Issue 7, 2023

Pyridyl-containing graphdiyne stabilizes sub-2 nm ultrasmall copper nanoclusters for the electrochemical reduction of CO2

Abstract

Developing novel carbonaceous materials with definite chemical structures is conducive to understanding structure–property relationships and expanding their applications in supported metal catalysts. Herein, a brand-new pyridine-substituted graphdiyne (Py-GDY) is synthesized through the cross-coupling of 1,3,5-triethynyl-2,4,6-tris(4-pyridyl)benzene, and further applied as a promising carrier in electrocatalysis. Thanks to the precisely introduced pyridyl groups, strong metal–support interaction between the confined Cu species and Py-GDY is desirably obtained, resulting in uniformly dispersed Cu sub-nanoclusters (<2 nm) (Py-GDY-Cu). Conversely, the Cu size increased dramatically when the pyridyl group of Py-GDY was replaced by the phenyl group (Ph-GDY-Cu). In a proof-of-concept demonstration of the electrochemical CO2 reduction reaction, Py-GDY-Cu is found to produce CH4 preferentially to Ph-GDY-Cu, owing to the favorable sub-nanocluster size. As a result, an optimum CH4 faradaic efficiency of 58% is achieved on Py-GDY-Cu, which shows a 1.6-fold enhancement compared with that of Ph-GDY-Cu. This work broadens the scope of carbonaceous materials for rational metal species immobilization toward efficient catalysis.

Graphical abstract: Pyridyl-containing graphdiyne stabilizes sub-2 nm ultrasmall copper nanoclusters for the electrochemical reduction of CO2

Supplementary files

Article information

Article type
Research Article
Submitted
15 dec 2022
Accepted
04 mar 2023
First published
06 mar 2023

Inorg. Chem. Front., 2023,10, 2189-2196

Pyridyl-containing graphdiyne stabilizes sub-2 nm ultrasmall copper nanoclusters for the electrochemical reduction of CO2

H. Dai, H. Zou, T. Song, L. Gao, S. Wei, H. Liu, H. Xiong, C. Huang and L. Duan, Inorg. Chem. Front., 2023, 10, 2189 DOI: 10.1039/D2QI02671F

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