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Mixed-Valence Single-Atom Catalyst Derived from Functionalized Graphene.

Aristides Bakandritsos1, Ravishankar G Kadam1, Pawan Kumar1

  • 1Regional Centre of Advanced Technologies and Materials, Department of Physical Chemistry, Faculty of Science, Palacký University Olomouc, Šlechtitelu˚ 27, 783 71, Olomouc, Czech Republic.

Advanced Materials (Deerfield Beach, Fla.)
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Summary

This study introduces a novel single-atom catalyst using cyanographene to anchor copper ions, enabling efficient and selective oxidation reactions crucial for pharmaceuticals. The catalyst demonstrates high performance and recyclability with minimal metal usage.

Keywords:
CH oxidationamine couplingcooperative catalysisgraphenesingle-atom catalysis

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Area of Science:

  • Catalysis
  • Materials Science
  • Nanotechnology

Background:

  • Single-atom catalysts (SACs) offer advantages over traditional catalysts but face challenges in metal atom stability and valence state control.
  • Developing robust ligands for stable metal coordination and preventing leaching or nanoparticle formation are key hurdles in SAC development.

Purpose of the Study:

  • To develop a stable and efficient single-atom catalyst for oxygen-mediated reactions.
  • To explore the use of functionalized graphene as a robust support for single-atom catalysts.
  • To investigate the catalytic activity of mixed-valence copper species on graphene for pharmaceutical synthesis.

Main Methods:

  • Functionalization of graphene with nitrile groups to create cyanographene for robust copper ion coordination.
  • Characterization of the resulting 2D mixed-valence single-atom catalyst (SAC).
  • Evaluation of the SAC's performance in O2-mediated oxidative coupling of amines and oxidation of benzylic C-H bonds.

Main Results:

  • Cyanographene effectively coordinated Cu(II) ions, which were partially reduced to Cu(I) via graphene-induced charge transfer, forming a mixed-valence SAC.
  • The developed SAC achieved high conversions (up to 98%) and selectivities (up to 99%) in amine oxidative coupling and benzylic C-H oxidation reactions.
  • The catalyst demonstrated excellent recyclability with very low metal loadings, highlighting the synergistic effect of Cu(I)/Cu(II) species.

Conclusions:

  • The developed 2D mixed-valence SAC based on cyanographene is highly effective for key pharmaceutical synthesis reactions.
  • The strategy of using functionalized graphene supports opens avenues for creating a diverse range of SACs, as shown with Fe on carboxy-graphene.
  • This work provides a robust platform for designing advanced single-atom catalysts with tunable electronic properties and enhanced stability.