Influence of the meso-macroporous ZrO -TiO calcination temperature on the pre-reduced Pd/ZrO -TiO (1/1) performances in chlorobenzene total oxidation

J.-F. Lamonier, T.B. Nguyen, M. Franco, J.-M. Giraudon, S. Siffert, R. Cousin, Y. Li, X.Y. Yang, B.-L. Su

Research output: Contribution to journalArticle

Abstract

The effect of two calcining temperatures (400 °C, 600 °C) on the texture, structure and thermal stability of a meso-macroporous ZrO -TiO of equal molar amount (ZrTi ; x = 4, 6) synthesized from hydrothermal conditions using a surfactant and metal alkoxide precursors was studied. Pd (0.5 wt.%) was dispersed on these innovative supports (Pd/ZrTi ; x = 4, 6) by a classic wet impregnation and calcined at 400 °C. The resulting catalysts were characterized by Elemental analysis (EA), X-Ray Diffraction (XRD), N adsorption-desorption, H -Temperature Programmed Reduction (H -TPR), Pd dispersion and tested as pre-reduced in the total oxidation of chlorobenzene. It was found that the calcination temperature did not provoke a significant effect on the physicochemical properties of the resulting binary oxide except the acidity which significantly decreased. The support was stable against phase transformation upon calcination as no crystalline phase could be detected indicating a homogeneous mixing of the Zr and Ti components. The Specific Surface Areas (SSAs) were superior to 400 m /g even after calcination at 600 °C. The Pd dispersion was around 40% and the palladium was totally reduced before catalytic testing. Lowering the temperature of calcination of the support enhanced the performances of the catalyst. Indeed PhCl conversion increased as the calcination temperature decreased and correlates with the Pd dispersion and SSA of the catalyst. A significant amount of polychlorinated benzenes PhCl (x = 2-6) was detected in the course of the reaction which practically disappeared at 100% PhCl conversion. This amount was reduced by a factor 2 as the temperature of calcination decreased. Compared to the performances of Pd/Ti and Pd/Zr for the same reaction, all things being kept equal, calcined ZrO -TiO supports show higher surface areas and higher thermal stability than their ZrO and TiO counterparts. In terms of activity for PhCl total oxidation based on T values the ZrO -TiO supports showed an intermediate behaviour while a beneficial effect was observed regarding the by-products production which is the lowest herein for the Pd/TiZr catalyst.
Original languageEnglish
Pages (from-to)566-570
Number of pages5
JournalCatalysis Today
Volume164
Issue number1
DOIs
Publication statusPublished - 30 Apr 2011

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Calcination
Oxidation
Catalysts
Specific surface area
Temperature
Thermodynamic stability
Palladium
Benzene
Catalyst supports
Acidity
Surface-Active Agents
Impregnation
Oxides
Byproducts
chlorobenzene
Desorption
Surface active agents
Textures
Phase transitions
Metals

Cite this

Lamonier, J.-F. ; Nguyen, T.B. ; Franco, M. ; Giraudon, J.-M. ; Siffert, S. ; Cousin, R. ; Li, Y. ; Yang, X.Y. ; Su, B.-L. / Influence of the meso-macroporous ZrO -TiO calcination temperature on the pre-reduced Pd/ZrO -TiO (1/1) performances in chlorobenzene total oxidation. In: Catalysis Today. 2011 ; Vol. 164, No. 1. pp. 566-570.
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abstract = "The effect of two calcining temperatures (400 °C, 600 °C) on the texture, structure and thermal stability of a meso-macroporous ZrO -TiO of equal molar amount (ZrTi ; x = 4, 6) synthesized from hydrothermal conditions using a surfactant and metal alkoxide precursors was studied. Pd (0.5 wt.{\%}) was dispersed on these innovative supports (Pd/ZrTi ; x = 4, 6) by a classic wet impregnation and calcined at 400 °C. The resulting catalysts were characterized by Elemental analysis (EA), X-Ray Diffraction (XRD), N adsorption-desorption, H -Temperature Programmed Reduction (H -TPR), Pd dispersion and tested as pre-reduced in the total oxidation of chlorobenzene. It was found that the calcination temperature did not provoke a significant effect on the physicochemical properties of the resulting binary oxide except the acidity which significantly decreased. The support was stable against phase transformation upon calcination as no crystalline phase could be detected indicating a homogeneous mixing of the Zr and Ti components. The Specific Surface Areas (SSAs) were superior to 400 m /g even after calcination at 600 °C. The Pd dispersion was around 40{\%} and the palladium was totally reduced before catalytic testing. Lowering the temperature of calcination of the support enhanced the performances of the catalyst. Indeed PhCl conversion increased as the calcination temperature decreased and correlates with the Pd dispersion and SSA of the catalyst. A significant amount of polychlorinated benzenes PhCl (x = 2-6) was detected in the course of the reaction which practically disappeared at 100{\%} PhCl conversion. This amount was reduced by a factor 2 as the temperature of calcination decreased. Compared to the performances of Pd/Ti and Pd/Zr for the same reaction, all things being kept equal, calcined ZrO -TiO supports show higher surface areas and higher thermal stability than their ZrO and TiO counterparts. In terms of activity for PhCl total oxidation based on T values the ZrO -TiO supports showed an intermediate behaviour while a beneficial effect was observed regarding the by-products production which is the lowest herein for the Pd/TiZr catalyst.",
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Influence of the meso-macroporous ZrO -TiO calcination temperature on the pre-reduced Pd/ZrO -TiO (1/1) performances in chlorobenzene total oxidation. / Lamonier, J.-F.; Nguyen, T.B.; Franco, M.; Giraudon, J.-M.; Siffert, S.; Cousin, R.; Li, Y.; Yang, X.Y.; Su, B.-L.

