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Tethered cationic alkaline earth - olefin complexes.

Sorin-Claudiu Roşca1, Vincent Dorcet, Thierry Roisnel

  • 1Université de Rennes 1, CNRS, Institut des Sciences Chimiques de Rennes, UMR 6226, Campus de Beaulieu, F-35042 Rennes Cedex, France. jean-francois.carpentier@univ-rennes1.fr yann.sarazin@univ-rennes1.fr.

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Summary
This summary is machine-generated.

This study introduces new alkaline earth metal complexes with unique side arms. Cationization of these complexes leads to the first observed binding of olefins to cationic heavy alkaline earth metals.

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Area of Science:

  • Organometallic Chemistry
  • Coordination Chemistry
  • Materials Science

Background:

  • Alkaline earth metal complexes are crucial in catalysis and materials science.
  • Designing complexes with specific functionalities, like olefinic and methoxy groups, is key for novel reactivity.
  • Understanding secondary interactions (e.g., Ae-C, Ae-H) is vital for complex stability and structure.

Purpose of the Study:

  • To synthesize and characterize novel heteroleptic charge-neutral alkaline earth complexes.
  • To investigate the coordination behavior of methoxy and olefinic side arms in these complexes.
  • To explore the formation and properties of cationic alkaline earth complexes and their interactions with olefins.

Main Methods:

  • Synthesis of aminofluoroalcohol ligand and subsequent complexation with calcium (Ca) and strontium (Sr).
  • Characterization using Nuclear Magnetic Resonance (NMR) spectroscopy and X-ray diffraction (XRD) crystallography.
  • Formation of discrete ion pairs via reaction with a proton source and weakly coordinating anion.

Main Results:

  • Two O-bridged dinuclear complexes, [{μ²-ROF}AeN(SiMe2H)2]2 (Ae = Ca, Sr), were successfully prepared and characterized.
  • XRD analysis revealed stabilization through intramolecular Ae-F-C and β-agostic Ae-H-Si interactions; the olefin remained unbound while the methoxy group coordinated.
  • Cationization led to the formation of ion pairs, [({μ²-ROF}Ae·(Et2O)2)2]2+·2[H2N{B(C6F5)3}2]−, with coordinated Et2O molecules.
  • A water adduct, [({μ²-ROF}Sr·(H2O))2]2+·2[H2N{B(C6F5)3}2]−, exhibited strong Sr-F-C interactions.
  • Crucially, the cationic strontium complex demonstrated the first instance of Sr-olefin coordination via Sr-Cπ interactions.

Conclusions:

  • The study successfully synthesized novel alkaline earth metal complexes with functionalized ligands.
  • Cationization of these complexes enhances metal center electrophilicity, enabling olefin coordination to heavy alkaline earth metals for the first time.
  • Further research is needed to create olefin-bound cationic complexes devoid of additional Lewis bases.