Photo-catalytic oxidation of cyclohexane over TiO2: a novel interpretation of temperature dependent performance

文献情報

出版日 2010-12-14

DOI 10.1039/C0CP00879F

インパクトファクター 3.676

著者

Ana Rita Almeida, Rob Berger, Jacob A. Moulijn, Guido Mul

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要旨

The rate of cyclohexane photo-catalytic oxidation to cyclohexanone over anatase TiO2 was studied at temperatures between 23 and 60 °C by in situATR-FTIR spectroscopy, and the kinetic parameters were estimated using a microkinetic model. At low temperatures, surface cyclohexanone formation is limited by cyclohexane adsorption due to unfavorable desorption of H2O, rather than previously proposed slow desorption of the product cyclohexanone. Up to 50 °C, the activation energy for photocatalytic cyclohexanone formation is zero, while carboxylates are formed with an activation energy of 18.4 ± 3.3 kJ mol−1. Above 50 °C, significant (thermal) oxidation of cyclohexanone contributes to carboxylate formation. The irreversibly adsorbed carboxylates lead to deactivation of the catalyst, and are most likely the predominant cause of the non-Arrhenius behavior at relatively high reaction temperatures, rather than cyclohexane adsorption limitations. The results imply that elevating the reaction temperature of photocatalytic cyclohexane oxidation reduces selectivity, and is not a means to suppress catalyst deactivation.

掲載誌

Physical Chemistry Chemical Physics

CiteScore: 5.5

自己引用率: 10.3%

年間論文数: 3036

Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.

Photo-catalytic oxidation of cyclohexane over TiO2: a novel interpretation of temperature dependent performance

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Physical Chemistry Chemical Physics

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