New mechanistic insights in the NH3-SCR reactions at low temperature

Ruggeri, Maria Pia; Selleri, Tomasso; Nova, Isabella; Tronconi, Enrico; Pihl, Josh A.; Toops, Todd J.; Partridge, Jr., William P.

doi:10.1007/s11244-016-0567-1

Title: New mechanistic insights in the NH₃-SCR reactions at low temperature

Journal Article · Fri May 06 00:00:00 EDT 2016 · Topics in Catalysis

DOI:https://doi.org/10.1007/s11244-016-0567-1· OSTI ID:1295099

Ruggeri, Maria Pia ^[1]; Selleri, Tomasso ^[1]; Nova, Isabella ^[1]; Tronconi, Enrico ^[1]; Pihl, Josh A. ^[2]; Toops, Todd J. ^[2]; Partridge, Jr., William P. ^[2]

Politecnico di Milano (Italy). Dipartimento di Energia
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Fuels Engines and Emissions Research Center

The present study is focused on the investigation of the low temperature Standard SCR reaction mechanism over Fe- and Cu-promoted zeolites. Different techniques are employed, including in situ DRIFTS, transient reaction analysis and chemical trapping techniques. The results present strong evidence of nitrite formation in the oxidative activation of NO and of their role in SCR reactions. These elements lead to a deeper understanding of the standard SCR chemistry at low temperature and can potentially improve the consistency of mechanistic mathematical models. Furthermore, comprehension of the mechanism on a fundamental level can contribute to the development of improved SCR catalysts.

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Research Organization:: Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Fuels, Engines and Emissions Research Center (FEERC); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). National Transportation Research Center (NTRC)

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

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1295099

Journal Information:: Topics in Catalysis, Vol. 59, Issue 10-12; ISSN 1022-5528

Publisher:: SpringerCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 14 works

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References (13)

