4.8 Article

[AuAg26(SR)18S]- Nanocluster: Open Shell Structure and High Faradaic Efficiency in Electrochemical Reduction of CO2 to CO

Journal

JOURNAL OF PHYSICAL CHEMISTRY LETTERS
Volume 12, Issue 1, Pages 552-557

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acs.jpclett.0c03416

Keywords

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Funding

  1. National Natural Science Foundation of China [21601178, 21802141]
  2. Liaoning Provincial Natural Science Foundation of China [2019-MS-314]
  3. National Key R&D Program of China [2019YFC1905300]
  4. Projects of International Cooperation and Exchanges NSFC [21961142006]

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This study reports the open shell structure of [AuAg26(SR)(18)S](-) nanocluster and its excellent catalytic activity in the electrochemical reduction of CO2 to CO. The innovative open shell configuration of Ag-14(SR)(18)S in AuAg26 nanocluster plays a crucial role in forming intermediate COOH*, leading to a high Faradaic efficiency of 98.4% for CO generation at -0.97 V.
For atomically precise metal nanoclusters, distinctive molecular architectures and promising applications are urgently required to be intensively explored. Herein, we have first reported the open shell structure of the [AuAg26(SR)(18)S](-) nanocluster and its application in the electrochemical reduction of CO2. The X-ray crystal structure of the AuAg26 nanocluster is composed of a AuAg 12 icosahedron kernel and a Ag-14(SR)(18)S open shell. The shell includes a Ag-6(SR)(3)S, a Ag-5(SR)(6) , and three Ag(SR)(3) motifs. It is the first time twisty propeller-like Ag-5(SR)(6) and trefoil-like Ag-6(SR)(3)S motifs in metal nanoclusters have been observed. Due to the novel open shell configuration of Ag-14(SR)(18)S, four triangular facets of the kernel are exposed. The AuAg26 nanocluster shows excellent catalytic activity in the electrochemical reduction of CO2 to CO. The Faradaic efficiency of CO is up to 98.4% under -0.97 V. The electrochemical in situ infrared study and DFT calculations demonstrate that the open shell structure of the AuAg26 nanocluster is beneficial to the forming of intermediate COOH* in the electrochemical reduction of CO2 to CO.

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