A redox model for NO oxidation, NH3 oxidation and high temperature standard SCR over Cu-SSZ-13

Daya, Rohil; Deka, Dhruba J.; Goswami, Anshuman; Menon, Unmesh; Trandal, Dylan; Partridge, William P.; Joshi, Saurabh Y.

doi:10.1016/j.apcatb.2023.122524

Title: A redox model for NO oxidation, NH₃ oxidation and high temperature standard SCR over Cu-SSZ-13

Journal Article · Sat Jul 01 00:00:00 EDT 2023 · Applied Catalysis. B, Environmental

DOI:https://doi.org/10.1016/j.apcatb.2023.122524· OSTI ID:1959607

^[1]; Deka, Dhruba J. ^[2]; Goswami, Anshuman ^[3]; Menon, Unmesh ^[1]; Trandal, Dylan ^[1];

^[2]; Joshi, Saurabh Y. ^[1]

Cummins, Columbus, IN (United States)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
University of Notre Dame, IN (United States)

A kinetic model is developed to predict the influence of temperature and hydrothermal aging on the redox of active Cu sites under standard SCR, NO oxidation and NH₃ oxidation conditions over a practically relevant fully-formulated Cu-SSZ-13 catalyst. NO₂/N₂ production during NO/NH₃ titration of Cu^II sites is utilized to identify rate parameters associated with NO-only RHC (reduction half cycle) and NH₃-only RHC respectively. Integral N₂ formation during subsequent NO + NH₃ titration is consistent with the production of one NO₂ per two CuII sites reduced during NO-only RHC and one N₂ per six Cu^II sites reduced during NH₃-only RHC. Decreased reduction of Cu^II sites by NO/NH³ upon hydrothermal aging, along with the production of one NO₂ per two CuII sites during NO-only RHC, is accordant with the involvement of proximal ZCuOH and oxygen-bridged dimeric Cu^II sites. Oxidation of partially solvated and framework coordinated ZCu (Cu^I) sites occurs in presence of O₂, does not produce N₂ and can lead to the consumption of Brønsted acid sites. A global OHC kinetic model is developed to predict transient and integral N₂ formation during exposure of CuI sites to a mixture of NO and O₂. The resulting redox kinetic model quantitatively predicts NO and NH₃ consumption during isothermal transient response Cu redox (TRCR) protocols, along with temperature and age dependent steady-state standard SCR and oxidation conditions. The redox model presented in this work synthesizes recent kinetic, spectroscopic and computational findings to provide a foundational description of active site redox during standard SCR, NO oxidation and NH3 oxidation over Cu-SSZ-13.

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

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1959607

Journal Information:: Applied Catalysis. B, Environmental, Vol. 328, Issue 1; ISSN 0926-3373

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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Title: A redox model for NO oxidation, NH3 oxidation and high temperature standard SCR over Cu-SSZ-13

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Title: A redox model for NO oxidation, NH₃ oxidation and high temperature standard SCR over Cu-SSZ-13