Structure sensitivity of dimethylamine deep oxidation over Pt/Al2O3 catalysts
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2009
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The deep oxidation of dimethylamine (DMA) was studied over Pt/Al2O3 catalysts with small (1 nm) and large (7.8-15.5 nm) Pt crystallite sizes. The turnover frequency (TOF) was higher for the large than for the small Pt crystallites, indicating that the reaction is structure sensitive. Two kinetic models were used to interpret the obtained results, i.e., the Mars van Krevelen and a mechanism based on the adsorption of oxygen and adsorption of dimethylamine on different active sites were employed. Both models showed that the activation energy for the oxygen chemisorption rate constant (k(o)) decreased with increasing of Pt crystallite size and that the activation energy for the surface reaction rate constant (k(i)) was independent of the Pt crystallite size. The structure sensitivity may be explained by differences in the reactivity of the oxygen adsorbed on these Pt crystallites. The Mars van Krevelen model fits the TOF values very well at concentrations of DMA higher than 1500 ppm, whil...e in the lower concentrations region, the model under predicts the experimental data. The model based on the adsorption of oxygen and DMA on different active sites fits the experimental data quite well over the whole temperature and concentration range. The fitted values of the Henry adsorption constant are independent of the Pt crystallite size.
Ključne reči:
Pt/Al2O3 Catalyst / Deep oxidation / Dimethylamine / Kinetics / Structure sensitivityIzvor:
Applied Catalysis B-Environmental, 2009, 90, 3-4, 478-484Izdavač:
- Elsevier
Finansiranje / projekti:
DOI: 10.1016/j.apcatb.2009.04.008
ISSN: 0926-3373
WoS: 000268042800020
Scopus: 2-s2.0-67649265084
Institucija/grupa
IHTMTY - JOUR AU - Grbić, Boško AU - Radić, Nenad AU - Arsenijević, Zorana AU - Garić Grulović, Radmila AU - Grbavčić, Željko PY - 2009 UR - https://cer.ihtm.bg.ac.rs/handle/123456789/539 AB - The deep oxidation of dimethylamine (DMA) was studied over Pt/Al2O3 catalysts with small (1 nm) and large (7.8-15.5 nm) Pt crystallite sizes. The turnover frequency (TOF) was higher for the large than for the small Pt crystallites, indicating that the reaction is structure sensitive. Two kinetic models were used to interpret the obtained results, i.e., the Mars van Krevelen and a mechanism based on the adsorption of oxygen and adsorption of dimethylamine on different active sites were employed. Both models showed that the activation energy for the oxygen chemisorption rate constant (k(o)) decreased with increasing of Pt crystallite size and that the activation energy for the surface reaction rate constant (k(i)) was independent of the Pt crystallite size. The structure sensitivity may be explained by differences in the reactivity of the oxygen adsorbed on these Pt crystallites. The Mars van Krevelen model fits the TOF values very well at concentrations of DMA higher than 1500 ppm, while in the lower concentrations region, the model under predicts the experimental data. The model based on the adsorption of oxygen and DMA on different active sites fits the experimental data quite well over the whole temperature and concentration range. The fitted values of the Henry adsorption constant are independent of the Pt crystallite size. PB - Elsevier T2 - Applied Catalysis B-Environmental T1 - Structure sensitivity of dimethylamine deep oxidation over Pt/Al2O3 catalysts VL - 90 IS - 3-4 SP - 478 EP - 484 DO - 10.1016/j.apcatb.2009.04.008 ER -
@article{ author = "Grbić, Boško and Radić, Nenad and Arsenijević, Zorana and Garić Grulović, Radmila and Grbavčić, Željko", year = "2009", abstract = "The deep oxidation of dimethylamine (DMA) was studied over Pt/Al2O3 catalysts with small (1 nm) and large (7.8-15.5 nm) Pt crystallite sizes. The turnover frequency (TOF) was higher for the large than for the small Pt crystallites, indicating that the reaction is structure sensitive. Two kinetic models were used to interpret the obtained results, i.e., the Mars van Krevelen and a mechanism based on the adsorption of oxygen and adsorption of dimethylamine on different active sites were employed. Both models showed that the activation energy for the oxygen chemisorption rate constant (k(o)) decreased with increasing of Pt crystallite size and that the activation energy for the surface reaction rate constant (k(i)) was independent of the Pt crystallite size. The structure sensitivity may be explained by differences in the reactivity of the oxygen adsorbed on these Pt crystallites. The Mars van Krevelen model fits the TOF values very well at concentrations of DMA higher than 1500 ppm, while in the lower concentrations region, the model under predicts the experimental data. The model based on the adsorption of oxygen and DMA on different active sites fits the experimental data quite well over the whole temperature and concentration range. The fitted values of the Henry adsorption constant are independent of the Pt crystallite size.", publisher = "Elsevier", journal = "Applied Catalysis B-Environmental", title = "Structure sensitivity of dimethylamine deep oxidation over Pt/Al2O3 catalysts", volume = "90", number = "3-4", pages = "478-484", doi = "10.1016/j.apcatb.2009.04.008" }
Grbić, B., Radić, N., Arsenijević, Z., Garić Grulović, R.,& Grbavčić, Ž.. (2009). Structure sensitivity of dimethylamine deep oxidation over Pt/Al2O3 catalysts. in Applied Catalysis B-Environmental Elsevier., 90(3-4), 478-484. https://doi.org/10.1016/j.apcatb.2009.04.008
Grbić B, Radić N, Arsenijević Z, Garić Grulović R, Grbavčić Ž. Structure sensitivity of dimethylamine deep oxidation over Pt/Al2O3 catalysts. in Applied Catalysis B-Environmental. 2009;90(3-4):478-484. doi:10.1016/j.apcatb.2009.04.008 .
Grbić, Boško, Radić, Nenad, Arsenijević, Zorana, Garić Grulović, Radmila, Grbavčić, Željko, "Structure sensitivity of dimethylamine deep oxidation over Pt/Al2O3 catalysts" in Applied Catalysis B-Environmental, 90, no. 3-4 (2009):478-484, https://doi.org/10.1016/j.apcatb.2009.04.008 . .