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    Reversible Size Control of Silver Nanoclusters via Ligand-exchange

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    Type
    Article
    Authors
    Bootharaju, Megalamane Siddaramappa cc
    Burlakov, Victor M.
    Besong, Tabot M.D. cc
    Joshi, Chakra Prasad
    Reshi, Owais A. cc
    Black, David
    Whetten, Robert
    Goriely, Alain cc
    Bakr, Osman cc
    KAUST Department
    Functional Nanomaterials Lab (FuNL)
    KAUST Catalysis Center (KCC)
    KAUST Solar Center (KSC)
    Material Science and Engineering Program
    Physical Science and Engineering (PSE) Division
    Date
    2015-06-05
    Online Publication Date
    2015-06-05
    Print Publication Date
    2015-06-23
    Permanent link to this record
    http://hdl.handle.net/10754/555643
    
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    Abstract
    The properties of atomically monodisperse noble metal nanoclusters (NCs) are intricately intertwined with their precise molecular formula. The vast majority of size-specific NC syntheses start from the reduction of the metal salt and thiol ligand mixture. Only in gold was it recently shown that ligand-exchange could induce the growth of NCs from one atomically precise species to another; a process of yet unknown reversibility. Here, we present a process for the ligand-exchange-induced growth of atomically precise silver NCs, in a biphasic liquid-liquid system, which is particularly of interest because of its complete reversibility and ability to occur at room temperature. We explore this phenomenon in-depth using Ag35(SG)18 [SG= glutathionate] and Ag44(4-FTP)30 [4-FTP= 4-fluorothiophenol] as model systems. We show that the ligand-exchange conversion of Ag35(SG)18 into Ag44(4-FTP)30 is rapid (< 5 min) and direct, while the reverse process proceeds slowly through intermediate cluster sizes. We adapt a recently developed theory of reverse Ostwald ripening to model the NCs’ interconvertibility. The model’s predictions are in good agreement with the experimental observations, and they highlight the importance of small changes in the ligand-metal binding energy in determining the final equilibrium NC size. Based on the insight provided by this model, we demonstrated experimentally that by varying the choice of ligands, ligand-exchange can be used to obtain different sized NCs. The findings in this work establish ligand-exchange as a versatile tool for tuning cluster sizes.
    Citation
    Reversible Size Control of Silver Nanoclusters via Ligand-exchange 2015:150521100629001 Chemistry of Materials
    Publisher
    American Chemical Society (ACS)
    Journal
    Chemistry of Materials
    DOI
    10.1021/acs.chemmater.5b00650
    Additional Links
    http://pubs.acs.org/doi/abs/10.1021/acs.chemmater.5b00650
    ae974a485f413a2113503eed53cd6c53
    10.1021/acs.chemmater.5b00650
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