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Issue 21, 2017
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Influence of the nature and environment of manganese in Mn-BEA zeolites on NO conversion in selective catalytic reduction with ammonia

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Abstract

Manganese-containing BEA zeolites, MnxSiBEA (x = 1–4 wt%) and Mn(I.E.)AlBEA, were prepared by a two-step post-synthesis method and a conventional wet ion-exchange, respectively, and applied as catalysts in the selective catalytic reduction of NO with ammonia (NH3-SCR). The physicochemical analysis of zeolite properties by high-energy-resolution fluorescence-detected XANES (HERFD-XANES) and X-ray emission spectroscopy (XES) uncovered that the coordination, geometry and oxidation state of Mn species are strongly related to the preparation method. Additionally, the study of catalyst acidity by FTIR spectroscopy with CO and pyridine probe molecules provided important insight into the number and type of acidic centres present on the catalyst surface. The catalytic results revealed that NO conversion depended on the state and content of Mn. The zeolites obtained by the two-step post-synthesis method and with a low Mn content were very active in the medium temperature range (NO conversion ∼100%) with simultaneous high selectivity to N2 due to the presence of isolated, framework Mn(III) and Mn(II) species. The N2O formation was especially high in the case of catalysts containing extra-framework polynuclear Mn species and negligible in the case of Mn(I.E.)AlBEA containing predominantly isolated, extra-framework Mn(II) species.

Graphical abstract: Influence of the nature and environment of manganese in Mn-BEA zeolites on NO conversion in selective catalytic reduction with ammonia

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Supplementary files

Article information


Submitted
31 Mar 2017
Accepted
27 Apr 2017
First published
17 May 2017

Phys. Chem. Chem. Phys., 2017,19, 13553-13561
Article type
Paper

Influence of the nature and environment of manganese in Mn-BEA zeolites on NO conversion in selective catalytic reduction with ammonia

R. Baran, L. Valentin, J.-M. Krafft, T. Grzybek, P. Glatzel and S. Dzwigaj, Phys. Chem. Chem. Phys., 2017, 19, 13553
DOI: 10.1039/C7CP02096A

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