A DFT study on the copper-single-atom modified 2D electride Ca2N monolayer for ethanol dehydrogenation.
In: International Journal of Hydrogen Energy, Jg. 51 (2024-01-15), S. 970-981
Online
academicJournal
Zugriff:
Two-dimensional (2D) electrides, with electrons confined in interlayer spaces instead of at atomic proximities, have received considerable attention due to their exotic properties. However, the current exploration of electrides in the field of catalysis urgently needs to be expanded. Here, we report novel thermodynamically stable Cu single-atom-modified 2D electride Ca 2 N monolayer catalysts for ethanol dehydrogenation using density functional theory calculations. The interaction and synergistic catalytic mechanism of copper single atoms and Ca 2 N monolayers were thoroughly revealed. The coordination environment of copper greatly affects the reaction sites for ethanol dehydrogenation. Furthermore, it was found that the strong electron transfer ability of Ca 2 N monolayer promoted the adsorption and activation of ethanol molecules on the catalyst, resulting in a cleavage energy barrier of the O–H bond as low as 0.29 eV on Cu 1 /Ca 2 N. Furthermore, turnover frequency (TOF) analysis demonstrates that Cu 1 /Ca 2 N exhibits significantly higher activity compared to Ca 2 N with lower energetic span (δE) of 2.52 eV at 298.15 K for the cycle of ethanol dehydrogenation to acetaldehyde. Our work demonstrates a new avenue to the discovery of 2D electride-based catalysts and provides new insights into the mechanism of ethanol dehydrogenation. [Display omitted] • Cu single-atom-modified 2D electride Ca 2 N monolayer catalysts were constructed. • The mechanism of ethanol dehydrogenation to acetaldehyde has been revealed. • Ca 2 N monolayer boosts ethanol activation with strong electron transfer. • Copper promotes the formation and desorption of hydrogen. • Cu 1 /Ca 2 N monolayer exhibits the lowest energy span of 2.52 eV. [ABSTRACT FROM AUTHOR]
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A DFT study on the copper-single-atom modified 2D electride Ca2N monolayer for ethanol dehydrogenation.
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Autor/in / Beteiligte Person: | Ma, Yuli ; Lang, Junyu |
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Zeitschrift: | International Journal of Hydrogen Energy, Jg. 51 (2024-01-15), S. 970-981 |
Veröffentlichung: | 2024 |
Medientyp: | academicJournal |
ISSN: | 0360-3199 (print) |
DOI: | 10.1016/j.ijhydene.2023.07.121 |
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