Re-Co Alloys and Single-Atom Re Catalysts in Ammonia Synthesis: A DFT Study Full article
| Journal |
Molecular Catalysis
ISSN: 2468-8231 |
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| Output data | Year: 2021, Volume: 513, Article number : 111801, Pages count : 11 DOI: 10.1016/j.mcat.2021.111801 | ||
| Tags | Active site modeling; Ammonia synthesis; Re-Co alloy; Single-atom catalyst | ||
| Authors |
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| Affiliations |
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Funding (1)
| 1 | Ministry of Science and Higher Education of the Russian Federation | 0239-2021-0002 |
Abstract:
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.
Cite:
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 AN 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 AN OpenAlex
Dates:
| Submitted: | Jul 2, 2021 |
| Accepted: | Jul 30, 2021 |
| Published print: | Aug 1, 2021 |
| Published online: | Aug 13, 2021 |
Identifiers:
| Web of science: | WOS:000693014900009 |
| Scopus: | 2-s2.0-85112314434 |
| Elibrary: | 47017562 |
| Chemical Abstracts: | 2021:1788360 |
| OpenAlex: | W3195498928 |