danДоклады Национальной академии наук БеларусиDoklady of the National Academy of Sciences of Belarus1561-83232524-2431The Republican Unitary Enterprise Publishing House "Belaruskaya Navuka"10.29235/1561-8323-2024-68-1-36-45dan-1173Research ArticleХИМИЯCHEMISTRYКвантовохимические расчеты термодинамических характеристик некоторых гетерогенных каталитических процессов c использованием многослойных кластерных моделейQuantum-chemical calculations of thermodynamic characteristics of some heterogeneous catalytic processes with the use of multilayer cluster modelshttps://orcid.org/0000-0002-8344-8438РагойжаЕ. Г.RagoyjaE. G.

Рагойжа Екатерина Георгиевна – старший преподаватель.

Ул. Ленинградская, 14, 220006, Минск

Ragoyja Ekaterina G. – Senior Lecturer.

14, Leningradskaya Str., 220006, Minsk

kateragoyja@yandex.byhttps://orcid.org/0000-0001-9714-9087МатулисВ. Э.MatulisV. E.

Матулис Виталий Эдвардович – канд. хим. наук, доцент.

Ул. Ленинградская, 14, 220006, Минск

Matulis Vitaly E. – Ph. D. (Chemistry), Associate Professor.

14, Leningradskaya Str., 220006, Minsk

vitaly_matulis@lyceum.byhttps://orcid.org/0000-0002-5006-2715ИвашкевичО. А.IvashkevichO. A.

Ивашкевич Олег Анатольевич – академик, д-р хим. наук, гл. науч. сотрудник.

Ул. Ленинградская, 14, 220006, Минск

Ivashkevich Oleg A. – Academician, D. Sc. (Chemistry), Chief Researcher.

14, Leningradskaya Str., 220006, Minsk

ivashkevicho@bsu.byhttps://orcid.org/0000-0001-8034-9568ЛяховД. А.LyakhovD. A.

Ляхов Дмитрий Александрович – науч. сотрудник.

23955, Тувал

Lyakhov Dmitry A. – Researcher.

23955, Thuwal

dmitry.lyakhov@kaust.edu.saМихельсД.MichelsD.

Михельс Доминик – научный сотрудник.

23955, Тувал

Michels Dominik – Researcher.

23955, Thuwal

dominik.michels@kaust.edu.saБелорусский государственный университетBelarusian State UniversityНаучно-исследовательский институт физико-химических проблем Белорусского государственного университетаResearch Institute for Physical Chemical Problems of the Belarusian State UniversityНаучно-технологический университет имени короля АбдаллыKing Abdullah University of Science and Technology2024040320246813645Copyright © Рагойжа Е.Г., Матулис В.Э., Ивашкевич О.А., Ляхов Д.А., Михельс Д., 20242024Рагойжа Е.Г., Матулис В.Э., Ивашкевич О.А., Ляхов Д.А., Михельс Д.Ragoyja E.G., Matulis V.E., Ivashkevich O.A., Lyakhov D.A., Michels D.Данная работа распространяется под лицензией Creative Commons Attribution 4.0.This work is licensed under a Creative Commons Attribution 4.0 License.https://doklady.belnauka.by/jour/article/view/1173

Исследованы подходы к оценке изменения энтальпии, энтропии и энергии Гиббса в ходе процессов адсорбции и гетерогенных каталитических реакций на основании данных квантовохимических расчетов. На основании сравнения с экспериментальными данными по адсорбции CO на поверхности анатаза (TiO2) показана применимость разработанной многослойной кластерной модели для расчета энергии (энтальпии) адсорбции. Проанализированы данные по способам расчета изменения энтропии при гетерогенных процессах, показана применимость теорий идеального двумерного газа и идеального двумерного решетчатого газа для оценки конфигурационного вклада в энтропию гетерогенного процесса. Рассчитаны плотность центров адсорбции на поверхности (101) анатаза, а также заселенность, соответствующая стандартному состоянию идеального двумерного газа. Показана согласованность изученных моделей при небольших заселенностях, а также установлены границы их применимости.

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.

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The authors declare that there are no conflicts of interest present.