Decreasing the coordinated N atoms in a single-atom Cu catalyst to achieve selective transfer hydrogenation of alkynes†
Single-atom (SA) catalysts have attracted broad attention due to their distinctive catalytic properties in diverse reactions. Increasing the unsaturated coordination sites of active centers is a valid and challenging approach to improve the performance of such catalysts. Herein, we report an oxide compounding strategy to decrease the N coordination number of a SA Cu catalyst by reducing the thickness of the N-doped carbon carrier with a lower density of N atoms. The SA Cu catalyst with a more unsaturated N coordination structure can achieve transfer hydrogenation of alkynes with good activity and selectivity, which is disabled over the common N coordinated SA Cu catalyst on pure CN. It is found that individual Cu centers coordinated by fewer N atoms can accelerate the hydrogen transfer from ammonia–borane and still leave proper adsorption sites for alkynes to realize the entire hydrogenation reaction. This work will open up new opportunities to modulate the unsaturated coordination structure of SA catalysts for creating better-performing heterogeneous catalysts.