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Title: New operando method for quantifying the relative half-cycle rates of the NO SCR redox cycle over Cu-exchanged zeolites

An operando experimental method for monitoring relative variations in half-cycle rates of the Cu redox-cycle model of selective-catalytic-reduction (SCR) is demonstrated, along with a kinetic model for predicting the same. Conversion inflections (CI) can occur at SCR onset within Cu/SCR catalysts; transient CI involves initial conversion growth to an intermediate value greater than exists at steady state (SS) before degrading to the SS value. While similar CI has been reported for Fe/SCR catalysts as being due to NH 3 inhibition, Cu/SCR CI is inconsistent with a similar origin. Rather, Cu/SCR CI is due to imbalances in the redox-half-cycle rates, and will occur when reduction is faster than oxidation. The temporal CI shape varies with the redox-cycle kinetic parameters and model formulation, and can be used to study the same. Here, we demonstrate the first measurements of dynamic half-cycle rate balancing at SCR onset, use CI and onset transients to study variations in half-cycle rates under Standard, Fast and NO 2 SCR, and present the first redox-cycle model showing CI. The new operando method and model provides a basis for better understanding the SCR redox process, and determining the individual half-cycles kinetic model formulation and parameters.
Authors:
ORCiD logo [1] ;  [2] ; ORCiD logo [1] ;  [2]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  2. Cummins Inc., Columbus, IN (United States)
Publication Date:
Grant/Contract Number:
AC05-00OR22725
Type:
Accepted Manuscript
Journal Name:
Applied Catalysis. B, Environmental
Additional Journal Information:
Journal Volume: 236; Journal Issue: C; Journal ID: ISSN 0926-3373
Publisher:
Elsevier
Research Org:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org:
USDOE Office of Energy Efficiency and Renewable Energy (EERE)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; NH3SCR; Cu redox half cycles; Kinetic model; Operando SpaciMS
OSTI Identifier:
1458371

Partridge, William P., Joshi, Saurabh Y., Pihl, Josh A., and Currier, Neal W.. New operando method for quantifying the relative half-cycle rates of the NO SCR redox cycle over Cu-exchanged zeolites. United States: N. p., Web. doi:10.1016/j.apcatb.2018.04.071.
Partridge, William P., Joshi, Saurabh Y., Pihl, Josh A., & Currier, Neal W.. New operando method for quantifying the relative half-cycle rates of the NO SCR redox cycle over Cu-exchanged zeolites. United States. doi:10.1016/j.apcatb.2018.04.071.
Partridge, William P., Joshi, Saurabh Y., Pihl, Josh A., and Currier, Neal W.. 2018. "New operando method for quantifying the relative half-cycle rates of the NO SCR redox cycle over Cu-exchanged zeolites". United States. doi:10.1016/j.apcatb.2018.04.071.
@article{osti_1458371,
title = {New operando method for quantifying the relative half-cycle rates of the NO SCR redox cycle over Cu-exchanged zeolites},
author = {Partridge, William P. and Joshi, Saurabh Y. and Pihl, Josh A. and Currier, Neal W.},
abstractNote = {An operando experimental method for monitoring relative variations in half-cycle rates of the Cu redox-cycle model of selective-catalytic-reduction (SCR) is demonstrated, along with a kinetic model for predicting the same. Conversion inflections (CI) can occur at SCR onset within Cu/SCR catalysts; transient CI involves initial conversion growth to an intermediate value greater than exists at steady state (SS) before degrading to the SS value. While similar CI has been reported for Fe/SCR catalysts as being due to NH3 inhibition, Cu/SCR CI is inconsistent with a similar origin. Rather, Cu/SCR CI is due to imbalances in the redox-half-cycle rates, and will occur when reduction is faster than oxidation. The temporal CI shape varies with the redox-cycle kinetic parameters and model formulation, and can be used to study the same. Here, we demonstrate the first measurements of dynamic half-cycle rate balancing at SCR onset, use CI and onset transients to study variations in half-cycle rates under Standard, Fast and NO2 SCR, and present the first redox-cycle model showing CI. The new operando method and model provides a basis for better understanding the SCR redox process, and determining the individual half-cycles kinetic model formulation and parameters.},
doi = {10.1016/j.apcatb.2018.04.071},
journal = {Applied Catalysis. B, Environmental},
number = C,
volume = 236,
place = {United States},
year = {2018},
month = {5}
}