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

Xinzhang Lin; Weiguang Ma; Keju Sun; Bo Sun; Xuemei Fu; Xiuqing Ren; Chao Liu; Jiahui Huang

doi:10.1021/acs.jpclett.0c03416

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

J Phys Chem Lett. 2021 Jan 14;12(1):552-557. doi: 10.1021/acs.jpclett.0c03416. Epub 2020 Dec 30.

Authors

Xinzhang Lin^{1

2}, Weiguang Ma^{1

3}, Keju Sun⁴, Bo Sun⁵, Xuemei Fu^{1

2}, Xiuqing Ren¹, Chao Liu¹, Jiahui Huang¹

Affiliations

¹ Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China.
² University of Chinese Academy Sciences, Beijing 100049, China.
³ State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China.
⁴ College of Environmental and Chemical Engineering, Yanshan University, Qinhuangdao 066004, China.
⁵ Shanghai Synchrotron Radiation Facility, Shanghai Advanced Research Institute, Chinese Academy of Sciences, Shanghai 201204, China.

PMID: 33378198
DOI: 10.1021/acs.jpclett.0c03416

Abstract

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(S-Adm)₁₈S]^- nanocluster and its application in the electrochemical reduction of CO₂. The X-ray crystal structure of the AuAg₂₆ nanocluster is composed of a AuAg₁₂ icosahedron kernel and a Ag₁₄(SR)₁₈S open shell. The shell includes a Ag₆(SR)₃S, a Ag₅(SR)₆, and three Ag(SR)₃ motifs. It is the first time twisty propeller-like Ag₅(SR)₆ and trefoil-like Ag₆(SR)₃S motifs in metal nanoclusters have been observed. Due to the novel open shell configuration of Ag₁₄(SR)₁₈S, 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.