Synergistic Nanoscale Mn3O4‐CoO‐Co Heterojunctions for Boosting the Selectivity in Hydrogenation of Nitrostyrenes and Nitroarenes

Metal–metal oxide interface catalysts are in high demand for advanced catalytic applications due to their multi‐component active sites, which facilitate synergistic cooperation where a single component alone cannot effectively promote the desired reaction. Demonstrated herein graphene oxide‐supported nanoscale Mn3O4‐CoO‐Co as highly efficient catalysts for hydrogenation of nitro styrenes/nitro arenes to amino styrenes/arenes under mild reaction conditions (0.5 MPa and 100 °C in 1:1 THF/water). Charge relocalization at the Co‐CoO‐Mn3O4 heterojunction interfaces, primarily driven by Mn3O4, significantly improves reaction selectivity. Replacing Mn3O4 with MnO or using other supported bimetallic CoMnOx catalysts decreases selectivity, leading to the formation of a mixture of products. The catalyst demonstrated remarkable selectivity in converting nitro groups to amines, even in the presence of highly reactive functional groups such as C=C, O‐C=O, C=O, C≡N, chalcones, and halides. It also exhibited high yields, multiple reusability, and a broad substrate scope. This study demonstrates how Mn3O4, in synergy with CoO‐Co, fine‐tunes selectivity, paving the way for the development of advanced metal‐metal oxide interface catalysts to enhance both selectivity and efficiency in organic transformations.