Ordered mesoporous CuO–CeO2 mixed oxides as an effective catalyst for N2O decomposition

Zabilskiy, Maxim; Erjavec, Boštjan; Djinović, Petar; Pintar, Albin

doi:10.1016/j.cej.2014.05.127

Cited by 66 publications

(56 citation statements)

References 34 publications

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“…Also, electronic and other interactions between CuO clusters and CeO 2 support (synergetic effect) are less pronounced when the two phases are not in an intimate contact with a substantial interfacial surface area. Table 4 presents a comparison of catalytic N 2 O decomposition results over CuO/CeO 2 solids investigated in this work and over the catalysts utilized by other research groups [6,15,16,32,33]. As one can see, 10-CuO/CeO 2 -160 catalyst showed the highest activity during catalytic N 2 O degradation among CuO/CeO 2 based materials.…”

Section: N 2 O Decomposition Testsmentioning

confidence: 86%

Small CuO clusters on CeO2 nanospheres as active species for catalytic N2O decomposition

Zabilskiy

Djinović

Erjavec

et al. 2015

Applied Catalysis B: Environmental

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107

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Section: N 2 O Decomposition Testsmentioning

confidence: 86%

Small CuO clusters on CeO2 nanospheres as active species for catalytic N2O decomposition

Zabilskiy

Djinović

Erjavec

et al. 2015

Applied Catalysis B: Environmental

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107

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“…% Cu have two peaks with maxima located at 450-470 nm and 750-800 nm. The first peak could be attributed to Cu +1 clusters and/or bis(µ-oxo)dicopper core ([Cu 2 O] 2+ ), while the second peak is due to d-d Cu 2+ transition in more or less tetragonally distorted O h symmetry (these attributions were thoroughly discussed in our previous works 27,28 ). Increasing Cu loading to 4 wt.…”

Section: Catalytic Experimentsmentioning

confidence: 95%

“…23,24 Among the catalysts which can decompose N 2 O under moderate temperatures (300-500 °C), CuOCeO 2 materials show very promising results. [25][26][27][28] Interest in N 2 O decomposition arises from the fact that it is a potent greenhouse gas, produced in nitric acid and fertilizer industry, which contributes to ozone layer depletion. 29,30 As a result, understanding and design of the catalyst that enables its efficient destruction is of great importance.…”

Section: Introductionmentioning

confidence: 99%

Nanoshaped CuO/CeO₂ Materials: Effect of the Exposed Ceria Surfaces on Catalytic Activity in N₂O Decomposition Reaction

Zabilskiy¹,

Djinović²,

et al. 2015

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This study reports a thorough investigation of nanosized CuO/CeO 2 materials as an efficient catalyst for decomposition of N 2 O, which is a strong greenhouse gas largely produced by chemical industry. Effect of terminating CeO 2 crystalline planes ({100}, {110} and {111}) on the behavior of CuO dispersed over CeO 2 nanocubes, nanorods and polyhedral crystallites was examined in detail by using a variety of catalyst characterization techniques. The 4 wt. % Cu was found as the most advantageous metal loading, whereas higher Cu content resulted in lower dispersion and formation of significantly less active, segregated bulk CuO phase. It was discovered that CuO/CeO 2 solids should enable both excessive oxygen mobility on the catalyst surface as well as formation of highly reducible Cu defect sites, in order to ensure high intrinsic activity. Detailed studies further revealed that CeO 2 morphology needs to be tailored to expose {100} and {110} high-energy surface planes, as present in CeO 2 nanorods. Oxygen mobility and regeneration of active Cu phase on these surface planes is easier, which in turn facilitates higher catalytic activity through the recombination of surface oxygen atoms and desorption as molecular oxygen that replenishes active sites for subsequent catalytic cycles. As a consequence, CuO supported on CeO 2 nanorods demonstrated lower activation energy (87 kJ/mol) in N 2 O decomposition reaction compared to catalysts based on CeO 2 nanocubes (102 kJ/mol) or polyhedral CeO 2 (92 kJ/mol).

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“…There are many types of catalysts that can be used for N 2 O decomposition including perovskites [11–15], ceria-based catalysts [16–18], spinels [19–21] and iron containing zeolites [22]. In the latter case, H-ZSM-5 has been frequently used as a support [23–25].…”

Section: Introductionmentioning

confidence: 99%

Investigating the Influence of Fe Speciation on N2O Decomposition Over Fe–ZSM-5 Catalysts

et al. 2018

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The influence of Fe speciation on the decomposition rates of N2O over Fe–ZSM-5 catalysts prepared by Chemical Vapour Impregnation were investigated. Various weight loadings of Fe–ZSM-5 catalysts were prepared from the parent zeolite H-ZSM-5 with a Si:Al ratio of 23 or 30. The effect of Si:Al ratio and Fe weight loading was initially investigated before focussing on a single weight loading and the effects of acid washing on catalyst activity and iron speciation. UV/Vis spectroscopy, surface area analysis, XPS and ICP-OES of the acid washed catalysts indicated a reduction of ca. 60% of Fe loading when compared to the parent catalyst with a 0.4 wt% Fe loading. The TOF of N2O decomposition at 600 °C improved to 3.99 × 103 s−1 over the acid washed catalyst which had a weight loading of 0.16%, in contrast, the parent catalyst had a TOF of 1.60 × 103 s−1. Propane was added to the gas stream to act as a reductant and remove any inhibiting oxygen species that remain on the surface of the catalyst. Comparison of catalysts with relatively high and low Fe loadings achieved comparable levels of N2O decomposition when propane is present. When only N2O is present, low metal loading Fe–ZSM-5 catalysts are not capable of achieving high conversions due to the low proximity of active framework Fe3+ ions and extra-framework ɑ-Fe species, which limits oxygen desorption. Acid washing extracts Fe from these active sites and deposits it on the surface of the catalyst as FexOy, leading to a drop in activity. The Fe species present in the catalyst were identified using UV/Vis spectroscopy and speculate on the active species. We consider high loadings of Fe do not lead to an active catalyst when propane is present due to the formation of FexOy nanoparticles and clusters during catalyst preparation. These are inactive species which lead to a decrease in overall efficiency of the Fe ions and consequentially a lower TOF.

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Ordered mesoporous CuO–CeO2 mixed oxides as an effective catalyst for N2O decomposition

Cited by 66 publications

References 34 publications

Small CuO clusters on CeO2 nanospheres as active species for catalytic N2O decomposition

Small CuO clusters on CeO2 nanospheres as active species for catalytic N2O decomposition

Nanoshaped CuO/CeO₂ Materials: Effect of the Exposed Ceria Surfaces on Catalytic Activity in N₂O Decomposition Reaction

Investigating the Influence of Fe Speciation on N2O Decomposition Over Fe–ZSM-5 Catalysts

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Ordered mesoporous CuO–CeO2 mixed oxides as an effective catalyst for N2O decomposition

Cited by 66 publications

References 34 publications

Small CuO clusters on CeO2 nanospheres as active species for catalytic N2O decomposition

Small CuO clusters on CeO2 nanospheres as active species for catalytic N2O decomposition

Nanoshaped CuO/CeO2 Materials: Effect of the Exposed Ceria Surfaces on Catalytic Activity in N2O Decomposition Reaction

Investigating the Influence of Fe Speciation on N2O Decomposition Over Fe–ZSM-5 Catalysts

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Nanoshaped CuO/CeO₂ Materials: Effect of the Exposed Ceria Surfaces on Catalytic Activity in N₂O Decomposition Reaction