A Cobalt Sulfide-Based Amorphous/Crystalline Heterostructure with Enhanced Interface Charge Polarization for Efficient Hydrogenation of N-Heteroarenes

Constructing an amorphous/crystalline heterostructure to integrate the unique advantages of both amorphous and crystalline phases is an effective strategy for preparing high-performance catalysts. However, the exploration of such a heterogeneous catalyst for thermal catalysis is still in its infancy, especially for the hydrogenation of N-heteroarenes. In this study, a facile strategy was adopted to prepare a cobalt sulfide-based amorphous/crystalline heterostructure catalyst (named Co–S/NC). The catalyst Co–S/NC-800 with abundant amorphous/crystalline interfaces gave the best catalytic performance of more than 99% yield in the hydrogenation of quinoline to 1,2,3,4-tetrahydroquinoline. The experimental results suggested that Co–S/NC-800 possessed superior capacity for H2 dissociation and quinoline adsorption. The kinetic study verified that hydrogen dissociation was the rate-determining step. Besides, the theoretical study demonstrated that the amorphous/crystalline interface exhibited greater charge polarization than the crystalline surface, resulting in a superior quinoline adsorption and a lower energy barrier for H2 dissociation. This study revealed the relationship between the charge distribution at the amorphous/crystalline interface and its catalytic performance, bringing a new perspective on the application of amorphous/crystalline interfaces in catalytic hydrogenation reactions.