Moreno González, M.; Hueso Fuentes, B.; Boronat Zaragoza, M.; Blasco Lanzuela, T.; Corma Canós, A. (2015). Ammonia-Containing Species Formed in Cu-Chabazite As Per In SituEPR, Solid-State NMR, and DFT Calculations. Journal of Physical Chemistry Letters. 6(6):1011-1017. https://doi.org/10.1021/acs.jpclett.5b00069
Por favor, use este identificador para citar o enlazar este ítem: http://hdl.handle.net/10251/78062
Title:
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Ammonia-Containing Species Formed in Cu-Chabazite As Per In SituEPR, Solid-State NMR, and DFT Calculations
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Author:
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Moreno González, Marta
Hueso Fuentes, Beatriz
Boronat Zaragoza, Mercedes
Blasco Lanzuela, Teresa
Corma Canós, Avelino
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UPV Unit:
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Universitat Politècnica de València. Escuela Técnica Superior de Ingenieros Industriales - Escola Tècnica Superior d'Enginyers Industrials
Universitat Politècnica de València. Instituto Universitario Mixto de Tecnología Química - Institut Universitari Mixt de Tecnologia Química
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Issued date:
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Abstract:
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Nowadays, the most attractive technology for the elimination of nitric oxides
from the exhaust gas of diesel vehicles is the selective catalytic reduction with ammonia
(NH3-SCR-NOx) using Cu zeolite with the chabazite ...[+]
Nowadays, the most attractive technology for the elimination of nitric oxides
from the exhaust gas of diesel vehicles is the selective catalytic reduction with ammonia
(NH3-SCR-NOx) using Cu zeolite with the chabazite structure as the catalyst. Isolated
copper species are the active sites, but the reaction intermediates and the overall reaction
mechanism are still under debate. Here, we study the interaction of ammonia with zeolite
Cu-SSZ-13 (CHA topology) with a uniform distribution of Cu2+ sites prepared in one pot
and a conventional Cu-ZSM-5 (MFI topology) for comparison. In situ EPR and solid-state
NMR spectroscopies combined with DFT calculations have allowed the identification of
NH4+, [Cu(NH3)5]2+, [Cu(Of)2(NH3)2]2+, [Cu(Of)3NH3]2+, [Cu(NH3)2]+, and
[CuOf(NH3)]+ (Of being framework oxygen) under different conditions. The results
demonstrate that ammonia is able to reduce Cu2+ to Cu+ and provide new information on
the species formed in Cu-SSZ-13, which have important implications for the elucidation of
the SCR reaction mechanism.
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Subjects:
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Chabazite
,
EPR
,
NMR
,
DFT
,
Nitric oxides
,
ZSM-5
,
SCR.
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Copyrigths:
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Cerrado |
Source:
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Journal of Physical Chemistry Letters. (issn:
1948-7185
)
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DOI:
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10.1021/acs.jpclett.5b00069
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Publisher:
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American Chemical Society
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Publisher version:
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http://dx.doi. org/10.1021/acs.jpclett.5b00069
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Project ID:
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info:eu-repo/grantAgreement/MINECO//SEV-2012-0267/
info:eu-repo/grantAgreement/MINECO//MAT2012-38567-C02-01/ES/MATERIALES ZEOLITICOS COMO ESTRUCTURAS ANFITRIONAS DE NANOPARTICULAS. SINTESIS Y APLICACIONES NANOTECNOLOGICAS, CATALITICAS Y MEDIOAMBIENTALES/
info:eu-repo/grantAgreement/MICINN//CSD2009-00050/ES/Desarrollo de catalizadores más eficientes para el diseño de procesos químicos sostenibles y produccion limpia de energia/
/
info:eu-repo/grantAgreement/GVA//PROMETEOII%2F2013%2F011/ES/Catalizadores moleculares y supramoleculares altamente selectivos, estables y energéticamente eficientes en reacciones químicas (PROMETEO)/
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Thanks:
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The authors acknowledge financial support from the Spanish Ministry of Economy and Competitiveness through the Severo Ochoa program (SEV-2012-0267) and operating grants Consolider Ingenio Multicat CSD-2009-00050, ...[+]
The authors acknowledge financial support from the Spanish Ministry of Economy and Competitiveness through the Severo Ochoa program (SEV-2012-0267) and operating grants Consolider Ingenio Multicat CSD-2009-00050, MAT-2012-3856-C02-01, as well as Generalitat Valenciana through the PROMETEOII/2013/011 Project. Red Espanola de Super-computacion (RES) and Centre de Calcul de la Universitat de Valencia are gratefully acknowledged for computational facilities and technical assistance. M.M. and B.H. thank ITQ for grants.
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Type:
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Artículo
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