Tail gas catalyzed N2O decomposition over Fe-beta zeolite. On the promoting role of framework connected AlO6 sites in the vicinity of Fe by controlled dealumination during exchange

Melián‐Cabrera, Ignacio; Eck, Ernst R. H. van; Espinosa, Silvia; Siles-Quesada, Sandra; Falco, Lorena; Kentgens, A.P.M.; Kapteijn, Freek; Moulijn, Jacob A.

doi:10.1016/j.apcatb.2016.10.019

Cited by 25 publications

(21 citation statements)

References 59 publications

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“…The slightly lower Fe loading than the theoretical value 0.50 wt.% can be explained by the H + /Fe 3+ competition during the exchange; as discussed elsewhere. 30 The Si/Al ratio is comparable to that of the as-received zeolite material (8.9). Temperatureprogrammed reduction (TPR) characterization shed some light on the type of Fe species formed during exchange, on both the optimal and reference catalysts.…”

Section: Resultsmentioning

confidence: 71%

“…This region Accepted 26/Dec/17 -10.1021/acs.iecr.7b04584 Final version can be accessed through the ACS website corresponds to the reduction of the Fe 3+ in exchanged positions (cations and oxocations) on the zeolite framework. 16 The optimal catalyst shows a fraction of Fe 2 O 3 species, represented by the broad peak centred at 800 K, 30 that accounts for ca. 10% of the Fe, based on a TPR quantification method for Fe-zeolites.…”

Section: Resultsmentioning

confidence: 99%

“…The decomposition of N2O into N2 and O2 is a reaction with proven environmental benefits. 1,2 The greenhouse warming potential (GHWP) of N 2 O is 250-300 higher than that of CO 2 , 3 which means that eliminating relatively small N 2 O gas emissions will have a large impact in terms of CO 2 equivalent reduction, as compared to CH4 (GHWP of [28][29][30][31][32][33][34][35][36]. Moreover, N2O plays a role in ozone depletion.…”

Section: Introductionmentioning

confidence: 99%

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Overcoming the Engineering Constraints for Scaling-Up the State-of-the-Art Catalyst for Tail-Gas N₂O Decomposition

Melián‐Cabrera

Espinosa

Mentruit

et al. 2018

Ind. Eng. Chem. Res.

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An efficient process is reported for preparing a state-of-the-art Fe-ferrierite catalyst for N 2 O decomposition under industrial tail-gas conditions. In the synthesis procedure we evaluate the very demanding constraints for scale-up; i.e. large reactor volumes are typically needed, long processing times and considerable amounts of waste water is generated. The proposed synthesis minimizes the amount of water used, and therefore the amount produced waste water is minimal; in this approach there is no liquid residual water stream that would need intensive processing. This has remarkable benefits in terms of process design, since the volume of equipment is reduced and the energy-intensive filtration is eliminated. This route exemplifies the concept of process intensification, with the ambition to re-engineer an existing process to make the industrial catalyst manufacture more sustainable. The so-obtained catalyst is active, selective and very stable under tail gas conditions containing H2O, NO and O2, together with N2O; keeping a high conversion during 70 h time on stream at 700 K, with a decay of 0.01%/h, while the standard reference catalyst decays at 0.06%/h; hence it deactivates six times slower, with ~5% absolute points of higher conversion. The excellent catalytic performance is preliminary ascribed to the differential speciation.

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Section: Resultsmentioning

confidence: 71%

Section: Resultsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Overcoming the Engineering Constraints for Scaling-Up the State-of-the-Art Catalyst for Tail-Gas N₂O Decomposition

Melián‐Cabrera

Espinosa

Mentruit

et al. 2018

Ind. Eng. Chem. Res.