In: Catalysis Today, Vol. 164, No. 1, 30.04.2011, p. 566-570.

Research output: Contribution to journalArticle

TY - JOUR

T1 - Influence of the meso-macroporous ZrO -TiO calcination temperature on the pre-reduced Pd/ZrO -TiO (1/1) performances in chlorobenzene total oxidation

AU - Lamonier, J.-F.

AU - Nguyen, T.B.

AU - Franco, M.

AU - Giraudon, J.-M.

AU - Siffert, S.

AU - Cousin, R.

AU - Li, Y.

AU - Yang, X.Y.

AU - Su, B.-L.

N1 - Copyright 2011 Elsevier B.V., All rights reserved.

PY - 2011/4/30

Y1 - 2011/4/30

N2 - The effect of two calcining temperatures (400 °C, 600 °C) on the texture, structure and thermal stability of a meso-macroporous ZrO -TiO of equal molar amount (ZrTi ; x = 4, 6) synthesized from hydrothermal conditions using a surfactant and metal alkoxide precursors was studied. Pd (0.5 wt.%) was dispersed on these innovative supports (Pd/ZrTi ; x = 4, 6) by a classic wet impregnation and calcined at 400 °C. The resulting catalysts were characterized by Elemental analysis (EA), X-Ray Diffraction (XRD), N adsorption-desorption, H -Temperature Programmed Reduction (H -TPR), Pd dispersion and tested as pre-reduced in the total oxidation of chlorobenzene. It was found that the calcination temperature did not provoke a significant effect on the physicochemical properties of the resulting binary oxide except the acidity which significantly decreased. The support was stable against phase transformation upon calcination as no crystalline phase could be detected indicating a homogeneous mixing of the Zr and Ti components. The Specific Surface Areas (SSAs) were superior to 400 m /g even after calcination at 600 °C. The Pd dispersion was around 40% and the palladium was totally reduced before catalytic testing. Lowering the temperature of calcination of the support enhanced the performances of the catalyst. Indeed PhCl conversion increased as the calcination temperature decreased and correlates with the Pd dispersion and SSA of the catalyst. A significant amount of polychlorinated benzenes PhCl (x = 2-6) was detected in the course of the reaction which practically disappeared at 100% PhCl conversion. This amount was reduced by a factor 2 as the temperature of calcination decreased. Compared to the performances of Pd/Ti and Pd/Zr for the same reaction, all things being kept equal, calcined ZrO -TiO supports show higher surface areas and higher thermal stability than their ZrO and TiO counterparts. In terms of activity for PhCl total oxidation based on T values the ZrO -TiO supports showed an intermediate behaviour while a beneficial effect was observed regarding the by-products production which is the lowest herein for the Pd/TiZr catalyst.

AB - The effect of two calcining temperatures (400 °C, 600 °C) on the texture, structure and thermal stability of a meso-macroporous ZrO -TiO of equal molar amount (ZrTi ; x = 4, 6) synthesized from hydrothermal conditions using a surfactant and metal alkoxide precursors was studied. Pd (0.5 wt.%) was dispersed on these innovative supports (Pd/ZrTi ; x = 4, 6) by a classic wet impregnation and calcined at 400 °C. The resulting catalysts were characterized by Elemental analysis (EA), X-Ray Diffraction (XRD), N adsorption-desorption, H -Temperature Programmed Reduction (H -TPR), Pd dispersion and tested as pre-reduced in the total oxidation of chlorobenzene. It was found that the calcination temperature did not provoke a significant effect on the physicochemical properties of the resulting binary oxide except the acidity which significantly decreased. The support was stable against phase transformation upon calcination as no crystalline phase could be detected indicating a homogeneous mixing of the Zr and Ti components. The Specific Surface Areas (SSAs) were superior to 400 m /g even after calcination at 600 °C. The Pd dispersion was around 40% and the palladium was totally reduced before catalytic testing. Lowering the temperature of calcination of the support enhanced the performances of the catalyst. Indeed PhCl conversion increased as the calcination temperature decreased and correlates with the Pd dispersion and SSA of the catalyst. A significant amount of polychlorinated benzenes PhCl (x = 2-6) was detected in the course of the reaction which practically disappeared at 100% PhCl conversion. This amount was reduced by a factor 2 as the temperature of calcination decreased. Compared to the performances of Pd/Ti and Pd/Zr for the same reaction, all things being kept equal, calcined ZrO -TiO supports show higher surface areas and higher thermal stability than their ZrO and TiO counterparts. In terms of activity for PhCl total oxidation based on T values the ZrO -TiO supports showed an intermediate behaviour while a beneficial effect was observed regarding the by-products production which is the lowest herein for the Pd/TiZr catalyst.

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