Enhanced efficiency and stability of Cs-modified Ni-based catalysts for selective synthesis of primary aminesPrimary amines are crucial building blocks in the synthesis of various pharmaceuticals, agrochemicals, and polymers. Reductive amination is a convenient way to construct primary amines from aldehydes and ketones. In this work, we report the novel Cs-modified Ni-Al hydrotalcite-derived catalysts that catalyze reductive amination with high activity and stability. An outstanding yield of benzylamine (98 %) is obtained under 50 °C, 1 MPa H2 within the reaction time of 3.5 min. Furthermore, a wide range of aldehydes and ketones are also converted into corresponding primary amines with promising yields (>90 %). Our study reveals that improved hydrogen activation favors the conversion of imine and dibenzylimine, while strong acidity leads to strong ammonia adsorption and slows the reaction rate. Cs modification enhances primary amine yields by adjusting the Ni0 particle size and increasing Ni0 electron density while reducing the strong acid sites. As a result, the Ni1Al2-Cs1.0 catalyst achieves superior performance and promising stability (>500 h) with a significantly reduced nickel content. |