Structure of the Au23-x Agx (S-Adm)15 Nanocluster and Its Application for Photocatalytic Degradation of Organic Pollutants

Chao Liu; Xiuqing Ren; Feng Lin; Xuemei Fu; Xinzhang Lin; Tao Li; Keju Sun; Jiahui Huang

doi:10.1002/anie.201904612

Structure of the Au_23-x Ag_x (S-Adm)₁₅ Nanocluster and Its Application for Photocatalytic Degradation of Organic Pollutants

Angew Chem Int Ed Engl. 2019 Aug 12;58(33):11335-11339. doi: 10.1002/anie.201904612. Epub 2019 Jul 3.

Authors

Chao Liu¹, Xiuqing Ren¹, Feng Lin^{1

2}, Xuemei Fu^{1

3}, Xinzhang Lin^{1

3}, Tao Li⁴, Keju Sun⁵, Jiahui Huang¹

Affiliations

¹ Gold Catalysis Research Center, State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, CAS, 457 Zhongshan Road, Dalian, 116023, China.
² Key Laboratory of New Energy and Rare Earth Resource Utilization, State Ethnic Affairs Commission, School of Physics and Materials Engineering, Dalian Minzu University, Dalian, 116600, China.
³ University of Chinese Academy Science, Beijing, 10049, China.
⁴ School of Physical Science and Technology, Shanghai Tech University, Shanghai, 201210, China.
⁵ College of Environmental and Chemical Engineering, Yanshan University, Qinhuangdao, 066004, China.

PMID: 31134723
DOI: 10.1002/anie.201904612

Abstract

Ligands play an important role in determining the atomic arrangement within the metal nanoclusters. Here, we report a new nanocluster [Au_23-x Ag_x (S-Adm)₁₅ ] protected by bulky adamantanethiol ligands which was obtained through a one-pot synthesis. The total structure of [Au_23-x Ag_x (S-Adm)₁₅ ] comprises an Au_13-x Ag_x icosahedral core, three Au₃ (SR)₄ units, and one AgS₃ staple motif in contrast to the 15-atom bipyramidal core previously seen in [Au_23-x Ag_x (SR)₁₆ ]. UV/Vis spectroscopy indicates that the HOMO-LUMO gap of [Au_23-x Ag_x (S-Adm)₁₅ ] is 1.5 eV. DFT calculations reveal that [Au₁₉ Ag₄ (S-Adm)₁₅ ] is the most stable structure among all structural possibilities. Benefitting from Ag doping, [Au_23-x Ag_x (S-Adm)₁₅ ] exhibits drastically improved photocatalytic activity for the degradation of rhodamine B (RhB) and phenol under visible-light irradiation compared to Au₂₃ nanoclusters.

Keywords: alloys; nanoclusters; photocatalysis; thiols.

Abstract

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