Highly Efficient Selective Hydrogenation of Nitriles on Non-Noble Metal Catalysts at Low Temperatures

Highly efficient selective hydrogenation at low temperature is of significance for energy efficiency and cost-effectiveness. Herein, we describe a strategy of target reaction pathway reinforcement by metal-acid dual site construction through a hydrothermal nanocrystal carbon (NCC) templating method to enable high activity of non-noble metal catalysts at low temperatures in selective hydrogenation. In a typical selective hydrogenation of benzonitrile to a primary amine, the prepared catalyst NiAl-Zr-NCC successfully achieves complete conversion and high yield of benzylamine at 98% at a low temperature of 50 °C, which is reported as the lowest reaction temperature on a non-noble metal catalyst with a satisfactory benzylamine yield above 95%. Experimental and characterization results suggest that the strengthened hydrogen activation ability is responsible for a significantly promoted hydrogenation pathway to benzylamine, while well-matched acid/Ni−H dual sites inhibit the side reaction pathway to form byproducts of secondary amines by weakening the activation of intermediate secondary imines. This work provides a rational design conception of a highly efficient selective-hydrogenation catalyst for the energy-efficient chemistry industry.