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Controlling Substrate Binding to Fe4S4 Clusters through Remote Steric Effects.

Alexandra C Brown1, Daniel L M Suess1

  • 1Department of Chemistry , Massachusetts Institute of Technology , Cambridge , Massachusetts 02139 , United States.

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Area of Science:

  • Bioinorganic Chemistry
  • Organometallic Chemistry
  • Coordination Chemistry

Background:

  • Iron-sulfur (Fe-S) clusters are crucial in enzymes, with protein scaffolds dictating their reactivity.
  • Synthetic Fe-S clusters offer potential for controlled reactivity through ligand design.
  • N-heterocyclic carbene (NHC) ligands provide tunable steric and electronic properties for metal cluster stabilization.

Purpose of the Study:

  • To synthesize and characterize site-differentiated [Fe4S4] clusters ligated by NHC ligands with varying steric profiles.
  • To investigate the influence of ligand sterics on cluster reactivity, particularly ligand redistribution and substrate binding.
  • To establish a method for controlling the coordination chemistry at specific iron sites within cuboidal Fe-S clusters.

Main Methods:

  • Synthesis of 3:1 site-differentiated [Fe4S4] clusters using IMes and IiPrMe NHC ligands.
  • Reactions with counterions (NaBArF4) and solvents (Et2O, THF) to form adducts.
  • Displacement of solvent ligands with tert-butyl isocyanide (tBuNC) to form isocyanide adducts.
  • Comparative reactivity studies based on the steric bulk of the NHC ligands.

Main Results:

  • The sterically hindered IMes ligand prevented ligand redistribution, enabling the formation of a stable mono-isocyanide adduct [(IMes)3Fe4S4(CNtBu)][BArF4].
  • The less hindered IiPrMe ligand resulted in typical reactivity, including ligand redistribution to a homoleptic cluster and formation of a tri-isocyanide adduct.
  • The IMes ligand's steric bulk created a defined binding pocket at the apical iron, leading to a coordinatively unsaturated and labile Fe site.

Conclusions:

  • Steric control exerted by NHC ligands is a viable strategy to modulate the reactivity of synthetic Fe-S clusters.
  • This approach allows for the selective generation of coordinatively unsaturated sites on cuboidal metalloclusters.
  • The findings offer new avenues for designing functional Fe-S mimics with tailored reactivity for catalytic applications.