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Copper Doping Boosts Electrocatalytic CO2 Reduction of Atomically Precise Gold Nanoclusters

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Title
Copper Doping Boosts Electrocatalytic CO2 Reduction of Atomically Precise Gold Nanoclusters
Author(s)
Guocheng Deng; Hyewon Yun; Megalamane S. Bootharaju; Sun, Fang; Kangjae Lee; Xiaolin Liu; Seungwoo Yoo; Tang, Qing; Yun Jeong Hwang; Taeghwan Hyeon
Publication Date
2023-12
Journal
Journal of the American Chemical Society, v.145, no.50, pp.27407 - 27414
Publisher
American Chemical Society
Abstract
Unraveling the atomistic synergistic effects of nanoalloys on the electrocatalytic CO2 reduction reaction (eCO2RR), especially in the presence of copper, is of paramount importance. However, this endeavor encounters significant challenges due to the lack of the crystallographically determined atomic-level structure of appropriate monometallic and bimetallic analogues. Herein, we report a one-pot synthesis and structure characterization of a AuCu nanoalloy cluster catalyst, [Au15Cu4(DPPM)6Cl4(C≡CR)1]2+ (denoted as Au15Cu4). Single-crystal X-ray diffraction analysis reveals that Au15Cu4 comprises two interpenetrating incomplete, centered icosahedra (Au9Cu2 and Au8Cu3) and is protected by six DPPM, four halide, and one alkynyl ligand. The Au15Cu4 cluster and its closest monometal structural analogue, [Au18(DPPM)6Br4]2+ (denoted as Au18), as model systems, enable the elucidation of the atomistic synergistic effects of Au and Cu on eCO2RR. The results reveal that Au15Cu4 is an excellent eCO2RR catalyst in a gas diffusion electrode-based membrane electrode assembly (MEA) cell, exhibiting a high CO Faradaic efficiency (FECO) of >90%, and this efficiency is substantially higher than that of the undoped Au18 (FECO: 60% at −3.75 V). Au15Cu4 exhibits an industrial-level CO partial current density of up to −413 mA/cm2 at −3.75 V with the gas CO2-fed MEA, which is 2-fold higher than that of Au18. The density functional theory (DFT) calculations demonstrate that the synergistic effects are induced by Cu doping, where the exposed pair of AuCu dual sites was suggested for launching the eCO2RR process. Besides, DFT simulations reveal that these special dual sites synergistically coordinate a moderate shift in the d-state, thus enhancing its overall catalytic performance. © 2023 American Chemical Society.
URI
https://pr.ibs.re.kr/handle/8788114/14512
DOI
10.1021/jacs.3c08438
ISSN
0002-7863
Appears in Collections:
Center for Nanoparticle Research(나노입자 연구단) > 1. Journal Papers (저널논문)
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