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Infrared Evidence for the Existence of Nitrate Species on Cu-ZSM5 During Isothermal Rate Oscillations in the Decomposition of N2O

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Abstract

Isothermal oscillations in the rate of decomposition of N2O were studied on an over-exchanged Cu-ZSM-5 catalyst by mass spectroscopy and in situ transient FTIR. Oscillations in the production of O2 and N2 were observed to occur in a temperature range of 410–490°C at a total pressure of 1.0 Torr pure N2O. FTIR has provided the first spectroscopic evidence that surface nitrate species are present under oscillatory conditions. This study confirmed a previously proposed model that predicts a slow build-up of surface nitrates, followed by a rapid nitrate decomposition coupled with an increase in the rate of N2O decomposition. The IR signature of the surface nitrates suggests they are monodentate nitrate species bound to Cu2+ ions. Temperature-programmed desorption studies reveal a strong correlation between the stability of the surface nitrate species and the temperature range in which oscillations occur.

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Authors and Affiliations

  1. School of Chemical Engineering, Purdue University, West Lafayette, IN, 47907-1283, USA

    Paul T. Fanson, Martin W. Stradt, W. Nicholas Delgass & Jochen Lauterbach

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  1. Paul T. Fanson
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  2. Martin W. Stradt
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  3. W. Nicholas Delgass
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  4. Jochen Lauterbach
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Fanson, P.T., Stradt, M.W., Delgass, W.N. et al. Infrared Evidence for the Existence of Nitrate Species on Cu-ZSM5 During Isothermal Rate Oscillations in the Decomposition of N2O. Catalysis Letters 77, 15–19 (2001). https://doi.org/10.1023/A:1012726809704

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