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Equatorially connected diruthenium(II,III) units toward paramagnetic supramolecular structures with singular magnetic
M Carmen Barral1, Teresa Gallo, Santiago Herrero
1Departamento de Química Inorganica and Centro de Asistencia a la Investigación de Rayos X, Facultad de Ciencias Químicas, Universidad Complutense de Madrid, Ciudad Universitaria, 28040 Madrid, Spain.
Inorganic Chemistry
|April 26, 2006
Summary
This study synthesizes novel diruthenium complexes by substituting acetate ligands with various carboxylic acids. The resulting complexes exhibit high stability and unique magnetic properties, sensitive to axial ligand changes.
Area of Science:
- Coordination Chemistry
- Organometallic Chemistry
- Materials Science
Background:
- Diruthenium complexes with N,N'-diphenylformamidinate (DPhF) ligands are known for their stability.
- Substitution reactions offer a route to modify the properties of these complexes.
Purpose of the Study:
- To synthesize and characterize new diruthenium complexes by reacting Ru2Cl(O2CMe)(DPhF)3 with various carboxylic acids.
- To investigate the chemical stability, electronic properties, and magnetic behavior of the synthesized complexes.
- To explore the influence of axial ligands on the electronic configuration of the [Ru2(DPhF)3]2+ fragment.
Main Methods:
- Synthesis of seven new diruthenium complexes.
- Characterization using elemental analysis, IR and electronic spectroscopy, mass spectrometry, and cyclic voltammetry.
- Variable-temperature magnetic susceptibility measurements and crystal structure determination (for complexes 2 and 3).
Main Results:
- Successful synthesis of seven diruthenium complexes with diverse carboxylic acid ligands.
- Demonstrated high chemical stability of the [Ru2(DPhF)3]2+ core under various conditions.
- Electrochemical studies revealed a Ru2(5+) <--> Ru2(6+) redox process, with additional oxidations in polynuclear complex 7.
- Magnetic studies showed low antiferromagnetic coupling, with complex 7 exhibiting unusual behavior simulated by a mixture of spin states.
- Sensitivity of the [Ru2(DPhF)3]2+ unit's electronic configuration to axial ligand modifications was confirmed.
Conclusions:
- The [Ru2(DPhF)3]2+ fragment is highly stable, allowing for diverse ligand substitutions.
- The magnetic properties of diruthenium complexes are significantly influenced by the nature of axial ligands.
- Complex 7 presents unique magnetic behavior, suggesting a departure from typical diruthenium(II,III) systems.
- The study provides insights into the electronic structure and magnetic coupling in diruthenium complexes.
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