A Common Intermediate for N ₂ Formation in Enzymes and Zeolites: Side-On Cu-Nitrosyl Complexes Kwak, Ja Hun; Lee, Jong H.; Burton, Sarah D. Angewandte Chemie International Edition, Vol. 52, Issue 38 https://doi.org/10.1002/anie.201303498	journal	August 2013
Experimental Study of the NO Oxidation to NO2 Over Metal Promoted Zeolites Aimed at the Identification of the Standard SCR Rate Determining Step Ruggeri, Maria Pia; Nova, Isabella; Tronconi, Enrico Topics in Catalysis, Vol. 56, Issue 1-8 https://doi.org/10.1007/s11244-013-9937-0	journal	February 2013
Operando Spatially- and Time-Resolved XAS Study on Zeolite Catalysts for Selective Catalytic Reduction of NO _x by NH ₃ Doronkin, Dmitry E.; Casapu, Maria; Günter, Tobias The Journal of Physical Chemistry C, Vol. 118, Issue 19 https://doi.org/10.1021/jp5028433	journal	May 2014
In Situ-DRIFTS Study of Selective Catalytic Reduction of NO _x by NH ₃ over Cu-Exchanged SAPO-34 Wang, Di; Zhang, Li; Kamasamudram, Krishna ACS Catalysis, Vol. 3, Issue 5 https://doi.org/10.1021/cs300843k	journal	April 2013
In-situ DRIFTS measurements for the mechanistic study of NO oxidation over a commercial Cu-CHA catalyst Ruggeri, Maria Pia; Nova, Isabella; Tronconi, Enrico Applied Catalysis B: Environmental, Vol. 166-167 https://doi.org/10.1016/j.apcatb.2014.10.076	journal	May 2015
Investigation of NO2 and NO interaction with an Fe-ZSM-5 catalyst by transient response methods and chemical trapping techniques Ruggeri, Maria Pia; Selleri, Tommaso; Colombo, Massimo Journal of Catalysis, Vol. 328 https://doi.org/10.1016/j.jcat.2015.02.003	journal	August 2015
Identification of nitrites/HONO as primary products of NO oxidation over Fe-ZSM-5 and their role in the Standard SCR mechanism: A chemical trapping study Ruggeri, Maria Pia; Selleri, Tommaso; Colombo, Massimo Journal of Catalysis, Vol. 311 https://doi.org/10.1016/j.jcat.2013.11.028	journal	March 2014
A comparative study of the NH3-SCR reactions over a Cu-zeolite and a Fe-zeolite catalyst Colombo, Massimo; Nova, Isabella; Tronconi, Enrico Catalysis Today, Vol. 151, Issue 3-4 https://doi.org/10.1016/j.cattod.2010.01.010	journal	June 2010
Selective Catalytic Reduction of NO _x over H-ZSM-5 Under Lean Conditions Using Transient NH ₃ Supply Wallin, Mikaela; Karlsson, Carl-Johan; Palmqvist, Anders Topics in Catalysis, Vol. 30/31 https://doi.org/10.1023/B:TOCA.0000029737.89510.22	journal	July 2004
Detailed kinetic modeling of NH3 SCR over Cu-ZSM-5 Sjövall, Hanna; Blint, Richard J.; Olsson, Louise Applied Catalysis B: Environmental, Vol. 92, Issue 1-2 https://doi.org/10.1016/j.apcatb.2009.07.020	journal	October 2009
In situ DRIFTS-MS studies on the oxidation of adsorbed NH3 by NOx over a Cu-SSZ-13 zeolite Zhu, Haiyang; Kwak, Ja Hun; Peden, Charles H. F. Catalysis Today, Vol. 205 https://doi.org/10.1016/j.cattod.2012.08.043	journal	April 2013
NO2 adsorption on Fe- and Cu-zeolite catalysts: The effect of the catalyst red–ox state Colombo, Massimo; Nova, Isabella; Tronconi, Enrico Applied Catalysis B: Environmental, Vol. 111-112 https://doi.org/10.1016/j.apcatb.2011.10.031	journal	January 2012
NH3–NO/NO2 SCR for Diesel Exhausts Aftertreatment: Reactivity, Mechanism and Kinetic Modelling of Commercial Fe- and Cu-Promoted Zeolite Catalysts Grossale, Antonio; Nova, Isabella; Tronconi, Enrico Topics in Catalysis, Vol. 52, Issue 13-20 https://doi.org/10.1007/s11244-009-9354-6	journal	July 2009

Cited By (4)

Analysis of AdSCR Systems for NOx Removal During the Cold-Start Period of Diesel Engines Gramigni, Federica; Selleri, Tommaso; Nova, Isabella Topics in Catalysis, Vol. 62, Issue 1-4 https://doi.org/10.1007/s11244-019-01138-5	journal	January 2019
A PGM-free NO _x adsorber + selective catalytic reduction catalyst system (AdSCR) for trapping and reducing NO _x in lean exhaust streams at low temperature Selleri, Tommaso; Gramigni, Federica; Nova, Isabella Catalysis Science & Technology, Vol. 8, Issue 9 https://doi.org/10.1039/c8cy00343b	journal	January 2018
Temperature-dependent dynamics of NH ₃ -derived Cu species in the Cu-CHA SCR catalyst Borfecchia, Elisa; Negri, Chiara; Lomachenko, Kirill A. Reaction Chemistry & Engineering, Vol. 4, Issue 6 https://doi.org/10.1039/c8re00322j	journal	January 2019
Catalyst systems for selective catalytic reduction + NO x trapping: from fundamental understanding of the standard SCR reaction to practical applications for lean exhaust after-treatment Gramigni, Federica; Selleri, Tommaso; Nova, Isabella Reaction Chemistry & Engineering, Vol. 4, Issue 7 https://doi.org/10.1039/c9re00012g	journal	January 2019

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Title: New mechanistic insights in the NH3-SCR reactions at low temperature

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Title: New mechanistic insights in the NH₃-SCR reactions at low temperature