Methanol Oxidation to Formaldehyde on VSiBEA Zeolite: A Combined DFT/vdW/Transition Path Sampling and Experimental Study

Diana C. Tranca (1) , Frerich J. Keil (2) , Ionut Tranca , Monica Calatayud (3, 4) , Stanislaw Dzwigaj (5) , Maciej Trejda (3) , Frederik Tielens (6)

1 Technical University Hamburg Harburg [Hamburg]
2 Institute of Chemical Reaction Engineering
3 LCT - Laboratoire de chimie théorique
4 IUF - Institut universitaire de France
5 LRS - Laboratoire de Réactivité de Surface
6 LCMCP - Laboratoire de Chimie de la Matière Condensée de Paris

Density functional calculations have been performed applying periodic boundary conditions to investigate the oxidation of methanol on vanadium-containing SiBEA zeolite (VSiBEA). Different types of reaction configurations have been set up in conformity with the experimental conditions. Thermodynamic property calculations for T > 0 K have been performed and compared with the available experimental results. Transition path sampling was employed to unravel the reaction mechanisms for oxidation of methanol on vanadium-containing SiBEA zeolites at three temperatures (300, 415, and 523 K). Dispersion interactions were accounted for by adding a damped dispersion term to the PBE energies. The study of different reaction pathways was combined with experimental data that enabled us to shed more light on the reaction mechanism.

Domaines: Chimie

Diana C. Tranca, Frerich J. Keil, Ionut Tranca, Monica Calatayud, Stanislaw Dzwigaj, et al.. Methanol Oxidation to Formaldehyde on VSiBEA Zeolite: A Combined DFT/vdW/Transition Path Sampling and Experimental Study. Journal of Physical Chemistry C, 2015, 119 (24), pp.13619-13631. ⟨10.1021/acs.jpcc.5b01911⟩. ⟨hal-01226507⟩