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Quasi Pd1Ni single-atom surface alloy catalyst enables hydrogenation of nitriles to secondary amines
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Quasi Pd1Ni single-atom surface alloy catalyst enables hydrogenation of nitriles to secondary amines
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Quasi Pd1Ni single-atom surface alloy catalyst enables hydrogenation of nitriles to secondary amines
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Journal Article
Quasi Pd1Ni single-atom surface alloy catalyst enables hydrogenation of nitriles to secondary amines
2019
Overview
Hydrogenation of nitriles represents as an atom-economic route to synthesize amines, crucial building blocks in fine chemicals. However, high redox potentials of nitriles render this approach to produce a mixture of amines, imines and low-value hydrogenolysis byproducts in general. Here we show that quasi atomic-dispersion of Pd within the outermost layer of Ni nanoparticles to form a Pd
1
Ni single-atom surface alloy structure maximizes the Pd utilization and breaks the strong metal-selectivity relations in benzonitrile hydrogenation, by prompting the yield of dibenzylamine drastically from ∼5 to 97% under mild conditions (80 °C; 0.6 MPa), and boosting an activity to about eight and four times higher than Pd and Pt standard catalysts, respectively. More importantly, the undesired carcinogenic toluene by-product is completely prohibited, rendering its practical applications, especially in pharmaceutical industry. Such strategy can be extended to a broad scope of nitriles with high yields of secondary amines under mild conditions.
While nitrile hydrogenation may provide an appealing means to obtain secondary amines, poor selectivity plagues heterogeneous catalysts. Here, authors report single-atom palladium on nickel catalysts to afford high yields of secondary amines from a broad range of parent nitriles.
