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<p>The transformation of well-characterized, ligand-protected gold nanoclusters (AuNCs) is a promising approach for the targeted synthesis of novel AuNCs. Our group has previously reported that [MAu<sub>8</sub>(PPh<sub>3</sub>)<sub>8</sub>]<sup>2+</sup> (M&#xa0;=&#xa0;Au<sup>+</sup>, Pd) in methanol was transformed into unprecedented NCs by incorporating one or two AuCN units through atmospheric pressure plasma (APP) irradiation. In order to broaden the scope of the APP-based transformation, the reaction on a prototypical thiolate-protected AuNCs [Au<sub>25</sub>(SR)<sub>18</sub>]<sup>–</sup> was studied. APP irradiation of [Au<sub>25</sub>(4-PyET)<sub>18</sub>]<sup>–</sup> (4-PyET&#xa0;=&#xa0;4-pyridineethanethiol) resulted in a transformation to [Au<sub>20</sub>(4-PyET)<sub>14</sub>CN]<sup>–</sup>, accompanied by oxidation, while [Au<sub>25</sub>(<i>p</i>-MBA)<sub>18</sub>]<sup>–</sup> (<i>p</i>-MBA&#xa0;=&#xa0;4-mercaptobenzoic acid) was transformed into larger plasmonic Au nanoparticles. The geometric and electronic structures of a simplified model [Au<sub>20</sub>(SCH<sub>3</sub>)<sub>14</sub>CN]<sup>–</sup> were investigated by density functional theory (DFT) calculations. It was proposed that [Au<sub>20</sub>(SCH<sub>3</sub>)<sub>14</sub>CN]<sup>–</sup> has an oblate Au<sub>10</sub> superatomic core protected by two Au<sub>2</sub>(4-PyET)<sub>3</sub> and two Au<sub>3</sub>(4-PyET)<sub>4</sub> oligomers.</p>

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Transformation of [Au25(4-PyET)18]– into [Au20(4-PyET)14CN]– Induced by Atmospheric Pressure Plasma Irradiation in Methanol

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  • 发表日期：

    2025年6月14日

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  • Lewei Wang,
  • Kiichirou Koyasu,
  • Tatsuya Tsukuda

摘要

The transformation of well-characterized, ligand-protected gold nanoclusters (AuNCs) is a promising approach for the targeted synthesis of novel AuNCs. Our group has previously reported that [MAu8(PPh3)8]2+ (M = Au+, Pd) in methanol was transformed into unprecedented NCs by incorporating one or two AuCN units through atmospheric pressure plasma (APP) irradiation. In order to broaden the scope of the APP-based transformation, the reaction on a prototypical thiolate-protected AuNCs [Au25(SR)18]– was studied. APP irradiation of [Au25(4-PyET)18]– (4-PyET = 4-pyridineethanethiol) resulted in a transformation to [Au20(4-PyET)14CN]–, accompanied by oxidation, while [Au25(p-MBA)18]– (p-MBA = 4-mercaptobenzoic acid) was transformed into larger plasmonic Au nanoparticles. The geometric and electronic structures of a simplified model [Au20(SCH3)14CN]– were investigated by density functional theory (DFT) calculations. It was proposed that [Au20(SCH3)14CN]– has an oblate Au10 superatomic core protected by two Au2(4-PyET)3 and two Au3(4-PyET)4 oligomers.