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High nuclearity iridium-platinum clusters: synthesis, structures, bonding, and reactivity
Richard D Adams1, Burjor Captain, Michael B Hall
1Department of Chemistry and Biochemistry, USC Nanocenter, University of South Carolina, Columbia, South Carolina 29208, USA. Adams@mail.chem.sc.edu
Journal of the American Chemical Society
|January 20, 2005
Summary
This study synthesizes novel platinum-iridium cluster compounds, Ir4(CO)12[Pt(PBu(t)3)]2, Ir8(CO)12[Pt(PBu(t)3)]4, and Ir6(CO)10[Pt(PBu(t)3)]4, revealing complex structures and bonding. A new tetrahydrido complex, Ir6(CO)8[Pt(PBu(t)3)]4(mu-H)4, was also formed.
Area of Science:
- Organometallic Chemistry
- Inorganic Chemistry
- Materials Science
Background:
- Iridium carbonyl clusters are foundational in organometallic chemistry.
- Platinum phosphine complexes offer unique reactivity and structural diversity.
- Exploring mixed-metal clusters expands understanding of bonding and catalysis.
Purpose of the Study:
- To synthesize and characterize novel platinum-iridium carbonyl clusters.
- To investigate the structural evolution of these clusters with varying reaction conditions.
- To explore the reactivity of these clusters, including hydrogenation.
Main Methods:
- Reactions of iridium tetracarbonyl dodecacarbonyl (Ir4(CO)12) with bis(di-tert-butylphosphino)platinum(0) [Pt(PBu(t)3)2].
- Characterization using 1H and 31P Nuclear Magnetic Resonance (NMR) spectroscopy.
- Single-crystal X-ray diffraction analysis for structural determination.
- Fenske-Hall molecular orbital calculations to elucidate bonding.
Main Results:
- Synthesis of Ir4(CO)12[Pt(PBu(t)3)]2 at room temperature, featuring Pt groups bridging Ir4 edges.
- Formation of higher nuclearity clusters Ir8(CO)12[Pt(PBu(t)3)]4 and Ir6(CO)10[Pt(PBu(t)3)]4 at elevated temperatures.
- Characterization of a tetrahydrido complex Ir6(CO)8[Pt(PBu(t)3)]4(mu-H)4 via hydrogenation of Ir6(CO)10[Pt(PBu(t)3)]4.
- Molecular orbital calculations revealed delocalized Pt-Ir bonding.
Conclusions:
- The study successfully synthesized and structurally characterized four novel platinum-iridium clusters.
- Reaction conditions significantly influence the nuclearity and structure of the resulting clusters.
- The formation of the tetrahydrido complex demonstrates the reactivity of these mixed-metal systems.
- Delocalized bonding plays a crucial role in the stability of these complex organometallic structures.
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