AI Article Synopsis

  • - The study presents a new method for efficiently performing cross-coupling reactions using dehydrogenative routes with solid atomic catalysts, which could make the process more economical and sustainable.
  • - Researchers developed Cu-M dual-atom catalysts (using metals like Co, Ni, Cu, and Zn) on hierarchical USY zeolite, achieving over 80% yields with the Cu-Co variant, showcasing its superior reactivity.
  • - The improved effectiveness of the Cu-Co catalyst is due to its specially designed active sites that facilitate substrate co-adsorption and activation, and the efficient movement of organic substrates within the catalyst’s structure.

Article Abstract

A cross-coupling reaction via the dehydrogenative route over heterogeneous solid atomic catalysts offers practical solutions toward an economical and sustainable elaboration of simple organic substrates. The current utilization of this technology is, however, hampered by limited molecular definition of many solid catalysts. Here, we report the development of Cu-M dual-atom catalysts (where M = Co, Ni, Cu, and Zn) supported on a hierarchical USY zeolite to mediate efficient dehydrogenative cross-coupling of unprotected phenols with amine partners. Over 80% isolated yields have been attained over Cu-Co-USY, which shows much superior reactivity when compared with our Cu and other Cu-M analogues. This amination reaction has hence involved simple and non-forceful reaction condition requirements. The superior reactivity can be attributed to (1) the specifically designed bimetallic Cu-Co active sites within the micropore for "co-adsorption-co-activation" of the reaction substrates and (2) the facile intracrystalline (meso/micropore) diffusion of the heterocyclic organic substrates. This study offers critical insights into the engineering of next-generation solid atomic catalysts with complex reaction steps.

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http://dx.doi.org/10.1021/jacs.3c00114DOI Listing

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