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Au36(SPh)24 Nanomolecules: X-ray Crystal Structure, Optical Spectroscopy, Electrochemistry, and Theoretical Analysis

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    Au36(SPh)24 Nanomolecules: X-ray Crystal Structure, Optical Spectroscopy, Electrochemistry, and Theoretical Analysis
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    † Department of Chemistry and Biochemistry, University of Mississippi, Oxford, Mississippi 38677, United States
    ‡ Molecular Imaging and Photonics, Department of Chemistry, KU Leuven, Celestijnenlaan 200D, 3001 Heverlee, Belgium
    § Department of Chemistry, Kansas State University, Manhattan, Kansas 66506, United States
    *E-mail: [email protected]
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    The Journal of Physical Chemistry B

    Cite this: J. Phys. Chem. B 2014, 118, 49, 14157–14167
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    https://doi.org/10.1021/jp506508x
    Published October 15, 2014
    Copyright © 2014 American Chemical Society
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    Abstract

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    The physicochemical properties of gold:thiolate nanomolecules depend on their crystal structure and the capping ligands. The effects of protecting ligands on the crystal structure of the nanomolecules are of high interest in this area of research. Here we report the crystal structure of an all aromatic thiophenolate-capped Au36(SPh)24 nanomolecule, which has a face-centered cubic (fcc) core similar to other nanomolecules such as Au36(SPh-tBu)24 and Au36(SC5H9)24 with the same number of gold atoms and ligands. The results support the idea that a stable core remains intact even when the capping ligand is varied. We also correct our earlier assignment of “Au36(SPh)23” which was determined based on MALDI mass spectrometry which is more prone to fragmentation than ESI mass spectrometry. We show that ESI mass spectrometry gives the correct assignment of Au36(SPh)24, supporting the X-ray crystal structure. The electronic structure of the title compound was computed at different levels of theory (PBE, LDA, and LB94) using the coordinates extracted from the single crystal X-ray diffraction data. The optical and electrochemical properties were determined from experimental data using UV–vis spectroscopy, cyclic voltammetry, and differential pulse voltammetry. Au36(SPh)24 shows a broad electrochemical gap near 2 V, a desirable optical gap of ∼1.75 eV for dye-sensitized solar cell applications, as well as appropriately positioned electrochemical potentials for many electrocatalytic reactions.

    Copyright © 2014 American Chemical Society

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    Kohn–Sham orbitals and orbitals energies, the crystal structure data, and the cif file. CCDC number is 996171. This material is available free of charge via the Internet at http://pubs.acs.org.

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    Cite this: J. Phys. Chem. B 2014, 118, 49, 14157–14167
    Click to copy citationCitation copied!
    https://doi.org/10.1021/jp506508x
    Published October 15, 2014
    Copyright © 2014 American Chemical Society
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