Issue 36, 2024

Atomically precise alkynyl-protected Ag19Cu2 nanoclusters: synthesis, structure analysis, and electrocatalytic CO2 reduction application

Abstract

We report the synthesis, structure analysis, and electrocatalytic CO2 reduction application of Ag19Cu2(C[triple bond, length as m-dash]CArF)12(PPh3)6Cl6 (abbreviated as Ag19Cu2, C[triple bond, length as m-dash]CArF: 3,5-bis(trifluoromethyl)phenylacetylene) nanoclusters. Ag19Cu2 has characteristic absorbance features and is a superatomic cluster with 2 free valence electrons. Single-crystal X-ray diffraction (SC-XRD) revealed that the metal core of Ag19Cu2 is composed of an Ag11Cu2 icosahedron connected by two Ag4 tetrahedra at the two terminals of the Cu–Ag–Cu axis. Notably, Ag19Cu2 exhibited excellent catalytic performance in the electrochemical CO2 reduction reaction (eCO2RR), manifested by a high CO faradaic efficiency of 95.26% and a large CO current density of 257.2 mA cm−2 at −1.3 V. In addition. Ag19Cu2 showed robust long-term stability, with no significant drop in current density and FECO after 14 h of continuous operation. Density functional theory (DFT) calculations disclosed that the high selectivity of Ag19Cu2 for CO in the eCO2RR process is due to the shedding of the –C[triple bond, length as m-dash]CArF ligand from the Ag atom at the very center of the Ag4 unit, exposing the active site. This study enriches the potpourri of alkynyl-protected bimetallic nanoclusters and also highlights the great advantages of using atomically precise metal nanoclusters to probe the atomic-level structure–performance relationship in the catalytic field.

Graphical abstract: Atomically precise alkynyl-protected Ag19Cu2 nanoclusters: synthesis, structure analysis, and electrocatalytic CO2 reduction application

Supplementary files

Article information

Article type
Paper
Submitted
29 6月 2024
Accepted
14 8月 2024
First published
15 8月 2024

Nanoscale, 2024,16, 16952-16957

Atomically precise alkynyl-protected Ag19Cu2 nanoclusters: synthesis, structure analysis, and electrocatalytic CO2 reduction application

X. Zhu, P. Zhu, X. Cong, G. Ma, Q. Tang, L. Wang and Z. Tang, Nanoscale, 2024, 16, 16952 DOI: 10.1039/D4NR02702G

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