Quasi Pd1Ni single-atom surface alloy catalyst enables hydrogenation of nitriles to secondary amines

Hengwei Wang, Qiquan Luo, Wei Liu, Yue Lin, Qiaoqiao Guan, Xusheng Zheng, Haibin Pan, Junfa Zhu, Zhihu Sun, Shiqiang Wei, Jinlong Yang and Junling Lu ()
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Hengwei Wang: Hefei National Laboratory for Physical Sciences at the Microscale, University of Science and Technology of China
Qiquan Luo: Hefei National Laboratory for Physical Sciences at the Microscale, University of Science and Technology of China
Wei Liu: National Synchrotron Radiation Laboratory, University of Science and Technology of China
Yue Lin: Hefei National Laboratory for Physical Sciences at the Microscale, University of Science and Technology of China
Qiaoqiao Guan: Hefei National Laboratory for Physical Sciences at the Microscale, University of Science and Technology of China
Xusheng Zheng: National Synchrotron Radiation Laboratory, University of Science and Technology of China
Haibin Pan: National Synchrotron Radiation Laboratory, University of Science and Technology of China
Junfa Zhu: National Synchrotron Radiation Laboratory, University of Science and Technology of China
Zhihu Sun: National Synchrotron Radiation Laboratory, University of Science and Technology of China
Shiqiang Wei: National Synchrotron Radiation Laboratory, University of Science and Technology of China
Jinlong Yang: Hefei National Laboratory for Physical Sciences at the Microscale, University of Science and Technology of China
Junling Lu: Hefei National Laboratory for Physical Sciences at the Microscale, University of Science and Technology of China

Nature Communications, 2019, vol. 10, issue 1, 1-9

Abstract: Abstract 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 Pd1Ni 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.

Date: 2019
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DOI: 10.1038/s41467-019-12993-x

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