(Al16Ti)n± (n=0-3)离子团簇中Ti原子对电子结构及其与H2O分子相互作用的显著影响

doi:10.3866/PKU.WHXB201504222

Abstract

Abstract:

The most stable (Al₁₆Ti)^n± (n=0-3) ions were modeled and optimized using density functional theory combined with all-electron spin-polarized calculations. The geometries, stabilities, and electronic structures of the (Al₁₆Ti)n ± (n=0-3) ionic clusters, as well as the adsorption structures and adsorption energies of H₂O molecules on the (Al₁₆Ti)^n± (n=0-3) ionic clusters, were studied. The results were compared with those obtained for pure (Al₁₇Ti)^n± (n=0-3) ionic clusters. The spatial distributions of the highest occupied molecular orbitals and the lowest unoccupied molecular orbitals for the (Al₁₆Ti)^n± (n=0-3) ionic clusters showed that the free electrons tend to occupy Ti sites. And a few residual free electrons would occupy sites with large curvatures. An extensive structure search was performed to identify the low-energy conformations of (Al₁₆TiH₂O)^n± (n=0-3) complexes. Based on the geometries of the studied adsorption complexes, it was found that the most stable structures were prone to oxygen-based adsorption onto Ti atom. (Al₁₆TiH₂O)⁺ ion featured the shortest average O―H bond length, that was ~0.0003 nm longer than that observed in isolated H₂O molecule. The O―H bond length increased with either increasing or decreasing number of the electrons. The studies implied that Ti dopant in Al ionic clusters improved the dissociation efficiency of H₂O molecules. Furthermore, the doping effect played a more important role than the geometry effect in determining the electronic structures of the (Al₁₆Ti)n ionic clusters and their interaction with H₂O molecules.

Key words: (Al₁₆Ti)^n±, (n=0-3) ions, Adsorption of H₂O molecule, Geometric structure, Electronic structure, Effect of doping

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LIU Yi-Liang, HUA Ya-Wen, JIANG Gang, CHEN Jun. A Dramatic Influence of Ti Atom on the Electronic Structures of (Al₁₆Ti)^n± (n=0?3) Ionic Clusters and Their Interaction with H₂O Molecules[J].Acta Phys. -Chim. Sin., 2015, 31(7): 1315-1322.

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A Dramatic Influence of Ti Atom on the Electronic Structures of (Al₁₆Ti)^n± (n=0?3) Ionic Clusters and Their Interaction with H₂O Molecules

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A Dramatic Influence of Ti Atom on the Electronic Structures of (Al16Ti)n± (n=0?3) Ionic Clusters and Their Interaction with H2O Molecules

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A Dramatic Influence of Ti Atom on the Electronic Structures of (Al₁₆Ti)^n± (n=0?3) Ionic Clusters and Their Interaction with H₂O Molecules