The Role of Ionic and Cluster Active Centers of Pt/CeO2 Catalysts in CO Oxidation. Experimental Study and Mathematical Modeling
Научная публикация
| Общая информация |
Язык:
Английский,
Жанр:
Статья (Full article),
Статус опубликования:
Опубликована,
Оригинальность:
Оригинальная
|
| Журнал |
Chemical Engineering Science
ISSN: 0009-2509
, E-ISSN: 1873-4405
|
| Вых. Данные |
Год: 2023,
Том: 267,
Страницы: 118328
Страниц
: 14
DOI:
10.1016/j.ces.2022.118328
|
| Ключевые слова |
CO oxidation; Platinum-ceria catalysts; Cluster active centers; Low-temperature activity; Associative mechanism;
Mathematical modeling |
| Авторы |
Lashina Elena A.
1
,
Slavinskaya Elena M.
1
,
Stonkus Olga A.
1
,
Stadnichenko Andrei I.
1
,
Romanenko Anatolii V.
1
,
Boronin Andrei I.
1
|
| Организации |
| 1 |
Boreskov Institute of Catalysis SB RAS, Novosibirsk, Russian Federation
|
|
Информация о финансировании (1)
|
1
|
Министерство науки и высшего образования Российской Федерации
|
0239-2021-0003
|
In this work, for the first time, the experimental catalytic kinetics of the CO oxidation reaction on platinum–ceria catalysts was simulated in a wide temperature range −50–450 °C. On the basis of the experiments performed, a substantiation of the catalytic action of two types of Pt-containing active centers in the form of isolated [Pt2+-O4] ions and PtOx clusters is presented. The relative content of these platinum forms on the ceria surface is controlled by the loading of platinum. Using the catalysts with a low content of platinum, where the active centers are isolated [Pt2+-O4] ions, a satisfactory simulation of CO conversion depending on temperature was carried out based on the concepts of the Mars-van Krevelen (MvK) mechanism. It was established that these centers provide the catalysts activity in the temperature range above 100 °C. To simulate the reaction kinetics in the temperature range below 100 °C, the Pt-O-Pt active centers based on PtOx cluster forms were considered. The PtOx cluster forms made it possible to consider both the MvK mechanism and temperature-dependent associative Low-T mechanism. The introduction into the kinetic scheme of stages simulating the implementation of both the Low-T and the MvK mechanisms allowed us to perform complete quantitative modeling of the experimental data over the entire temperature range of the reaction from −50 °C to 450 °C.