Sciact
  • EN
  • RU

NO + H2 Reaction over Pd(110): TPD, TPR and DFT Study Научная публикация

Журнал Molecular Catalysis
ISSN: 2468-8231
Вых. Данные Год: 2018, Том: 448, Страницы: 53-62 Страниц : 10 DOI: 10.1016/j.mcat.2018.01.009
Авторы Bryliakova Anna A. 1 , Matveev Andrey V. 1,2 , Tapilin Vladimir M. 1 , Gorodetskii Vladimir V. 1
Организации
1 Boreskov Institute of Catalysis, Siberian Branch of the Russian Academy of Sciences, Pr. Acad. Lavrentieva, 5, 630090, Novosibirsk, Russia
2 Novosibirsk State University, Pirogova St. 2, 630090, Novosibirsk, Russia
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 Sciact
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
Sciact: 22994
Цитирование в БД:
БД Цитирований
Scopus 2
OpenAlex 1
Альметрики: