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Body-Centered-Cubic-Kernelled Ag15Cu6Nanocluster with Alkynyl Protection: Synthesis, Total Structure, and CO2Electroreduction

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Title
Body-Centered-Cubic-Kernelled Ag15Cu6Nanocluster with Alkynyl Protection: Synthesis, Total Structure, and CO2Electroreduction
Author(s)
Guocheng Deng; Jimin Kim; Megalamane S. Bootharaju; Sun, Fang; Kangjae Lee; Tang, Qing; Yun Jeong Hwang; Taeghwan Hyeon
Publication Date
2023-02
Journal
Journal of the American Chemical Society, v.145, no.6, pp.3401 - 3407
Publisher
American Chemical Society
Abstract
While atomically monodisperse nanostructured materials are highly desirable to unravel the size- and structure-catalysis relationships, their controlled synthesis and the atomic-level structure determination pose challenges. Particularly, copper-containing atomically precise alloy nanoclusters are potential catalyst candidates for the electrochemical CO2 reduction reaction (eCO2RR) due to high abundance and tunable catalytic activity of copper. Herein, we report the synthesis and total structure of an alkynyl-protected 21-atom AgCu alloy nanocluster [Ag15Cu6(CCR)18(DPPE)2]-, denoted as Ag15Cu6 (HCCR: 3,5-bis(trifluoromethyl)phenylacetylene; DPPE: 1,2-bis(diphenylphosphino)ethane). The single-crystal X-ray diffraction reveals that Ag15Cu6 consists of an Ag11Cu4 metal core exhibiting a body-centered cubic (bcc) structure, which is capped by 2 Cu atoms, 2 Ag2DPPE motifs, and 18 alkynyl ligands. Interestingly, the Ag15Cu6 cluster exhibits excellent catalytic activity for eCO2RR with a CO faradaic efficiency (FECO) of 91.3% at -0.81 V (vs the reversible hydrogen electrode, RHE), which is much higher than that (FECO: 48.5% at -0.89 V vs RHE) of Ag9Cu6 with bcc structure. Furthermore, Ag15Cu6 shows superior stability with no significant decay in the current density and FECO during a long-term operation of 145 h. Density functional theory calculations reveal that the de-ligated Ag15Cu6 cluster can expose more space at the pair of AgCu dual metals as the efficient active sites for CO formation. © 2022 American Chemical Society.
URI
https://pr.ibs.re.kr/handle/8788114/13142
DOI
10.1021/jacs.2c10338
ISSN
0002-7863
Appears in Collections:
Center for Nanoparticle Research(나노입자 연구단) > 1. Journal Papers (저널논문)
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