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The influence of spatial limits on the modeling chemical reactivity: the example of CO2 hydration in MeX zeolites (Me = K, Rb, Cs)статья
Статья опубликована в высокорейтинговом журнале
Информация о цитировании статьи получена из
Web of Science,
Scopus
Статья опубликована в журнале из списка Web of Science и/или Scopus
Дата последнего поиска статьи во внешних источниках: 10 апреля 2019 г.
- Авторы: Rybakov A.A., Bryukhanov I.A., Trubnikov D.N., Larin A.V.
- Журнал: International Journal of Quantum Chemistry
- Том: 119
- Номер: 5
- Год издания: 2019
- Издательство: John Wiley & Sons Inc.
- Местоположение издательства: United States
- Первая страница: e25820
- DOI: 10.1002/qua.25820
- Аннотация: Zeolite cell size variations upon cationic exchange are frequently disregarded while calculating chemical reactions with rather bulky reagents using periodic boundary conditions. Traditional cluster models are often constructed from a fixed unit cell and cannot be influenced by spatial limits imposed by the cationic exchange. Herein, an example of the reaction between the small reagents (H2O and CO2) illustrates a necessity to check this assumption for zeolites with large porous space such as alkali exchanged forms of FAU zeolites. The interplay of two factors (space for the reaction center and mobility of alkali cations) forces lattice parameters to play a crucial role for the accurate computation of activation barrier of CO2 hydration. While the CO2 hydration is modeled in the MeX forms (Me = K, Rb, or Cs) with a fixed volume of NaX one, barrierless reactions were predicted for Me = Rb or Cs that is not confirmed by experimental data. When the cell parameters were optimized with VASP in models with Rb or Cs cations after Na/Me exchange, activation energies were obtained in agreement with the experimental data that CO2 hydration in CsX occurs at room temperature.
- Добавил в систему: Ларин Александр Владимирович
Прикрепленные файлы
| № | Имя | Описание | Имя файла | Размер | Добавлен |
|---|---|---|---|---|---|
| 1. | Полный текст | 10.1002qua.25820.pdf | 2,2 МБ | 4 ноября 2018 [Starmm11] |