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Bonding and Charge Distribution in Polyoxometalates: A Bond Valence Approach pp 67–127Cite as

A bond model for polyoxometalate ions composed of MO6 octahedra (MOk polyhedra with k>4)

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Part of the book series: Structure and Bonding ((STRUCTURE,volume 93))

Abstract

The literature relating to the bonding in polyoxometalate ions is reviewed. The author's opinions are presented and expanded to give a bond model for polyoxometalate ions of the early transition elements (groups V and VI) composed of MO6 octahedra (MOk polyhedra with k>4). This bond model concerns in particular the bond valence (bond lengths) and charge distribution in the polyoxometalate ions and the factors modifying them. It is based on the following commonly used concepts and principles as applied to polyoxometalate ions:

  • Lewis's octet rule, extended to the decet and dodecet rule for MV and MVI;

  • pπ-dπ M=O double bond and the coordinate bond (dative bond);

  • the resonance concept;

  • the resonance bond number (or the bond valence concept and the valence sum rule);

  • polydentate ligands and the chelate effect;

  • the larger space requirements of unshared electron pairs (cf. the VSEPR model);

  • the model of multicenter pπ-dπ multiple bonds for certain μ-oxo bridges between metal atoms;

  • Brønsted's acid/base concept and acid/base equilibria;

  • Pauling's rules for the acid/base strength of (monomeric) oxoacids/oxoanions;

  • the law of mass action (Le Chatelier's principle), and others.

The result is a set of resonance structures for polyoxometalate species in which three types of resonance can be distinguished. These, in turn, explain:

  • the cohesion of the strongly distorted tetrahedral MO4 building units in the structures by formation of MO6 octahedra and hence the enhanced stability of the polyoxometalate ions;

  • the distribution of the formal ionic charge over (nearly) all types of oxygen atoms, but preferably the terminal ones;

  • the occurrence of positively charged oxygen atoms, caused by charge separation processes;

  • the enhanced basicity of polyoxometalate ions; and further features.

A “meshing effect” defines the increase of the bond valence in inner (bridging) M−O bonds and hence the stabilization of the structures due to extension of the coordination spheres of MO4 tetrahedra. Thus, the bond lengths of the different structure types are governed by a maximization of the bond valence of the inner, bridging (or minimization of the bond valence of the outer, terminal, in contrast to frequent statements in the literature) M−O bonds. The limits of the maximization of the inner bond valences of the polyoxometalate ions are determined

  • by minimum stoichiometric requirements for corresponding resonance formulae (inevitability of charge on bridging oxygen atoms);

  • by the necessity to fulfill simultaneously the geometrical relationships of the M−O bond lengths (as defined by their interdependence in the M−O frameworks) and the valence sum rule for M and O atoms which are interrelated through the bond length-bond valence function;

  • by (for the solid state) the packing of (poly)anions, cations, and molecules of water of crystallization with respect to the requirements of their size, shape, and charge;

  • and/or by the capacity of the terminal oxygen atoms for the acceptance of unshared electron pairs in relation to that of the bridging oxygen atoms.

The principle of the stabilization of polymeric species by maximization of their inner bond valence, which is simultaneously connected with an increase of the basicity of the species, is, however, only valid for a certain range of acidification of the oxometalate solution from which or in which the species form. The overlying principle is ultimately the consumption of H+ ions in the MO w−4 /H+ systems, thus fulfilling the requirements of Le Chatelier's principle.

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  1. Institut für Anorganische Chemie, Universität Göttigen, Tammannstraße 4, D-37077, Göttingen, Germany

    K. H. Tytko

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Allen J. Bard Ian G. Dance Peter Day FRS James A. Ibers Toyohi Kunitake Thomas J. Meyer D. Michael P. Mingos Herbert W. Roesky Jean-Pierre Sauvage Arndt Simon Fred Wudl

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Tytko, K.H. (1999). A bond model for polyoxometalate ions composed of MO6 octahedra (MOk polyhedra with k>4). In: Bard, A.J., et al. Bonding and Charge Distribution in Polyoxometalates: A Bond Valence Approach. Structure and Bonding, vol 93. Springer, Berlin, Heidelberg. https://doi.org/10.1007/BFb0103380

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