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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

Abstract

Downsizing the costly noble metals to 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 benzene ring (PdPc-TAP), we successfully anchor the isolated Pd single atoms on graphene (Pd ISAs/GNS) through in-suit immobilization and pyrolysis of PdPc-TAP. The omni bearing imprison of Pd sites (XY-axis stabilized by planar macrocyclic Pc and Z-axis anchored by the interaction between 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 reveals that the catalytic activity of Pd ISAs/GNS demonstrates 21.3 times higher than that of the Pd/C, which is attributed to the near-to-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 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.

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Publication details

The article was received on 20 Oct 2019, accepted on 21 Nov 2019 and first published on 21 Nov 2019


Article type: Paper
DOI: 10.1039/C9CY02110H
Catal. Sci. Technol., 2019, Accepted Manuscript

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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

    Q. Liu, J. Wang, J. Zhang, Y. Yan, X. Qiu, S. Wei and Y. Tang, Catal. Sci. Technol., 2019, Accepted Manuscript , DOI: 10.1039/C9CY02110H

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