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Structure sensitivity of dimethylamine deep oxidation over Pt/Al2O3 catalysts

Samo za registrovane korisnike
2009
Autori
Grbić, Boško
Radić, Nenad
Arsenijević, Zorana
Garić Grulović, Radmila
Grbavčić, Željko
Članak u časopisu (Objavljena verzija)
Metapodaci
Prikaz svih podataka o dokumentu
Apstrakt
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 sensitivity
Izvor:
Applied Catalysis B-Environmental, 2009, 90, 3-4, 478-484
Izdavač:
  • Elsevier
Finansiranje / projekti:
  • Istraživanje fenomena prenosa značajnih za razvoj višefaznih procesa i opreme (RS-142014)

DOI: 10.1016/j.apcatb.2009.04.008

ISSN: 0926-3373

WoS: 000268042800020

Scopus: 2-s2.0-67649265084
[ Google Scholar ]
6
1
URI
https://cer.ihtm.bg.ac.rs/handle/123456789/539
Kolekcije
  • Radovi istraživača / Researchers' publications
Institucija/grupa
IHTM
TY  - 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 . .

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