NO + H2 Reaction over Pd(110): TPD, TPR and DFT Study Научная публикация
| Журнал |
Molecular Catalysis
ISSN: 2468-8231 |
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| Вых. Данные | Год: 2018, Том: 448, Страницы: 53-62 Страниц : 10 DOI: 10.1016/j.mcat.2018.01.009 | ||||
| Ключевые слова | DFT, NO dissociation, NO reduction, Palladium, Surface chemical reactions | ||||
| Авторы |
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| Организации |
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Информация о финансировании (2)
| 1 | Федеральное агентство научных организаций России | 0303-2016-0003 |
| 2 | Федеральное агентство научных организаций России | 0303-2016-0001 |
Реферат:
Temperature-programming desorption (TPD) and temperature-programmed reaction (TPR) have been applied to study the reduction of 15NO by deuterium on a Pd(110) surface. TPR results show that the reaction occurs in the autocatalytic regime of surface explosion with the rate-limiting step of 15NOads dissociation into highly reactive Oads and 15Nads atoms. The steady-state reaction leads to formation of 15N2, D2O, 15ND3 and 15N2O products. The phenomena of a reaction rate hysteresis observed during a heating-cooling cycle can be attributed to accumulation of 15NOads at low temperatures followed by surface explosion at T ∼ 490 K. The binding energies and structural parameters of species involved in the NO + H2 reaction over Pd(110) have been calculated by the DFT technique, and plausible reaction pathways have been considered. NO dissociation from the most stable short bridge site (Eb = −1.94 eV) occurs via the intermediates in on-top and long bridge modes with lower binding energy (Eb = −1.31 to 1.65 eV). The energy of transition states reaches 0.2–0.26 eV over energy of NO in a gas phase, which confirms the rate-limiting role of NO dissociation. It has been demonstrated that OHads-group formation is the rate-limiting step of water molecule generation. Subsequent H2O formation occurs via disproportionation of the OHads intermediates.
Библиографическая ссылка:
Bryliakova A.A.
, Matveev A.V.
, Tapilin V.M.
, Gorodetskii V.V.
NO + H2 Reaction over Pd(110): TPD, TPR and DFT Study
Molecular Catalysis. 2018. V.448. P.53-62. DOI: 10.1016/j.mcat.2018.01.009 WOS Scopus РИНЦ CAPlusCA OpenAlex
NO + H2 Reaction over Pd(110): TPD, TPR and DFT Study
Molecular Catalysis. 2018. V.448. P.53-62. DOI: 10.1016/j.mcat.2018.01.009 WOS Scopus РИНЦ CAPlusCA OpenAlex
Даты:
| Поступила в редакцию: | 1 окт. 2017 г. |
| Принята к публикации: | 10 янв. 2018 г. |
| Опубликована online: | 21 февр. 2018 г. |
| Опубликована в печати: | 1 апр. 2018 г. |
Идентификаторы БД:
| Web of science: | WOS:000428498500007 |
| Scopus: | 2-s2.0-85042407334 |
| РИНЦ: | 35531700 |
| Chemical Abstracts: | 2018:1320087 |
| Chemical Abstracts (print): | 169:311734 |
| OpenAlex: | W2792718760 |