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“…The acidity features were evaluated by pyridine-adsorbed FTIR spectroscopy ( is higher for the non-Fenton H2O2 material than the fresh counterpart; 10 % higher for the Brønsted and 50% higher for the Lewis sites. This could be explained by 1) the removal of amorphous domains (invisible to XRD) during the treatment, rendering a material with a higher intrinsic acidity and 2) due to the Al-dislodgement forming framework connected hexacoordinated Al [47]. In the case of the Fenton treatment (AP27-Fe70), similar acidity value as for the fresh ZSM-5 was found.…”

Section: Properties Of the Reactivated Materialsmentioning

confidence: 59%

Advanced oxidation process for coke removal: A systematic study of hydrogen peroxide and OH-derived-Fenton radicals of a fouled zeolite

Morales

Góra‐Marek

Musch

et al. 2018

Applied Catalysis A: General

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“…Nitrous oxide has increased approximately linearly by about 0.8 ppb per year over the past few decades [7]. Permanent increase in N 2 O concentration in the atmosphere resulted in a search for an effective catalytic method of its decomposition [8][9][10][11][12][13][14][15][16][17][18]. The U.S. Environmental Protection Agency reported that in the years 1990-2014, almost 80% of N 2 O emitted in the US.…”

Section: Nitrous Oxide As a Greenhouse Gas And An Oxidantmentioning

confidence: 99%

Catalytic oxidation of methanol in the cenospheric fluidized bed

et al. 2019

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Original scientific paper https://doi.org/10.2298/TSCI19S4231BThe process of oxidation of gaseous CH 3 OH by N 2 O was carried out over an Ag-Fe 2 O 3 -cenosphere catalyst whose structure can be defined as double shell-core catalyst. Preparation of the catalyst was carried out in two stages: thermal decomposition of Fe(CO) 5 at above 160 °C and then electroless Ag plating. The process of methanol degradation by N 2 O was carried out in a fluidized bed reactor. The study confirms that it is possible to achieve complete degradation of N 2 O and CH 3 OH for the obtained catalyst at above 450 °C when the contact time of the reactants with the catalyst is approximately 6 second and when the substrates are used in stoichiometric ratios. More than 60% of the hydrogen contained in CH 3 OH can be converted to molecular hydrogen at 500 °C with a ratio of N 2 O/CH 3 OH not greater than 0.6 and with a contact time of reactants with the catalyst of approx. 6 seconds.

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Tail gas catalyzed N2O decomposition over Fe-beta zeolite. On the promoting role of framework connected AlO6 sites in the vicinity of Fe by controlled dealumination during exchange

Abstract: Tail Gas Catalyzed N2O decomposition over Fe-beta zeolite.On the promoting role of framework connected AlO6 sites in the vicinity of Fe by controlled dealumination during exchange, Applied Catalysis B, Environmental http://dx.

Cited by 25 publications

References 59 publications

Overcoming the Engineering Constraints for Scaling-Up the State-of-the-Art Catalyst for Tail-Gas N₂O Decomposition

Overcoming the Engineering Constraints for Scaling-Up the State-of-the-Art Catalyst for Tail-Gas N₂O Decomposition

Advanced oxidation process for coke removal: A systematic study of hydrogen peroxide and OH-derived-Fenton radicals of a fouled zeolite

Catalytic oxidation of methanol in the cenospheric fluidized bed

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Tail gas catalyzed N2O decomposition over Fe-beta zeolite. On the promoting role of framework connected AlO6 sites in the vicinity of Fe by controlled dealumination during exchange

Abstract: Tail Gas Catalyzed N2O decomposition over Fe-beta zeolite.On the promoting role of framework connected AlO6 sites in the vicinity of Fe by controlled dealumination during exchange, Applied Catalysis B, Environmental http://dx.

Cited by 25 publications

References 59 publications

Overcoming the Engineering Constraints for Scaling-Up the State-of-the-Art Catalyst for Tail-Gas N2O Decomposition

Overcoming the Engineering Constraints for Scaling-Up the State-of-the-Art Catalyst for Tail-Gas N2O Decomposition

Advanced oxidation process for coke removal: A systematic study of hydrogen peroxide and OH-derived-Fenton radicals of a fouled zeolite

Catalytic oxidation of methanol in the cenospheric fluidized bed

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Product

Resources

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Overcoming the Engineering Constraints for Scaling-Up the State-of-the-Art Catalyst for Tail-Gas N₂O Decomposition

Overcoming the Engineering Constraints for Scaling-Up the State-of-the-Art Catalyst for Tail-Gas N₂O Decomposition