| 摘要： |
Aerobic oxidative cross-dehydrogenative coupling represents one of the most straightforward and atom-economic methods for construction of C-C and C-X (X = N, O, S, or P) bonds, especially when environmentally friendly air is used as the oxidant. Herein, we report the development of an inexpensive, stable, and highly dispersed ultrafine Ni2P nanoparticles with narrow size distribution supported on N,P-codoped biomass-derived porous carbon. The as-prepared catalyst is highly active and stable for the synthesis of pharmaceutically important N-heterocycles, including quinazolines, quinazolinones, and imidazoles, through oxidative cross-dehydrogenative coupling of a wide range of alcohols with diamines or 2-aminobenzamides using atmospheric air as the sole oxidant under mild reaction conditions. This work provides a new method to access N-heterocycles, which is operationally simple, widely applicable to various alcohols and diamines (or 2-aminobenzamides), and capable for gram-scale synthesis, highlighting its practical potential. Mechanistic studies reveal that the coupling proceeds in a cascade manner, with atmospheric air as a hydrogen acceptor that significantly boosts the overall reaction efficiency. |
