Pt Single Atoms Embedded in the Surface of Ni Nanocrystals
as Highly Active Catalysts for Selective Hydrogenation of Nitro Compounds
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Abstract
Single-atom
catalysts exhibit high selectivity in hydrogenation
due to their isolated active sites, which ensure uniform adsorption
configurations of substrate molecules. Compared with the achievement
in catalytic selectivity, there is still a long way to go in exploiting
the catalytic activity of single-atom catalysts. Herein, we developed
highly active and selective catalysts in selective hydrogenation by
embedding Pt single atoms in the surface of Ni nanocrystals (denoted
as Pt<sub>1</sub>/Ni nanocrystals). During the hydrogenation of 3-nitrostyrene,
the TOF numbers based on surface Pt atoms of Pt<sub>1</sub>/Ni nanocrystals
reached ∼1800 h<sup>–1</sup> under 3 atm of H<sub>2</sub> at 40 °C, much higher than that of Pt single atoms supported
on active carbon, TiO<sub>2</sub>, SiO<sub>2</sub>, and ZSM-5. Mechanistic
studies reveal that the remarkable activity of Pt<sub>1</sub>/Ni nanocrystals
derived from sufficient hydrogen supply because of spontaneous dissociation
of H<sub>2</sub> on both Pt and Ni atoms as well as facile diffusion
of H atoms on Pt<sub>1</sub>/Ni nanocrystals. Moreover, the ensemble
composed of the Pt single atom and nearby Ni atoms in Pt<sub>1</sub>/Ni nanocrystals leads to the adsorption configuration of 3-nitrostyrene
favorable for the activation of nitro groups, accounting for the high
selectivity for 3-vinylaniline