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Area of Science:

  • Organometallic Chemistry
  • Coordination Chemistry
  • Main Group Chemistry

Background:

  • Pincer complexes offer unique reactivity due to their tridentate coordination.
  • Aluminum and boron are key elements in main group and organometallic chemistry, respectively.
  • Understanding the stabilization and reactivity of low-coordinate main group elements is crucial.

Purpose of the Study:

  • To synthesize and characterize novel rhodium pincer complexes featuring bis(N-pyrrolyl)aluminyl (PAlP) and boryl (PBP) units.
  • To investigate the reactivity of the aluminyl site in the PAlP rhodium complex.
  • To explore methods for accessing three-coordinate aluminum centers within a pincer framework.

Main Methods:

  • Synthesis of PAlP and PBP rhodium dicarbonyl complexes.
  • Coordination of pyridine to stabilize the aluminyl site in (PAlpyP)Rh(CO)2.
  • Reactions involving Lewis acid-mediated pyridine abstraction using BF3·Et2O and B(C6F5)3.

Main Results:

  • Successful synthesis of (PAlpyP)Rh(CO)2 with a four-coordinate aluminum center stabilized by pyridine.
  • Unexpected B/Al metathesis occurred upon treatment with BF3·Et2O, forming the (PBP)Rh(CO)2 complex while preserving the pincer structure.
  • Attempted pyridine abstraction with B(C6F5)3 led to dimerization of the PAlP complex via isocarbonyl bridging.

Conclusions:

  • The coordination of pyridine is effective in stabilizing a four-coordinate aluminyl site in rhodium pincer complexes.
  • Lewis acid-mediated reactions can induce unexpected B/Al metathesis, offering an alternative route to boryl complexes.
  • The reactivity of the aluminyl pincer complex is sensitive to the abstraction agent, leading to dimerization under certain conditions.