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Radical reactions can occur either intermolecularly or intramolecularly. In an intermolecular radical reaction, a nucleophilic radical adds to an electrophilic alkene or vice versa. In such reactions, the radical and generally the alkene, which is also called the radical trap, are two different molecules. Additionally, for such intermolecular reactions to occur, the radical trap must be active, present in an excess concentration, and the radical starting material must have a weak...
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Area of Science:

  • Nanochemistry
  • Materials Science
  • Physical Chemistry

Background:

  • Monolayer protected clusters (MPCs) are atomically precise nanomaterials with unique properties.
  • Interactions between individual MPCs are crucial for developing new materials and applications.
  • Understanding reaction mechanisms in MPCs is essential for their controlled synthesis and functionalization.

Purpose of the Study:

  • To demonstrate the first example of intercluster reactions between atomically precise noble metal clusters.
  • To investigate the mechanism and thermodynamic feasibility of these reactions.
  • To explore the potential of intercluster reactions for alloying and heteroatom doping.

Main Methods:

  • Utilized gold (Au25(SR)18) and silver (Ag44(SR)30) clusters as model systems.
  • Employed electrospray ionization and matrix-assisted laser desorption/ionization mass spectrometry to analyze reaction products.
  • Conducted Density Functional Theory (DFT) calculations to assess thermodynamic feasibility and propose a reaction mechanism.

Main Results:

  • Observed spontaneous intercluster reactions between Au and Ag clusters under ambient conditions.
  • Demonstrated metal atom and ligand exchange during the reaction.
  • Achieved facile heteroatom doping of silver into gold clusters, incorporating up to 20 silver atoms.
  • Identified the metal core-thiolate interface as critical for reaction initiation and kinetics.

Conclusions:

  • Intercluster reactions represent a novel pathway for creating alloyed noble metal clusters.
  • This method provides an efficient route for doping MPCs with different metal atoms.
  • The findings establish a foundation for the broader chemistry of monolayer protected clusters and their applications.