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Detection of key transient Cu intermediates in SSZ-13 during NH3-SCR deNOx by modulation excitation IR spectroscopy

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Abstract

The small pore zeolite Cu-SSZ-13 is an efficient material for the standard selective catalytic reduction of nitrogen oxides (NOx) by ammonia (NH3). In this work, Cu-SSZ-13 has been studied at 250 °C under high conversion using a modulation excitation approach and analysed with phase sensitive detection (PSD). While the complementary X-ray absorption near edge structure (XANES) spectroscopy measurements showed that the experiments were performed under cyclic Cu+/Cu2+ redox, Diffuse Reflectance Infrared Fourier Transform Spectroscopy (DRIFTS) experiments provide spectroscopic evidence for previously postulated intermediates Cu–N([double bond, length as m-dash]O)–NH2 and Cu–NO3 in the NH3-SCR deNOx mechanism and for the role of [Cu2+(OH)]+. These results therefore help in building towards a more comprehensive understanding of the reaction mechanism which to date has only been postulated in silico.

Graphical abstract: Detection of key transient Cu intermediates in SSZ-13 during NH3-SCR deNOx by modulation excitation IR spectroscopy

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Publication details

The article was received on 29 Sep 2019, accepted on 15 Nov 2019 and first published on 18 Nov 2019


Article type: Edge Article
DOI: 10.1039/C9SC04905C
Chem. Sci., 2020, Advance Article
  • Open access: Creative Commons BY license
    All publication charges for this article have been paid for by the Royal Society of Chemistry

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    Detection of key transient Cu intermediates in SSZ-13 during NH3-SCR deNOx by modulation excitation IR spectroscopy

    A. G. Greenaway, A. Marberger, A. Thetford, I. Lezcano-González, M. Agote-Arán, M. Nachtegaal, D. Ferri, O. Kröcher, C. R. A. Catlow and A. M. Beale, Chem. Sci., 2020, Advance Article , DOI: 10.1039/C9SC04905C

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