Document Type

Article

Original Publication Date

2011

Journal/Book/Conference Title

The Journal of Chemical Physics

Volume

134

DOI of Original Publication

10.1063/1.3570578

Comments

Originally published at https://doi.org/10.1063/1.3570578

Date of Submission

October 2015

Abstract

Using density functional theory with generalized gradient approximation, we have performed a systematic study of the structure and properties of neutral and charged trioxides (MO3) and tetraoxides (MO4) of the 3d-metal atoms. The results of our calculations revealed a number of interesting features when moving along the 3d-metal series. (1) Geometrical configurations of the lowest total energy states of neutral and charged trioxides and tetraoxides are composed of oxo and/or peroxo groups, except for CuO3 and ZnO3 which possess a superoxo group, CuO4 + and ZnO4 + which possess two superoxo groups, and CuO3 +, ZnO3 +, and ZnO4 which possess an ozonide group. While peroxo groups are found in the early and late transition metals, all oxygen atoms bind chemically to the metal atom in the middle of the series. (2) Attachment or detachment of an electron to/from an oxide often leads to a change in the geometry. In some cases, two dissociatively attached oxygen atoms combine and form a peroxo group or a peroxo group transforms into a superoxo group and vice versa. (3) The adiabatic electron affinity of as many as two trioxides (VO3 and CoO3) and four tetraoxides (TiO4, CrO4, MnO4, and FeO4) are larger than the electron affinity of halogen atoms. All these oxides are hence superhalogens although only VO3 and MnO4 satisfy the general superhalogen formula.

Rights

Pradhan, K., Gutsev, G.L., Weatherford, C.A., et al. A systematic study of neutral and charged 3d-metal trioxides and tetraoxides. The Journal of Chemical Physics, 134, 144305 (2011). Copyright © 2011 AIP Publishing LLC.

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