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Adsorption and decomposition mechanism of N2O molecule over MC23 (M = Ru, Mn, V, Pd, and Rh) nanoclusters: A comparative DFT investigation

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Abstract

The adsorption and decomposition of N2O molecule over the surface of the MC23 clusters (M = Ru, Mn, V, Rh, and Pd) clusters were investigated using the dispersion-corrected PBE calculations (PBE-D3). The mechanism of the N2O dissociation over the above clusters has also been proposed, and the results show that the activation energies in PdC23, MnC23, VC23, RuC23, and RhC23 clusters are respectively 33.5, 7.9, 9.3, 24.4, and 42.4 kcal mol−1 in process 1 (TS1), and 68.5, 55.0, 55.3, 23.8, and 52.4 kcal mol−1 in process 2 (TS2). It was also demonstrated that the O2 desorption step in VC23 cluster was considered as the rate-limiting step, while the N2O decomposition step was found to be the rate-determining step for the other clusters. Moreover, the small desorption energies of O2 were obtained in RhC23, MnC23, RuC23, and PdC23 clusters, suggesting that the O2 desorption from the surface of the MC23 catalysts is easy; thereby, the regeneration of their surface metal sites is possible. This characteristic makes the MC23 (M = Mn, Rh, Pd, and Ru) clusters behave as highly active catalysts and therefore they could be potentially used as effective nanocatalysts for the N2O decomposition reaction.

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The data supporting the findings of this study are available within its supplementary material and from corresponding author on reasonable request.

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Authors and Affiliations

  1. Computational Catalysis Group, Laboratory of Applied Chemistry, University of Guelma, Box 401, 24000, Guelma, Algeria

    Meryem Derdare, Abdel-Ghani Boudjahem & Mouhssin Boulbazine

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  2. Abdel-Ghani Boudjahem
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All persons who meet authorship criteria are listed as authors, and all authors certify that they have participated competently in the work to take overall responsibility for the content, including participation in the concept, design, analysis, writing, or revision of the manuscript. Abdel-Ghani Boudjahem: supervision, project administration, writing-original draft, writing- review and editing. Meryem Derdare: software, methodology. Mouhssin Boulbazine: conceptualization, investigation.

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Derdare, M., Boudjahem, AG. & Boulbazine, M. Adsorption and decomposition mechanism of N2O molecule over MC23 (M = Ru, Mn, V, Pd, and Rh) nanoclusters: A comparative DFT investigation. Struct Chem 33, 2043–2062 (2022). https://doi.org/10.1007/s11224-022-01984-2

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