Assessing impact of real-world aging on Cu-redox half cycles of a Cu-SSZ-13 SCR catalyst via transient response measurements and kinetic modeling

Deka, Dhruba J.; Daya, Rohil; Ladshaw, Austin P.; Trandal, Dylan; Joshi, Saurabh Y.; Partridge, Jr, William P.

doi:10.1016/j.apcatb.2022.121233

Assessing impact of real-world aging on Cu-redox half cycles of a Cu-SSZ-13 SCR catalyst via transient response measurements and kinetic modeling

Journal Article · Wed Feb 23 00:00:00 EST 2022 · Applied Catalysis. B, Environmental

DOI:https://doi.org/10.1016/j.apcatb.2022.121233· OSTI ID:1854464

Deka, Dhruba J. ^[1]; Daya, Rohil ^[2]; ^[1]; Trandal, Dylan ^[2]; Joshi, Saurabh Y. ^[2]; ^[1]

Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Cummins Inc., Columbus, IN (United States)

We report that the SCR reaction on Cu-SSZ-13 is a redox process consisting of a reduction half-cycle (RHC) and an oxidation half-cycle (OHC). Despite extensive efforts to understand hydrothermal aging and sulfur poisoning, the impact of real-world aging on the SCR activity of Cu-SSZ-13 has not been reported. This work employs a transient response methodology consisting of experiments and kinetic models to investigate the SCR redox cycles at intra-catalyst locations of commercial Cu-SSZ-13 monolith catalysts in their degreened and real-world aged states, in the temperature range of 200–450 °C. Moreover, H₂-TPR, NH₃-TPD, SO₂-TPD, ICP-OES and solid-state NMR were performed to investigate the catalyst properties. Sulfur aging and dealumination caused by real-world exposure decreased the reducible Cu density and SCR performance. Real-world aging was found to selectively slow OHC more than RHC, mainly due to lower mobility of the Cu ions coordinated to sulfur-related species leading to decreased formation of Cu-dimers necessary for OHC.

View Accepted Manuscript (DOE)

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Vehicle Technologies Office

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1854464

Journal Information:: Applied Catalysis. B, Environmental, Journal Name: Applied Catalysis. B, Environmental Journal Issue: 1 Vol. 309; ISSN 0926-3373

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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Assessing impact of real-world aging on Cu-redox half cycles of a Cu-SSZ-13 SCR catalyst via transient response measurements and kinetic modeling

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