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Structure sensitivity and kinetics of D-glucose oxidation to D-gluconic acid over carbon-supported gold catalysts

Önal, Yücel and Schimpf, Sabine and Claus, Peter (2004):
Structure sensitivity and kinetics of D-glucose oxidation to D-gluconic acid over carbon-supported gold catalysts.
In: Journal of Catalysis, pp. 122-133, 223, (1), [Online-Edition: http://www.sciencedirect.com/science/article/B6WHJ-4BWMRCN-3...],
[Article]

Abstract

The heterogeneously catalyzed oxidation of Image -glucose to Image -gluconic acid over Au/C catalysts has been studied. A series of Au/C catalysts were prepared by the gold sol method with different reducing agents and different kinds of carbon support providing Au mean particle diameters in the range 3–6 nm. The activities of these catalysts with respect to Image -glucose oxidation were compared, and several aspects influencing activity, especially Au particle size, were discussed. The influence of reaction conditions (T=30–90 °C, pH 7.0–9.5) on the kinetics of the Image -glucose oxidation has been examined using the most active Au/C catalyst. By a detailed analysis of all reaction products under different reaction conditions, a reaction network of the Image -glucose oxidation is presented, and a reaction mechanism for Image -glucose oxidation that explains the influence of pH on reaction rate is proposed. Ensuring that Image -glucose oxidation takes place in the kinetic regime (sufficient stirring rate and airflow rate), a semiempirical model based on a Langmuir–Hinshelwood-type reaction pathway is assumed. At 50 °C and pH 9.5 kinetic parameters were calculated by an optimization routine. The resulting concentration courses of Image -glucose and Image -gluconic acid were in good agreement with the experimental data. All experiments were carried out in a semibatch reactor under pH control at atmospheric pressure.

Item Type: Article
Erschienen: 2004
Creators: Önal, Yücel and Schimpf, Sabine and Claus, Peter
Title: Structure sensitivity and kinetics of D-glucose oxidation to D-gluconic acid over carbon-supported gold catalysts
Language: English
Abstract:

The heterogeneously catalyzed oxidation of Image -glucose to Image -gluconic acid over Au/C catalysts has been studied. A series of Au/C catalysts were prepared by the gold sol method with different reducing agents and different kinds of carbon support providing Au mean particle diameters in the range 3–6 nm. The activities of these catalysts with respect to Image -glucose oxidation were compared, and several aspects influencing activity, especially Au particle size, were discussed. The influence of reaction conditions (T=30–90 °C, pH 7.0–9.5) on the kinetics of the Image -glucose oxidation has been examined using the most active Au/C catalyst. By a detailed analysis of all reaction products under different reaction conditions, a reaction network of the Image -glucose oxidation is presented, and a reaction mechanism for Image -glucose oxidation that explains the influence of pH on reaction rate is proposed. Ensuring that Image -glucose oxidation takes place in the kinetic regime (sufficient stirring rate and airflow rate), a semiempirical model based on a Langmuir–Hinshelwood-type reaction pathway is assumed. At 50 °C and pH 9.5 kinetic parameters were calculated by an optimization routine. The resulting concentration courses of Image -glucose and Image -gluconic acid were in good agreement with the experimental data. All experiments were carried out in a semibatch reactor under pH control at atmospheric pressure.

Journal or Publication Title: Journal of Catalysis
Volume: 223
Number: 1
Uncontrolled Keywords: Glucose oxidation; Au/C catalysts; Structure sensitivity; Specific gold surface area; Gold nanoparticle; Gold sol method; Mass transfer; Langmuir–Hinshelwood kinetics
Divisions: 07 Department of Chemistry > Fachgebiet Technische Chemie > Technische Chemie II
07 Department of Chemistry > Fachgebiet Technische Chemie
07 Department of Chemistry
Date Deposited: 20 Mar 2009 09:01
Official URL: http://www.sciencedirect.com/science/article/B6WHJ-4BWMRCN-3...
Identification Number: doi:10.1016/j.jcat.2004.01.010
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