Microkinetic Modeling of Benzyl Alcohol Oxidation on Carbon-Supported Palladium Nanoparticles
Abstract
Abstract Six products are formed from benzyl alcohol oxidation over Pd nanoparticles using O 2 as the oxidant: benzaldehyde, toluene, benzyl ether, benzene, benzoic acid, and benzyl benzoate. Three experimental parameters were varied here: alcohol concentration, oxygen concentration, and temperature. Microkinetic modeling using a mechanism published recently with surface intermediates was able to produce all 18 trends observed experimentally with mostly quantitative agreement. Approximate analytical equations derived from the microkinetic model for isothermal conditions reproduced the isothermal trends and provided insight. The most important activation energies are E a2 =57.9 kJ mol −1 , E a5 =129 kJ mol −1 , and E a6 =175 kJ mol −1 , which correspond to alcohol dissociation, alkyl hydrogenation, and the reaction of alkyl species with alkoxy species. Upper limits for other activation energies were identified. The concepts of a sticking coefficient and steric factor in solution were applied.
- Authors:
-
[1];
[2];
[2]
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division
- Univ. degli Studi di Milano (Italy). Dipartimento di Chimica
- Publication Date:
- Research Org.:
- Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1295106
- Alternate Identifier(s):
- OSTI ID: 1401220
- Grant/Contract Number:
- AC05-00OR22725
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ChemCatChem
- Additional Journal Information:
- Journal Volume: 8; Journal Issue: 15; Journal ID: ISSN 1867-3880
- Publisher:
- ChemPubSoc Europe
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; alcohols; kinetics; molecular modeling; oxidation; palladium
Citation Formats
Savara, Aditya, Rossetti, Ilenia, Chan-Thaw, Carine E., Prati, Laura, and Villa, Alberto. Microkinetic Modeling of Benzyl Alcohol Oxidation on Carbon-Supported Palladium Nanoparticles. United States: N. p., 2016.
Web. doi:10.1002/cctc.201600368.
Savara, Aditya, Rossetti, Ilenia, Chan-Thaw, Carine E., Prati, Laura, & Villa, Alberto. Microkinetic Modeling of Benzyl Alcohol Oxidation on Carbon-Supported Palladium Nanoparticles. United States. https://doi.org/10.1002/cctc.201600368
Savara, Aditya, Rossetti, Ilenia, Chan-Thaw, Carine E., Prati, Laura, and Villa, Alberto. Thu .
"Microkinetic Modeling of Benzyl Alcohol Oxidation on Carbon-Supported Palladium Nanoparticles". United States. https://doi.org/10.1002/cctc.201600368. https://www.osti.gov/servlets/purl/1295106.
@article{osti_1295106,
title = {Microkinetic Modeling of Benzyl Alcohol Oxidation on Carbon-Supported Palladium Nanoparticles},
author = {Savara, Aditya and Rossetti, Ilenia and Chan-Thaw, Carine E. and Prati, Laura and Villa, Alberto},
abstractNote = {Abstract Six products are formed from benzyl alcohol oxidation over Pd nanoparticles using O 2 as the oxidant: benzaldehyde, toluene, benzyl ether, benzene, benzoic acid, and benzyl benzoate. Three experimental parameters were varied here: alcohol concentration, oxygen concentration, and temperature. Microkinetic modeling using a mechanism published recently with surface intermediates was able to produce all 18 trends observed experimentally with mostly quantitative agreement. Approximate analytical equations derived from the microkinetic model for isothermal conditions reproduced the isothermal trends and provided insight. The most important activation energies are E a2 =57.9 kJ mol −1 , E a5 =129 kJ mol −1 , and E a6 =175 kJ mol −1 , which correspond to alcohol dissociation, alkyl hydrogenation, and the reaction of alkyl species with alkoxy species. Upper limits for other activation energies were identified. The concepts of a sticking coefficient and steric factor in solution were applied.},
doi = {10.1002/cctc.201600368},
journal = {ChemCatChem},
number = 15,
volume = 8,
place = {United States},
year = {Thu Jul 14 00:00:00 EDT 2016},
month = {Thu Jul 14 00:00:00 EDT 2016}
}
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