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Experimental Approaches for the Synthesis of Low-Valent Metal-Organic Frameworks from Multitopic Phosphine Linkers

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Electronic structures of Pd(II) dimers.

John E Bercaw¹, Alec C Durrell, Harry B Gray

¹Arnold and Mabel Beckman Laboratories of Chemical Synthesis, California Institute of Technology, Pasadena, California 91125, USA.

Inorganic Chemistry

|January 23, 2010

Summary

Palladium(II) dimers adopt an unusual "clamshell" geometry due to Pd-Pd bonding, influencing their electronic structure and photophysical properties unlike related metal complexes.

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Area of Science:

Inorganic Chemistry
Organometallic Chemistry
Materials Science

Background:

Palladium(II) dimers with bridging ligands (X = OAc or TFA) were investigated.
Expected planar geometry (D(2h) symmetry) was contrasted with observed structures.

Purpose of the Study:

To elucidate the unusual "clamshell" geometry of Pd(II) dimers.
To investigate the electronic structure and bonding interactions within these dimers.
To understand the photophysical properties and their relation to geometry and electronic structure.

Main Methods:

Synthesis and characterization of palladium(II) dimers.
UV-visible and low-temperature fluorescence spectroscopy.
Density Functional Theory (DFT) and Atoms in Molecules (AIM) analyses.

Main Results:

Pd(II) dimers adopted a "clamshell" structure with close Pd-Pd contacts (approx. 2.85 Å) due to a d(8)-d(8) bonding interaction.
These dimers undergo two successive one-electron oxidations.
Distinct photophysical differences were observed compared to planar dimers and monomers lacking Pd-Pd contacts.
Computational studies confirmed Pd-Pd bonding and identified the HOMO as a Pd-Pd antibonding orbital, differing from Rh, Ir, and Pt dimers.

Conclusions:

The "clamshell" geometry is stabilized by a Pd-Pd bonding interaction.
The electronic structure, particularly the orbital ordering, is unique to palladium dimers.
This unique electronic structure explains the observed photophysical properties and differences from other d(8)-d(8) metal dimers.