AI Article Synopsis

  • C-N bond formation is crucial for creating nitrogen-containing compounds in chemistry, but traditional noble-metal catalysts are expensive and toxic.
  • Researchers developed a low-cost, low-toxicity iron complex catalyst (Fe-N /CNTs) that outperformed noble-metal catalysts, achieving yields up to 96% in synthesizing C-N bonds from aromatic amines and ketones.
  • The iron in the Fe-N /CNTs catalyst was well dispersed and identified as the active component; it also demonstrated potential for industrial use by maintaining its effectiveness over seven cycles.

Article Abstract

C-N bond formation is regarded as a very useful and fundamental reaction for the synthesis of nitrogen-containing molecules in both organic and pharmaceutical chemistry. Noble-metal and homogeneous catalysts have frequently been used for C-N bond formation, however, these catalysts have a number of disadvantages, such as high cost, toxicity, and low atom economy. In this work, a low-toxic and cheap iron complex (iron ethylene-1,2-diamine) has been loaded onto carbon nanotubes (CNTs) to prepare a heterogeneous single-atom catalyst (SAC) named Fe-N /CNTs. We employed this SAC in the synthesis of C-N bonds for the first time. It was found that Fe-N /CNTs is an efficient catalyst for the synthesis of C-N bonds starting from aromatic amines and ketones. Its catalytic performance was excellent, giving yields of up to 96 %, six-fold higher than the yields obtained with noble-metal catalysts, such as AuCl /CNTs and RhCl /CNTs. The catalyst showed efficacy in the reactions of thirteen aromatic amine substrates, without the need for additives, and seventeen enaminones were obtained. High-angle annular dark-field scanning transmission electron microscopy in combination with X-ray absorption spectroscopy revealed that the iron species were well dispersed in the Fe-N /CNTs catalyst as single atoms and that Fe-N might be the catalytic active species. This Fe-N /CNTs catalyst has potential industrial applications as it could be cycled seven times without any significant loss of activity.

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http://dx.doi.org/10.1002/chem.201905468DOI Listing

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