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In situ immobilization of isolated Pd single-atoms on graphene by employing amino-functionalized rigid molecules and their prominent catalytic performance

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Abstract

Downsizing the costly noble metals to the single-atomic level has attracted extensive attention due to the maximum atom efficiency, low coordination, and sufficient exposure of isolated active metal centers. Herein, with a focus on the functionalization of the palladium phthalocyanines with four aminophenoxy groups at the periphery of the benzene ring (PdPc-TAP), we successfully anchored the isolated Pd single atoms onto graphene (Pd ISAs/GNS) via the in situ immobilization and pyrolysis of PdPc-TAP. The omni bearing imprisonment of the Pd sites (XY-axis stabilized by the planar macrocyclic Pc and Z-axis anchored from the interactions between the claw-like tetra-amino groups and GO) is the key factor for the formation of Pd ISAs/GNS. The model hydrogenation reaction and density functional theory calculation revealed that the demonstrated catalytic activity of Pd ISAs/GNS was 21.3 times higher than that of the Pd/C, which is attributed to the near-zero adsorption of active H* species on Pd ISAs/GNS that can accelerate the preferential migration of dissociative H* species to the target molecule. This work not only highlights the synthesis and application of the noble metal-based single-atom catalyst, but also provides a versatile strategy for the construction of single-atom catalysts from the viewpoint of substituent-modified rigid molecules.

Graphical abstract: In situ immobilization of isolated Pd single-atoms on graphene by employing amino-functionalized rigid molecules and their prominent catalytic performance

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Supplementary files

Article information


Submitted
20 Oct 2019
Accepted
21 Nov 2019
First published
21 Nov 2019

Catal. Sci. Technol., 2020, Advance Article
Article type
Paper

In situ immobilization of isolated Pd single-atoms on graphene by employing amino-functionalized rigid molecules and their prominent catalytic performance

Q. Liu, J. Wang, J. Zhang, Y. Yan, X. Qiu, S. Wei and Y. Tang, Catal. Sci. Technol., 2020, Advance Article , DOI: 10.1039/C9CY02110H

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