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Methods of Ex Situ and In Situ Investigations of Structural Transformations: The Case of Crystallization of Metallic Glasses

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Closo versus hypercloso metallaboranes: A DFT study.

Oottikkal Shameema¹, Eluvathingal D Jemmis

¹Department of Inorganic and Physical Chemistry, Indian Institute of Science, Bangalore -12, India.

Inorganic Chemistry

|July 16, 2009

Summary

Transition metals stabilize hypercloso metallaboranes by occupying high-degree vertices, with heavier metals and specific ligand sizes enhancing stability. This study explores their electronic structure and interconversion.

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Area of Science:

* Inorganic Chemistry
* Computational Chemistry
* Materials Science

Background:

* Explores the structural and electronic relationships in metallaboranes.
* Focuses on 9- to 12-vertex closo and hypercloso (isocloso) structures.
* Investigates the role of transition metals in stabilizing these complex borane frameworks.

Purpose of the Study:

* To elucidate the electronic factors governing the stability of hypercloso metallaboranes.
* To understand the influence of transition metal identity and ligand size on structure.
* To analyze the orbital compatibility and bonding interactions within these systems.

Main Methods:

* Density Functional Theory (DFT) calculations were employed.
* Fragment Molecular Orbital (FMO) approach was used for interaction analysis.
* Correlation diagrams were utilized to discuss electronic interconversions.

Main Results:

* Hypercloso structures require n skeleton electron pairs (SEPs) and feature high-degree vertices, unlike closo structures (n+1 SEPs).
* Transition metals, particularly heavier ones with diffused orbitals, effectively stabilize hypercloso geometries.
* Ligand size around the metal atom influences the overall stability of the hypercloso framework.

Conclusions:

* Orbital compatibility is key for transition metal stabilization of hypercloso boranes.
* Heavier transition metals are preferred for forming stable hypercloso structures.
* Electronic interconversion between closo and hypercloso forms is possible via electron addition/removal.