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This study reveals how a redox-active ligand in a cobalt complex influences spin states upon donor coordination. Weak donors induce spin flips, while strong donors cause electron transfer, altering the complex

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Area of Science:

  • Inorganic Chemistry
  • Coordination Chemistry
  • Spin Crossover Materials

Background:

  • Cobalt complexes with redox-active ligands are key in understanding spin dynamics.
  • The dipyrrin-bis(phenolato) (DPP) ligand's redox activity influences metal center properties.
  • Exogenous donor coordination can trigger spin-changing events in metal complexes.

Purpose of the Study:

  • To investigate the influence of a redox-active DPP ligand on spin-changing events in a cobalt complex.
  • To elucidate the structural, spin state, and electronic properties of cobalt-donor adducts.
  • To understand the mechanism of spin state changes induced by varying donor strengths.

Main Methods:

  • Synthesis and characterization of a cobalt complex with a redox-active DPP ligand.
  • Coordination of various exogenous donors (THF, pyridine, amines) to the cobalt complex.
  • Utilized experimental techniques: X-ray diffraction, NMR, UV-visible spectroscopy, SQUID, Evans' method.
  • Employed computational methods: Density Functional Theory (DFT), NEVPT2-CASSCF.

Main Results:

  • The starting complex [Co(DPP·)] is an open-shell singlet with a DPP radical coupled to Co(II).
  • Coordination of weak donor THF leads to a triplet adduct [Co(DPP·)(THF)] via spin flip.
  • Stronger donors (pyridine, amines) induce metal-to-ligand electron transfer, forming singlet Co(III) complexes [Co(DPP)(L)].

Conclusions:

  • The redox-active DPP ligand is crucial for stabilizing the cobalt complex and mediating spin changes.
  • Donor strength dictates the outcome: weak donors cause spin flips, strong donors induce redox events.
  • This work provides insights into designing switchable spin states in coordination complexes.