[en] The geometrical structure, stability, hydriding properties of Mg_nZr (n=1 ~ 11) clusters are studied by the B3LYP method of the density functional theory (DFT) at 6-31+G* (for Mg, H atoms) and Lanl2dz (for Zr atom) levels. The results show that, in most cases, the basic framework of the host Mg_nZr clusters can’t be changed by the adsorption of H₂ and the H₂ molecule prefers a dissociative chemisorption. The Zr atoms tend to stay in the center of clusters and the stability of Mg_nZr clusters becomes better after hydrogenation by comparing the electronic properties, such as VIP and VEA parameters, HOMO-LUMO gaps and chemical hardness. The Mg₃ZrH₂, Mg₆Zr and Mg₈ZrH₂ have better distribution uniformity and symmetry of spin density, indicating better structural stability. Calculated chemisorption energy of the Mg₃ZrH₂ cluster is found maximum in the series. The NEC and DOS of Mg₃ZrH₂ further illuminate the charge transfer and orbitals interactions among the atoms of Mg₃ZrH₂, which suggests the chemical stability after the adsorption of H₂. Finally, the calculated enthalpy difference further confirms the chemisorption of hydrogen on Mg_nZr clusters and the clusters Mg_nZrH₂ (for n=3, 6 and 8) are more exothermic than other considered clusters. Graphical abstract:

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