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In the presence of an aqueous base and a halogen, primary amides can lose the carbonyl (as carbon dioxide) and undergo rearrangement to form primary amines. This reaction, called the Hofmann rearrangement, can produce primary amines (aryl and alkyl) in high yields without contamination by secondary and tertiary amines.
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Excited-State N2 Dissociation Pathway on Fe-Functionalized Au.

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Localized surface plasmon resonances (LSPRs) can enable light-activated catalysis. This study shows LSPRs can significantly lower the energy barrier for nitrogen dissociation, a key step in ammonia synthesis.

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Area of Science:

  • Surface science and catalysis
  • Plasmonics and nanotechnology
  • Computational chemistry

Background:

  • Localized surface plasmon resonances (LSPRs) facilitate light-driven chemical reactions on metal nanoparticles.
  • Nitrogen (N2) dissociation is a challenging, energy-intensive step in ammonia synthesis via the Haber-Bosch process.
  • Overcoming the high activation energy for N2 dissociation is crucial for efficient ammonia production.

Purpose of the Study:

  • To investigate the potential of LSPRs to lower the activation energy for N2 dissociation on a catalytic surface.
  • To explore the use of an Fe-doped Au(111) surface for enhanced N2 dissociation via plasmonic effects.
  • To calculate excited-state potential energy surfaces for N2 dissociation on the Fe-doped Au(111) surface.

Main Methods:

  • Density functional embedding theory with embedded n-electron valence second-order perturbation theory.
  • Calculation of excited-state potential energy surfaces for N2 dissociation.
  • Modeling of N2 dissociation on an Fe-doped Au(111) surface.

Main Results:

  • The ground-state dissociation activation energy for N2 on Fe-doped Au(111) was calculated to be 4.74 eV/N2, with Fe as the active site.
  • Multiple resonance energy transfers (RETs) between electronically excited states were identified.
  • These RETs effectively reduced the dissociation barrier to 1.33 eV.

Conclusions:

  • LSPRs, coupled with resonance energy transfers, can significantly lower the activation barrier for N2 dissociation.
  • This plasmon-enhanced approach offers a promising pathway to overcome kinetic limitations in ammonia synthesis.
  • The findings demonstrate a strategy for utilizing light energy to facilitate challenging chemical transformations.