Affiliation:
1. Belarusian State University
2. Research Institute for Physical Chemical Problems of the Belarusian State University
3. King Abdullah University of Science and Technology
Abstract
The approaches to estimating the changes in enthalpy, entropy, and Gibbs energy of adsorption processes and heterogeneous catalytic reactions on the basis of the quantum chemical calculation data were studied. By comparing with the experimental data on CO adsorption on the anatase (TiO2) surface, the applicability of the developed multilayer cluster model for calculation of the adsorption energy (enthalpy) was shown. The data on the calculation methods of the entropy change in heterogeneous processes were analyzed. The use of the theories of an ideal two-dimensional gas and an ideal two-dimensional lattice gas for estimating a configuration contribution to the entropy of a heterogeneous process was studied. The density of adsorption centers on the (101) anatase surface and the population corresponding to the standard state of an ideal two-dimensional gas were calculated. The consistency of the studied models at low populations was shown, and the limits of their applicability were established.
Publisher
Publishing House Belorusskaya Nauka
Reference15 articles.
1. Matulis V. E., Ragoyja E. G., Ivashkevich O. A., Lyakhov D. A., Michels D. DFT Study of NO Reduction Process on Ag/ γ-Al2O3 Catalyst: Some Aspects of Mechanism and Catalyst Structure. Journal of Physical Chemistry C, 2021, vol. 125, no. 1, pp. 419–426. https://doi.org/10.1021/acs.jpcc.0c08417
2. Ragoyja E. G., Matulis V. E., Ivashkevich O. A. Development of the approach to quantum chemical study of nitrogen oxides reduction catalysts based on titanium dioxide and heteropolyacids. Sviridov Readings. Minsk, 2022, vol. 18, pp. 54−66 (in Russian).
3. Cho K. B., Kim E. J., Seo M. S., Shaik S., Nam W. Correlating DFT-Calculated Energy Barriers to Experiments in Nonheme Octahedral FeIVO Species. Chemistry – A European Journal, 2012, vol. 18, no. 33, pp. 10444–10453. https://doi.org/10.1002/chem.201200096
4. Lin C. H., Qin R. C., Cao N., Wang D., Liu C.-G. Synergistic Effects of Keggin-Type Phosphotungstic Acid-Supported Single-Atom Catalysts in a Fast NH3–SCR Reaction. Inorganic Chemistry, 2022, vol. 61, no. 48, pp. 19156–19171. https://doi.org/10.1021/acs.inorgchem.2c02759
5. Piccini G., Alessio M., Sauer J. Ab initio Calculation of Rate Constants for Molecule-Surface Reactions with Chemical Accuracy. Angewandte Chemie International Edition, 2016, vol. 55, no. 17, pp. 5235–5237. https://doi.org/10.1002/anie.201601534