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Magic-Number Gold Nanoclusters with Diameters from 1 to 3.5 nm: Relative Stability and Catalytic Activity for CO Oxidation

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    Magic-Number Gold Nanoclusters with Diameters from 1 to 3.5 nm: Relative Stability and Catalytic Activity for CO Oxidation
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    † Institute of Physics, Chinese Academy of Sciences, Beijing 100190, People’s Republic of China
    ‡ Department of Chemistry and Nebraska Center for Materials and Nanoscience, University of Nebraska—Lincoln, Lincoln, Nebraska 68588, United States
    § Science Institute of University of Iceland, 101 Reykjavík, Iceland
    ∥ Shanghai Institute of Applied Physics, Chinese Academy of Sciences, Shanghai 201800, People’s Republic of China
    ⊥ Department of Applied Physics, Aalto University, 02150 Espoo, Finland
    *E-mail: [email protected]
    *E-mail: [email protected]
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    Nano Letters

    Cite this: Nano Lett. 2015, 15, 1, 682–688
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    https://doi.org/10.1021/nl504192u
    Published December 10, 2014
    Copyright © 2014 American Chemical Society
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    Abstract

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    Relative stability of geometric magic-number gold nanoclusters with high point-group symmetry (Ih, D5h, Oh) and size up to 3.5 nm, as well as structures obtained by global optimization using an empirical potential, is investigated using density functional theory (DFT) calculations. Among high-symmetry nanoclusters, our calculations suggest that from Au(147) to Au(923), the stability follows the order Ih > D5h > Oh. However, at the largest size of Au(923), the computed cohesive energy differences among high-symmetry Ih, D5h and Oh isomers are less than 4 meV/atom (at PBE level of theory), suggesting the larger high-symmetry clusters are similar in stability. This conclusion supports a recent experimental demonstration of controlling morphologies of high-symmetry Au(923) clusters (Plant, S. R.; Cao, L.; Palmer, R. E. J. Am. Chem. Soc. 2014, 136, 7559). Moreover, at and beyond the size of Au(549), the face-centered cubic-(FCC)-based structure appears to be slightly more stable than the Ih structure with comparable size, consistent with experimental observations. Also, for the Au clusters with the size below or near Au(561), reconstructed icosahedral and decahedral clusters with lower symmetry are slightly more stable than the corresponding high-symmetry isomers. Catalytic activities of both high-symmetry and reconstructed Ih-Au(147) and both Ih-Au(309) clusters are examined. CO adsorption on Au(309) exhibits less sensitivity on the edge and vertex sites compared to Au(147), whereas the CO/O2 coadsorption is still energetically favorable on both gold nanoclusters. Computed activation barriers for CO oxidation are typically around 0.2 eV, suggesting that the gold nanoclusters of ∼2 nm in size are highly effective catalysts for CO oxidation.

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    Cite this: Nano Lett. 2015, 15, 1, 682–688
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    Published December 10, 2014
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