Re-Co Alloys and Single-Atom Re Catalysts in Ammonia Synthesis: A DFT Study Научная публикация
| Журнал |
Molecular Catalysis
ISSN: 2468-8231 |
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| Вых. Данные | Год: 2021, Том: 513, Номер статьи : 111801, Страниц : 11 DOI: 10.1016/j.mcat.2021.111801 | ||
| Ключевые слова | Active site modeling; Ammonia synthesis; Re-Co alloy; Single-atom catalyst | ||
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| Организации |
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Информация о финансировании (1)
| 1 | Министерство науки и высшего образования Российской Федерации (с 15 мая 2018) | 0239-2021-0002 |
Реферат:
In this study, density functional theory calculations and microkinetic modeling were used to estimate the catalytic activity of ReδCo1-δ(0001) alloys (δ = 0; 0.25; 0.5; 0.75, 1), and Co(0001)-supported single- Re1 and dual-atom Re2 centers in the synthesis of ammonia. Nitrogen atoms (Nad) form an ordered structure, and the bridge state is most active among others on the Re(0001) plane; while Nad are concentrated around the Re1 and Re2 centers, splitting in electronic and thermodynamic properties. The specific catalytic activity of the centers Re1, Re2 and the Re(0001) plane changes in the order of 8.0·103, 32.0, and 1.0, respectively, due to weakly bound but highly active Nad, which are stabilized by strongly bound and low-active Nad. The calculations revealed the NRe3 state on the Re3Co1 alloy with an abnormally high binding energy (BE) of -7.05 eV, unequal Re-N distances and Re5d fillings, in contrast to the similar NRe3 state on Re(0001) with BE = -6.71 eV. A variable synergism of Re-Co alloys was established: the Re3Co1 or Re1Co3 alloy exhibits maximum catalytic activity if the rate-determining step is the formation or hydrogenation of Nad under appropriate experimental conditions, respectively.
Библиографическая ссылка:
Cholach A.R.
, Bryliakova A.A.
Re-Co Alloys and Single-Atom Re Catalysts in Ammonia Synthesis: A DFT Study
Molecular Catalysis. 2021. V.513. 111801 :1-11. DOI: 10.1016/j.mcat.2021.111801 WOS Scopus РИНЦ CAPlus OpenAlex
Re-Co Alloys and Single-Atom Re Catalysts in Ammonia Synthesis: A DFT Study
Molecular Catalysis. 2021. V.513. 111801 :1-11. DOI: 10.1016/j.mcat.2021.111801 WOS Scopus РИНЦ CAPlus OpenAlex
Даты:
| Поступила в редакцию: | 2 июл. 2021 г. |
| Принята к публикации: | 30 июл. 2021 г. |
| Опубликована в печати: | 1 авг. 2021 г. |
| Опубликована online: | 13 авг. 2021 г. |
Идентификаторы БД:
| Web of science: | WOS:000693014900009 |
| Scopus: | 2-s2.0-85112314434 |
| РИНЦ: | 47017562 |
| Chemical Abstracts: | 2021:1788360 |
| OpenAlex: | W3195498928 |