Development of high-performance heterogeneous catalytic materials is important for the rapid upgrade of chemicals, which remains a challenge. Here, the benzene oxidation reaction was used to demonstrate the effectiveness of the atomic interface strategy to improve catalytic performance. The developed B,N-cocoordinated Cu single atoms anchored on carbon nanosheets (Cu1/B-N) with the Cu-N2B1 atomic interface was prepared by the pyrolysis of a precoordinated Cu precursor. Benefiting from the unique atomic Cu-N2B1 interfacial structure, the designed Cu1/B-N exhibited considerable activity in the oxidation of benzene, which was much higher than Cu1/N-C, Cu NPs/N-C, and N-C catalysts. A theoretical study showed that the enhanced catalytic performance resulted from the optimized adsorption of intermediates, which originated from the manipulation of the electronic structure of Cu single atoms induced by B atom coordination in the Cu-N2B1 atomic interface. This study provides an innovative approach for the rational design of high-performance heterogeneous catalytic materials at the atomic level.
Keywords: atomic interface; benzene oxidation; catalytic performance; single-atom catalysts; theoretical simulations.