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Activated Mn-MACHO Complexes Form Stable CO2 Adducts.

Ajeet Singh1, Gregor Kemper1, Thomas Weyhermüller1

  • 1Max Planck Institute for Chemical Energy Conversion, Stiftstrasse 34-36, 45470, Mülheim an der Ruhr, Germany.

Chemistry (Weinheim an Der Bergstrasse, Germany)
|November 30, 2023
PubMed
Summary

Manganese complexes with MACHO ligands react with carbon dioxide (CO2) to form metallacycles. These CO2 adducts are less reactive, acting as masked catalysts in CO2 transformations.

Keywords:
carbon dioxide activationhomogeneous catalysismanganese catalystsmetal-ligand cooperativitypincer complexes

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Area of Science:

  • Organometallic Chemistry
  • Coordination Chemistry
  • Catalysis

Background:

  • Manganese carbonyl complexes with MACHO ligands are known catalysts.
  • Carbon dioxide (CO2) activation is crucial for sustainable chemistry.
  • Understanding reaction intermediates is key to catalyst design.

Purpose of the Study:

  • To investigate the reaction of manganese(I) amido complexes with CO2.
  • To characterize the resulting metallacycle adducts.
  • To evaluate the reactivity and stability of these adducts.

Main Methods:

  • Synthesis of manganese(I) carbonyl complexes with MACHO ligands.
  • Reaction of amido complexes with CO2.
  • Characterization of the {Mn-N-C-O} metallacycles.
  • Comparative reactivity studies.

Main Results:

  • Formation of stable 4-membered {Mn-N-C-O} metallacycles upon CO2 reaction.
  • Adduct stability inversely correlates with the steric bulk of phosphine substituents (R=isopropyl > adamantyl).
  • CO2 adducts exhibit reduced reactivity compared to parent amido complexes.

Conclusions:

  • The CO2 adducts serve as masked forms of active amido catalysts.
  • These metallacycles may function as off-loop species or branching points in CO2 catalytic cycles.
  • This work provides insights into CO2 fixation mechanisms and catalyst deactivation pathways.