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Summary
This summary is machine-generated.

Square-planar d(8)-ML4 complexes exhibit Lewis acidic sites that enable M⋅⋅⋅H-C agostic interactions. A new method using high-pressure IR and diffraction studies is proposed to better characterize these interactions, challenging traditional NMR shift criteria.

Keywords:
agostic interactionsbond activationcharge densityhigh pressure

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Area of Science:

  • Inorganic Chemistry
  • Organometallic Chemistry
  • Solid-State Chemistry

Background:

  • Square-planar d(8)-ML4 complexes possess axial Lewis acidic sites.
  • These sites facilitate weak M⋅⋅⋅H-C agostic interactions.
  • Previous assumptions about these interactions are challenged.

Purpose of the Study:

  • To investigate the nature of Lewis acidity in square-planar d(8)-ML4 complexes.
  • To explore the formation of M⋅⋅⋅H-C agostic interactions.
  • To propose a novel method for characterizing M⋅⋅⋅H-C interactions under pressure.

Main Methods:

  • Theoretical analysis of Lewis acidic sites in square-planar d(8)-ML4 complexes.
  • Combined high-pressure infrared (IR) spectroscopy and diffraction studies.
  • Evaluation of (1)H NMR shifts as a criterion for agostic/anagostic interactions.

Main Results:

  • Local Lewis acidic sites in the axial direction of the metal atom were identified.
  • These sites support weakly attractive 3-center-2-electron (3c-2e) M⋅⋅⋅H-C agostic interactions.
  • The use of (1)H NMR shifts to classify M⋅⋅⋅H-C interactions can be unreliable.

Conclusions:

  • Square-planar d(8)-ML4 complexes can form agostic interactions via axial Lewis acidity.
  • A new pressure-based characterization method combining IR and diffraction is proposed.
  • This method offers a more robust way to study M⋅⋅⋅H-C interactions compared to NMR shifts.