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Structure and Bonding Patterns in Large Molecular Ligated Metal Clusters

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The Chemical Bond I

Part of the book series: Structure and Bonding ((STRUCTURE,volume 169))

Abstract

Although there will always be an Edisonian component to a search for new cluster compounds, the greater the understanding of the underlying chemistry, the more focused and efficient the search. It is why the rapid expansion of the synthesis and characterization of ligated transition-metal clusters over the last decades has been accompanied by theories about their bonding and electronic properties with the aid of conceptual ideas and theoretical models such as the development of electron-counting rules which govern the relationship between the structure and the electron count. This review summarizes these theoretical models, their historical development, their limits, and using a selection of specific examples among the extensive panoply of large ligated metal clusters available in the literature, shows how they can help in understanding their structural and electronic properties.

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Notes

  1. 1.

    In some cases, nonbonding orbitals can be unoccupied because lying too high in energy for being accessible.

  2. 2.

    This process is nicely detailed for the octahedron example in Ref. [7].

  3. 3.

    Organometallic chemists often count electrons in adding to the skeletal electrons all the other electrons lying in the metal coordination sphere, but not participating significantly to the skeletal bonding. An ML3 fragment will thus contribute to this count with 12 additional electrons (6 nonbonding “t 2g ” d-type electrons and the 6 electrons coming from the ligands) (see Fig. 1). Within this electron-counting scheme, [Ru6(CO)18]2−, and [Ru4(CO)12Bi2] are 86 (14 + 6 x 12) and 62 (14 + 4 x 12) electron species, respectively.

  4. 4.

    This simple rule may not apply in the case of multicapped clusters, but symmetry considerations may be used to evaluate the number of additional bonding MOs present (see Ref [7]).

  5. 5.

    Variations of this model can be found in Refs. [89, 90].

  6. 6.

    The tetracapped tetrahedron can also accommodate 8 electrons (see ref. [117]).

Abbreviations

AO:

Atomic orbital

ccp:

Cubic close packed

Cp*:

Pentamethylcyclopentadienyl

CVE:

Cluster valence electron

DFT:

Density functional theory

EAN:

Effective atomic number

Et:

Ethyl

fcc:

Face-centered cubic

FO:

Frontier orbital

hcp:

Hexagonal close packed

HOMO:

Highest occupied molecular orbital

i-Pr:

Isopropyl

LUMO:

Lowest unoccupied molecular orbital

Me:

Methyl

MO:

Molecular orbital

n-Pr:

n-propyl

NR2 :

Organoamino

Ph:

Phenyl

PR3 :

Organophosphine

PSEPT:

Polyhedral skeletal electron pair theory

p-Tol:

4-Methylphenyl

SEP:

Skeletal electron pair

SMO:

Skeletal molecular orbital

SR:

Organothiolato

TSH:

Tensor surface harmonic

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Acknowledgments

We would like to thank Dr Samia Kahlal (Rennes) for providing helpful comments.

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Authors and Affiliations

  1. Institut des Sciences Chimiques de Rennes, UMR 6226 CNRS-Université de Rennes 1, 35042, Rennes cedex, France

    Jean-Yves Saillard & Jean-François Halet

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  1. Jean-Yves Saillard
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Editors and Affiliations

  1. Inorganic Chemistry Laboratory, University of Oxford, Oxford, United Kingdom

    D. Michael P. Mingos

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Saillard, JY., Halet, JF. (2016). Structure and Bonding Patterns in Large Molecular Ligated Metal Clusters. In: Mingos, D. (eds) The Chemical Bond I. Structure and Bonding, vol 169. Springer, Cham. https://doi.org/10.1007/430_2015_210

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