Study of N2O Formation over Rh- and Pt-Based LNT Catalysts

In this paper, mechanistic aspects involved in the formation of N2O over Pt-BaO/Al2O3 and Rh-BaO/Al2O3 model NOx Storage-Reduction (NSR) catalysts are discussed. The reactivity of both gas-phase NO and stored nitrates was investigated by using H2 and NH3 as reductants. It was found that N2O formatio...

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Main Authors: Lukasz Kubiak, Roberto Matarrese, Lidia Castoldi, Luca Lietti, Marco Daturi, Pio Forzatti
Format: Article
Language:English
Published: MDPI AG 2016-03-01
Series:Catalysts
Subjects:
Online Access:http://www.mdpi.com/2073-4344/6/3/36
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spelling doaj-cfc199e42e10405ca1cb3ec9c458df9a2020-11-24T20:59:23ZengMDPI AGCatalysts2073-43442016-03-01633610.3390/catal6030036catal6030036Study of N2O Formation over Rh- and Pt-Based LNT CatalystsLukasz Kubiak0Roberto Matarrese1Lidia Castoldi2Luca Lietti3Marco Daturi4Pio Forzatti5Laboratory of Catalysis and Catalytic Processes, Dipartimento di Energia, Politecnico di Milano, Via La Masa, 34, 20156 Milano, ItalyLaboratory of Catalysis and Catalytic Processes, Dipartimento di Energia, Politecnico di Milano, Via La Masa, 34, 20156 Milano, ItalyLaboratory of Catalysis and Catalytic Processes, Dipartimento di Energia, Politecnico di Milano, Via La Masa, 34, 20156 Milano, ItalyLaboratory of Catalysis and Catalytic Processes, Dipartimento di Energia, Politecnico di Milano, Via La Masa, 34, 20156 Milano, ItalyLaboratoire Catalyse et Spectrochimie, ENSICAEN, Université de Caen, CNRS, 6 Bd du Maréchal Juin, 14050 Caen, FranceLaboratory of Catalysis and Catalytic Processes, Dipartimento di Energia, Politecnico di Milano, Via La Masa, 34, 20156 Milano, ItalyIn this paper, mechanistic aspects involved in the formation of N2O over Pt-BaO/Al2O3 and Rh-BaO/Al2O3 model NOx Storage-Reduction (NSR) catalysts are discussed. The reactivity of both gas-phase NO and stored nitrates was investigated by using H2 and NH3 as reductants. It was found that N2O formation involves the presence of gas-phase NO, since no N2O is observed upon the reduction of nitrates stored over both Pt- and Rh-BaO/Al2O3 catalyst samples. In particular, N2O formation involves the coupling of undissociated NO molecules with N-adspecies formed upon NO dissociation onto reduced Platinum-Group-Metal (PGM) sites. Accordingly, N2O formation is observed at low temperatures, when PGM sites start to be reduced, and disappears at high temperatures where PGM sites are fully reduced and complete NO dissociation takes place. Besides, N2O formation is observed at lower temperatures with H2 than with NH3 in view of the higher reactivity of hydrogen in the reduction of the PGM sites and onto Pt-containing catalyst due to the higher reducibility of Pt vs. Rh.http://www.mdpi.com/2073-4344/6/3/36lean NOx trapN2O formationNOx storage reductionPt-BaO/Al2O3Rh-BaO/Al2O3
collection DOAJ
language English
format Article
sources DOAJ
author Lukasz Kubiak
Roberto Matarrese
Lidia Castoldi
Luca Lietti
Marco Daturi
Pio Forzatti
spellingShingle Lukasz Kubiak
Roberto Matarrese
Lidia Castoldi
Luca Lietti
Marco Daturi
Pio Forzatti
Study of N2O Formation over Rh- and Pt-Based LNT Catalysts
Catalysts
lean NOx trap
N2O formation
NOx storage reduction
Pt-BaO/Al2O3
Rh-BaO/Al2O3
author_facet Lukasz Kubiak
Roberto Matarrese
Lidia Castoldi
Luca Lietti
Marco Daturi
Pio Forzatti
author_sort Lukasz Kubiak
title Study of N2O Formation over Rh- and Pt-Based LNT Catalysts
title_short Study of N2O Formation over Rh- and Pt-Based LNT Catalysts
title_full Study of N2O Formation over Rh- and Pt-Based LNT Catalysts
title_fullStr Study of N2O Formation over Rh- and Pt-Based LNT Catalysts
title_full_unstemmed Study of N2O Formation over Rh- and Pt-Based LNT Catalysts
title_sort study of n2o formation over rh- and pt-based lnt catalysts
publisher MDPI AG
series Catalysts
issn 2073-4344
publishDate 2016-03-01
description In this paper, mechanistic aspects involved in the formation of N2O over Pt-BaO/Al2O3 and Rh-BaO/Al2O3 model NOx Storage-Reduction (NSR) catalysts are discussed. The reactivity of both gas-phase NO and stored nitrates was investigated by using H2 and NH3 as reductants. It was found that N2O formation involves the presence of gas-phase NO, since no N2O is observed upon the reduction of nitrates stored over both Pt- and Rh-BaO/Al2O3 catalyst samples. In particular, N2O formation involves the coupling of undissociated NO molecules with N-adspecies formed upon NO dissociation onto reduced Platinum-Group-Metal (PGM) sites. Accordingly, N2O formation is observed at low temperatures, when PGM sites start to be reduced, and disappears at high temperatures where PGM sites are fully reduced and complete NO dissociation takes place. Besides, N2O formation is observed at lower temperatures with H2 than with NH3 in view of the higher reactivity of hydrogen in the reduction of the PGM sites and onto Pt-containing catalyst due to the higher reducibility of Pt vs. Rh.
topic lean NOx trap
N2O formation
NOx storage reduction
Pt-BaO/Al2O3
Rh-BaO/Al2O3
url http://www.mdpi.com/2073-4344/6/3/36
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