catalytic behavior for the zeolite catalyst. In light of that, the present work systematically investigated the local electric field effect of the transition-metal-ion modified 尾 zeolites [TMI (Fe, Co, Cu)-BEA] during N₂O direct decomposition based on Mulliken charge transfer (CT) analysis, frontier molecular orbital analysis (FMO), and diffuse reflectance infrared Fourier transform spectra (DRIFTS). For the O₂ formation mechanism, the EFEs of TMI-BEA and formed 伪O greatly influenced adsorption and further activation of N₂O through the CT, which was quantitatively determined by the FMO gaps between TMI-BEA and N₂O. For the NO_x formation mechanism, the weak EFEs of Fe-BEA and formed 伪O during N₂O adsorption through its N end gave a clue of low NO selectivity of Fe-BEA. The EFE investigation of zeolite catalyst facilitates the deeper understanding of the reaction mechanism and clarifies the principle for catalyst design.