Spatial intimacy of binary active-sites for selective sequential hydrogenation-condensation of nitriles into secondary imines

Sai Zhang, Zhaoming Xia, Yong Zou, Mingkai Zhang and Yongquan Qu ()
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Sai Zhang: Northwestern Polytechnical University
Zhaoming Xia: Xi’an Jiaotong University
Yong Zou: Xi’an Jiaotong University
Mingkai Zhang: Xi’an Jiaotong University
Yongquan Qu: Northwestern Polytechnical University

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

Abstract: Abstract Precisely controlling the spatial intimacy of multiple active sites at sub-nanoscale in heterogeneous catalysts can improve their selectivity and activity. Herein, we realize a highly selective nitrile-to-secondary imine transformation through a cascaded hydrogenation and condensation process by Pt1/CoBOx comprising the binary active sites of the single-dispersed Pt and interfacial Lewis acidic B. Atomic Pt sites with large inter-distances (>nanometers) only activate hydrogen for nitrile hydrogenation, but inhibit condensation. Both adjacent B…B on CoBOx and neighbouring Pt…B pairs with close intimacy of ~0.45 nm can satisfy the spatial prerequisites for condensation. Mechanism investigations demonstrate the energetically favorable pathway occurred on adjacent Lewis acidic B sites through the nitrile adsorption (acid-base interaction), hydrogenation via hydrogen spillover from Pt to B sites and sequential condensation. Strong intermolecular tension and steric hindrance of secondary imines on active sites lead to their effective desorption and thereby a high chemoselectivity of secondary imines.

Date: 2021
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DOI: 10.1038/s41467-021-23705-9

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