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How Solid Surfaces Control Stability and Interactions of Supported Cationic CuI(dppf) Complexes─A Solid-State NMR

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Interactions between organometallic complexes and solid surfaces significantly alter their properties. This study shows how surface interactions affect complex stability, identifying Cu(dppf)(L)+ complexes as solid-state NMR probes.

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Area of Science:

  • Inorganic Chemistry
  • Materials Science
  • Solid-State NMR Spectroscopy

Background:

  • Organometallic complexes are often immobilized on solid surfaces, but the impact of these interactions on their properties remains poorly understood.
  • Understanding complex-surface interactions is crucial for designing advanced materials and catalysts.

Purpose of the Study:

  • To investigate how different surface immobilization methods (physisorption, ion exchange, covalent bonding) affect the properties and stability of copper(I) organometallic complexes.
  • To explore the use of these complexes as solid-state Nuclear Magnetic Resonance (NMR) probes for studying surface interactions.

Main Methods:

  • Synthesis of Cu(dppf)(L)+ complexes with various ligands.
  • Immobilization of complexes on different solid supports (silica, γ-Al2O3, Na-[Al]SBA-15) via physisorption, ion exchange, and covalent linking.
  • Characterization using 31P Magic Angle Spinning (MAS) NMR spectroscopy, including 31P-31P RFDR and 1H-31P FSLG HETCOR experiments.
  • Density Functional Theory (DFT) calculations to elucidate structural and electronic changes.

Main Results:

  • Physisorption on silica resulted in stable complexes with weak interactions.
  • Adsorption on acidic γ-Al2O3 led to slow complex decomposition.
  • Ion exchange into Na-[Al]SBA-15 induced magnetic inequivalence of 31P nuclei, with DFT confirming MeCN ligand dissociation.
  • Covalent immobilization and ion exchange with bidentate ligands resulted in rigidly bound complexes exhibiting broad 31P Chemical Shift Anisotropy (CSA) tensors.

Conclusions:

  • The interaction between organometallic complexes and functionalized surfaces critically determines and modifies the stability of the complexes.
  • The studied Cu(dppf)(L)+ complexes are effective solid-state NMR probes for analyzing the influence of support surfaces on deposited inorganic complexes.