Citation: Benben Huang, Mengzhou Yang, Xin Lei, Wen Gan, Zhixun Luo. A comparative study on the reactivity of cationic niobium clusters with nitrogen and oxygen[J]. Chinese Chemical Letters, ;2022, 33(2): 1058-1064. doi: 10.1016/j.cclet.2021.04.020 shu

A comparative study on the reactivity of cationic niobium clusters with nitrogen and oxygen

Benben Huang ^{a, b} ,
Mengzhou Yang ^{a, b} ,
Xin Lei ^b ,
Wen Gan ^{a, b} ,
Zhixun Luo ^{a, *,}

a.
Beijing National Laboratory for Molecular Sciences (BNLMS), State Key Laboratory for Structural Chemistry of Unstable and Stable Species, Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, China
b.
University of Chinese Academy of Sciences, Beijing 100049, China

zxluo@iccas.ac.cn

Received Date: 22 February 2021
Revised Date: 1 April 2021
Accepted Date: 12 April 2021
Available Online: 19 April 2021

Figures(6)

We have prepared well-resolved Nb_n⁺ (n = 1–10) clusters and report here an in-depth study on the essentially different reactivity with N₂ and O₂, by utilizing a multiple-ion laminar flow tube reactor in tandem with a customized triple quadrupole mass spectrometer (MIFT-TQMS). As results, the Nb_n⁺ clusters are found to readily react with N₂ and form adsorption products Nb_nN_2m⁺; in contrast, the reactions with O₂ give rise to Nb_nO₁₋₄⁺Oproducts, and the odd-oxygen products indicate O-O bond dissociation, as well as increased mass abundance of NbO⁺ pertaining to oxygen-etching reactions. We illustrate how N₂ prefers a physical adsorption on Nb_n⁺ clusters with an end-on orientation for all the products, and allow for size-selective Nb_n⁺ clusters to act as electron donor or acceptor in forming Nb_nN_2m⁺. In contrast to these nitrides, the dioxides Nb_nO₂⁺ display much larger binding energies, with O₂ always as an electron acceptor, corresponding to superoxide or peroxide states in the initial reactions. Density-of-states and orbital analyses show that the interactions between Nb_n⁺ and O₂ are dominated by strong π-backdonation indicative of incidental electron transfer; whereas weak π-backdonation and simultaneous σ donation interactions exist in Nb_nN₂⁺. Further, reaction dynamics analysis illustrates the different interactions for N₂ and O₂ in approaching the Nb_n⁺ clusters, showing the energy diagrams for N₂ adsorption and O-O bond dissociation in producing odd-oxygen products. Fragment analyses with orbital correlation and donor-acceptor charge transfer are also performed, giving rise to full insights into the reactivities and interactions of such transition metal clusters with typical diatomic molecules.
- Gas phase reaction,
- Nb cluster,
- Chemical adsorption,
- Orbital analysis,
- Energy decomposition analysis
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