Single atom catalysts for electrocatalytic C–N coupling: From dynamic mechanism to rational design

Résumé fourni par la source

Electrocatalysis for C−N coupling reactions (EcnRR) plays a crucial role in the synthesis of various organic molecules. However, the C−N coupling process is inherently complex and kinetically sluggish. Single-atom catalysts (SACs), with their high atomic efficiency, tunable structures, and remarkable catalytic activity, exhibit exceptional performance and hold great promise for C−N coupling reactions. The design of SACs requires a deep understanding of the reaction mechanisms, particularly the dynamic evolution of multi-component reactions. This necessitates systematic studies of multi-species coupling mechanisms to move beyond traditional trial-and-error approaches. This review elucidates the activation mechanisms of carbon- and nitrogen-containing molecules, providing fundamental insights into the SACs-mediated electrocatalytic C−N coupling process. Notably, the core focus lies in proposing novel design principles for SACs systems tailored for C−N coupling, based on theoretical frameworks and experimental findings. These insights not only guide the improvement of existing methodologies but also offer transformative pathways for electrocatalytic organic nitrogenation via C−N coupling chemistry, potentially reshaping the landscape of organic synthesis. Looking ahead, a comprehensive understanding of the structure–activity relationships in SAC design will be key to advancing this rapidly evolving field.

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