N2O decomposition over Fe-zeolites: Structure of the active sites and the origin of the distinct reactivity of Fe-ferrierite, Fe-ZSM-5, and Fe-beta. A combined periodic DFT and multispectral study

Sklenák, Štěpán; Andrikopoulos, Prokopis C.; Boekfa, Bundet; Jansang, Bavornpon; Nováková, J.; Benco, Ľ.; Bučko, Tomáš; Hafner, J.; Dědeček, Jiřı́; Sobalı́k, Zdenĕk

doi:10.1016/j.jcat.2010.04.008

Cited by 119 publications

(189 citation statements)

References 59 publications

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“…Up to now, many catalytic systems such as noble metals [5,6,7], metal oxides [8,9,10], ion-exchanged zeolites, calcined hydrotalcites [ [11,12,13], mesoporous silicas [14,15] were investigated for the low temperature deN 2 O reaction. One of the simple promising generic systems exhibiting high catalytic activity in this reaction is cobalt spinel [16,17,18,19,20], which can be additionally modified by structural [21,22,23,24] and surface donation [24,25,26,27,28] …”

Section: Introductionmentioning

confidence: 99%

Strong dispersion effect of cobalt spinel active phase spread over ceria for catalytic N2O decomposition: The role of the interface periphery

Grzybek

Stelmachowski

Gudyka

et al. 2016

Applied Catalysis B: Environmental

103

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dispersion effect of cobalt spinel active phase spread over ceria for catalytic N2O decomposition: the role of the interface periphery, Applied Catalysis B, Environmental http://dx.doi.org/10. 1016/j.apcatb.2015.07.027 This is a PDF file of an unedited manuscript that has been accepted for publication. As a service to our customers we are providing this early version of the manuscript. The manuscript will undergo copyediting, typesetting, and review of the resulting proof before it is published in its final form. Please note that during the production process errors may be discovered which could affect the content, and all legal disclaimers that apply to the journal pertain. The catalytic tests in deN 2 O reaction revealed that the 10 wt.% of cobalt spinel in supported system is able to reproduce the activity of bare Co 3 O 4 catalyst. However, it was found that the catalyst with the lowest content of Co 3 O 4 equal to 1 wt.% exhibits the highest apparent reaction rate per mass of the spinel active phase. The observed activity was explained basing on the transmission electron microscopy analysis in terms of the dispersion of spinel phase over ceria support. A simple model that accounts for the observed strong dispersion effect is proposed. It consists in a two-step mechanism, where N 2 O is dissociated on the spinel nanograins and the resultant oxygen species are preferentially recombined at the Co 3 O 4 /CeO 2 interface periphery.

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Section: Introductionmentioning

confidence: 99%

Strong dispersion effect of cobalt spinel active phase spread over ceria for catalytic N2O decomposition: The role of the interface periphery

Grzybek

Stelmachowski

Gudyka

et al. 2016

Applied Catalysis B: Environmental

103

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“…Anthropogenic N 2 O comes from the combustion of fossil fuels and biomass, the production of nitric and adipic acids, the use of nitrogen fertilizers, etc. Concerning the catalytic decomposition of N 2 O over Fe-containing zeolites, the influence of preparation methods [34][35][36][37][38], topology of zeolites [39,40], Fe content [14,[41][42][43], activation conditions (e.g., temperature [44,45], ambient/atmosphere [45,46]), and co-fed gases (O 2 , H 2 O, and NO) [23,47,48], as well as reaction mechanisms and kinetics [47,[49][50][51] have been studied in detail. However, the nature of active Fe species is still controversial.…”

Section: Introductionmentioning

confidence: 99%

Catalytic decomposition of N2O over Fe-ZSM-11 catalysts prepared by different methods: Nature of active Fe species

Xie

Luo

Ma³

et al. 2015

Journal of Catalysis

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“…Na busca por catalisadores ativos, seletivos, estáveis e de baixo custo para a de-N 2 O, tem se destacado os estudos usando zeólitas [15,16]. As zeólitas trocadas com íons de metais de transição são excelentes candidatos para a reação de-N 2 O. Os cátions de ferro, cobalto e cobre são geralmente os mais empregados, devido às altas atividades na decomposição dos óxidos de nitrogênio [17,18].…”

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“…A zeólita ZSM-5 tem sido a mais estudada e os estudos experimentais e teóricos da de-N 2 O sobre Fe-ZSM-5 têm se concentrado sobre a influência do método de preparação, pré-tratamento e as propriedades dos sítios ativos [20]. Estudos incipientes com a zeólita BETA têm mostrado características atraentes e vantajosas desse material para a catálise, como: ampla abertura de poros, grande área específica, alta estabilidade térmica e hidrotérmica e seletividade de forma [15,20].…”

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Estudo do desempenho catalítico das zeólitas Beta e ZSM-5 contendo ferro para decomposição de óxido nitroso

Moura

Batista

2017

Matéria (Rio J.)

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RESUMOCatalisadores Fe-ZSM-5 tem mostrado alta atividade para decomposição de N 2 O (de-N 2 O), mas poucos trabalhos apresentam o seu desempenho junto com gases que coexistem nas emissões (CO 2 Palavras-chave: óxido nitroso, catalisador, Fe-ZSM-5, Fe-BETA. ABSTRACTFe-ZSM-5 catalysts has shown high activity for decomposition of N 2 O (de-N 2 O), but few works show their performance with coexisting gas emissions (CO 2 , CH 4 , O 2 and H 2 O). Recently, Fe-BETA presented N 2 O conversion more high than Fe-ZSM-5, however, the activity of these catalysts still needs to compare in real conditions. This work aims to study the performance of Fe-BETA, Fe-ZSM-5 and Fe 2 O 3 in the de-N 2 O with addition of gases present in real conditions. For this, Fe-BETA (prepared by ion exchange), Fe-ZSM-5 and Fe 2 O 3 catalysts were calcined, characterized by XRF, XRD and H 2 -TPR and, evaluated in the N 2 O decomposition in the presence of CO 2 , CH 4 , O 2 and H 2 O. The results showed the presence of iron oxide on surface and iron ions compensating load in the structure of the zeolites. The N 2 O conversion increased with increasing reaction temperature and the Fe-ZSM-5 and Fe-BETA catalysts were much more active than Fe 2 O 3 pure. These results show that the iron species in the exchange position of zeolites are the most active for the reaction of N 2 O decomposition. The Fe-ZSM-5 and Fe-BETA catalysts showed high activity (> 90%) and resistance in the presence of CO 2 , CH 4 , O 2 and H 2 O. Fe-BETA was more selective the reaction of decomposition of N 2 O and showed great potential for the reduction of N 2 O emissions in real conditions.

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N2O decomposition over Fe-zeolites: Structure of the active sites and the origin of the distinct reactivity of Fe-ferrierite, Fe-ZSM-5, and Fe-beta. A combined periodic DFT and multispectral study

Cited by 119 publications

References 59 publications

Strong dispersion effect of cobalt spinel active phase spread over ceria for catalytic N2O decomposition: The role of the interface periphery

Strong dispersion effect of cobalt spinel active phase spread over ceria for catalytic N2O decomposition: The role of the interface periphery

Catalytic decomposition of N2O over Fe-ZSM-11 catalysts prepared by different methods: Nature of active Fe species

Estudo do desempenho catalítico das zeólitas Beta e ZSM-5 contendo ferro para decomposição de óxido nitroso

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