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

Dai，Hao1; Zou，Haiyuan1; Song，Tao1; Gao，Lei2; Wei，Shuting1; Liu，Hong1; Xiong，Huatian1; Huang，Changshui3; Duan，Lele1

2023-03-06

10.1039/d2qi02671f

Inorganic Chemistry Frontiers   影响因子和分区

2052-1553

2052-1553

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 CO reduction reaction, Py-GDY-Cu is found to produce CH preferentially to Ph-GDY-Cu, owing to the favorable sub-nanocluster size. As a result, an optimum CH 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.

SCI ; EI

英语

第一 ; 通讯

National Natural Science Foundation of China[22179057];

Chemistry

Chemistry, Inorganic & Nuclear

WOS:000949492700001

ROYAL SOC CHEMISTRY

20231313813190

Catalysts ; Copper ; Electrocatalysis ; Electrolytic reduction ; Nanoclusters ; Synthesis (chemical)

Ore Treatment:533.1 ; Copper:544.1 ; Nanotechnology:761 ; Electrochemistry:801.4.1 ; Chemical Reactions:802.2 ; Chemical Agents and Basic Industrial Chemicals:803 ; Chemical Products Generally:804 ; Inorganic Compounds:804.2 ; Solid State Physics:933

2-s2.0-85151035361

Scopus

1.Department of Chemistry and Shenzhen Grubbs Institute,Southern University of Science and Technology,Shenzhen,518055,China
2.National Laboratory of Solid State Microstructures (NLSSM),Jiangsu Key Laboratory of Artificial Functional Materials,College of Engineering and Applied Sciences,Nanjing University,Nanjing,210093,China
3.Beijing National Laboratory for Molecular Sciences,Organic Solids Laboratory,Institute of Chemistry,Chinese Academy of Sciences,Beijing,100190,China

Dai，Hao,Zou，Haiyuan,Song，Tao,et al. Pyridyl-containing graphdiyne stabilizes sub-2 nm ultrasmall copper nanoclusters for the electrochemical reduction of CO2[J]. Inorganic Chemistry Frontiers,2023,10(7):2189-2196.

Dai，Hao.,Zou，Haiyuan.,Song，Tao.,Gao，Lei.,Wei，Shuting.,...&Duan，Lele.(2023).Pyridyl-containing graphdiyne stabilizes sub-2 nm ultrasmall copper nanoclusters for the electrochemical reduction of CO2.Inorganic Chemistry Frontiers,10(7),2189-2196.

Dai，Hao,et al."Pyridyl-containing graphdiyne stabilizes sub-2 nm ultrasmall copper nanoclusters for the electrochemical reduction of CO2".Inorganic Chemistry Frontiers 10.7(2023):2189-2196.