Tuning the selectivity of catalytic nitriles hydrogenation by structure regulation in atomically dispersed Pd catalysts

Zhibo Liu, Fei Huang, Mi Peng, Yunlei Chen, Xiangbin Cai, Linlin Wang, Zenan Hu, Xiaodong Wen, Ning Wang, Dequan Xiao, Hong Jiang, Hongbin Sun (), Hongyang Liu () and Ding Ma ()
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Zhibo Liu: Northeastern University
Fei Huang: Chinese Academy of Sciences
Mi Peng: Peking University
Yunlei Chen: Chinese Academy of Sciences
Xiangbin Cai: Hong Kong University of Science and Technology
Linlin Wang: Northeastern University
Zenan Hu: Northeastern University
Xiaodong Wen: Chinese Academy of Sciences
Ning Wang: Hong Kong University of Science and Technology
Dequan Xiao: University of New Haven
Hong Jiang: Peking University
Hongbin Sun: Northeastern University
Hongyang Liu: Chinese Academy of Sciences
Ding Ma: Peking University

Nature Communications, 2021, vol. 12, issue 1, 1-8

Abstract: Abstract The product selectivity in catalytic hydrogenation of nitriles is strongly correlated with the structure of the catalyst. In this work, two types of atomically dispersed Pd species stabilized on the defect-rich nanodiamond-graphene (ND@G) hybrid support: single Pd atoms (Pd1/ND@G) and fully exposed Pd clusters with average three Pd atoms (Pdn/ND@G), were fabricated. The two catalysts show distinct difference in the catalytic transfer hydrogenation of nitriles. The Pd1/ND@G catalyst preferentially generates secondary amines (Turnover frequency (TOF@333 K 709 h−1, selectivity >98%), while the Pdn/ND@G catalyst exhibits high selectivity towards primary amines (TOF@313 K 543 h−1, selectivity >98%) under mild reaction conditions. Detailed characterizations and density functional theory (DFT) calculations show that the structure of atomically dispersed Pd catalysts governs the dissociative adsorption pattern of H2 and also the hydrogenation pathway of the benzylideneimine (BI) intermediate, resulting in different product selectivity over Pd1/ND@G and Pdn/ND@G, respectively. The structure-performance relationship established over atomically dispersed Pd catalysts provides valuable insights for designing catalysts with tunable selectivity.

Date: 2021
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DOI: 10.1038/s41467-021-26542-y

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