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

Liu, QC (Liu, Qicheng)[ 1 ] ; Wang, JC (Wang, Jingchun)[ 1 ] ; Zhang, JZ (Zhang, Jingzi)[ 1 ] ; Yan, YW (Yan, Yawei)[ 1 ] ; Qiu, XY (Qiu, Xiaoyu)[ 1 ]*（邱晓雨）; Wei, SH (Wei, Shaohua)[ 1,2 ] ; Tang, YW (Tang, Yawen)[ 1 ]*（唐亚文）

[ 1 ] Nanjing Normal Univ, Sch Chem & Mat Sci, Nanjing 210023, Peoples R China

[ 2 ] Yancheng Inst Technol, Yancheng 224007, Peoples R China

CATALYSIS SCIENCE & TECHNOLOGY，202001,10(2),450-457

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.

文章链接：

https://pubs.rsc.org/en/content/articlelanding/2020/CY/C9CY02110H#!divAbstract

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