Exploration of the Atomic Pathway of Seed-Mediated Growth from Icosahedral [Au25(SR)18]− to Bi-Icosahedral Au38(SR)24 and Au44(SR)26 Clusters Based on the 2e– Hopping Mechanism,Inorganic Chemistry

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Exploration of the Atomic Pathway of Seed-Mediated Growth from Icosahedral [Au25(SR)18]− to Bi-Icosahedral Au38(SR)24 and Au44(SR)26 Clusters Based on the 2e– Hopping Mechanism
Inorganic Chemistry ( IF 4.3 ) Pub Date : 2023-04-10 , DOI: 10.1021/acs.inorgchem.2c03997
Jiao Peng ₁ , Yong Pei ₁

Affiliation

Size growth is ubiquitous in the gold nanocluster synthesis. However, the atomic-level mechanism of seed-mediated growth of gold clusters remains mysterious. In this study, the seed-mediated growth pathway from the icosahedral [Au₂₅(SR)₁₈]⁻ cluster to the bi-icosahedral Au₃₈(SR)₂₄ and Au₄₄(SR)₂₆ clusters is studied based on the two-electron (2e^–) hopping mechanism. First, atomic structures of three key intermediate clusters, [Au₂₉(SR)₂₀]⁻, [Au₃₃(SR)₂₂]⁻, and Au₄₁(SR)₂₅, are predicted based on the 2e^–-unit decomposition strategy. The theoretically simulated UV–Vis spectra based on the predicted structure model of [Au₂₉(SR)₂₀]⁻ and [Au₃₃(SR)₂₂]⁻ matched well with the experimental curves reported previously. Based on the predicted intermediate cluster structures, the size growth pathway from the eight-electron (8e^–) [Au₂₅(SR)₁₈]⁻ cluster to 14-electron (14e^–) Au₃₈(SR)₂₄ and 18-electron (18e^–) Au₄₄(SR)₂₆ clusters is determined. In the step of formation of bi-icosahedral Au₃₈(SR)₂₄ from icosahedral [Au₂₅(SR)₁₈]⁻, two Au₄ units are first formed. The third 2e^– hopping step results in formation of an icosahedron unit. The present studies offered new insights into the formation and size conversion mechanism of ligand-protected gold nanoclusters containing icosahedral cores.

中文翻译：

基于 2e-跳跃机制探索种子介导的从二十面体 [Au25(SR)18]− 到双二十面体 Au38(SR)24 和 Au44(SR)26 簇生长的原子途径

尺寸增长在金纳米团簇合成中无处不在。然而，种子介导的金簇生长的原子级机制仍然是个谜。在这项研究中，基于双电子研究了从二十面体 [Au ₂₅ (SR) ₁₈ ] ⁻簇到双二十面体 Au ₃₈ (SR) ₂₄和 Au ₄₄ (SR) ₂₆簇的种子介导的生长途径(2 e ^– ) 跳跃机制。首先，三个关键中间簇的原子结构，[Au ₂₉ (SR) ₂₀ ] ^-、[Au ₃₃ (SR) ₂₂ ] ^-和 Au₄₁ (SR) ₂₅ , 是基于 2 e——^单元分解策略预测的。基于 [Au ₂₉ (SR) ₂₀ ] ⁻和 [Au ₃₃ (SR) ₂₂ ] ⁻预测结构模型的理论模拟 UV-Vis 光谱与先前报道的实验曲线非常吻合。基于预测的中间团簇结构，从八电子 (8 e ^– ) [Au ₂₅ (SR) ₁₈ ] ⁻团簇到 14 电子 (14 e ^– ) Au ₃₈ (SR) _{24的尺寸增长途径}和 18 电子 (18 e ^– ) Au ₄₄ (SR) ₂₆簇被确定。在从二十面体[Au ₂₅ (SR) ₁₈ ] ^{-形成双二十面体Au}₃₈ (SR) ₂₄的步骤中，首先形成两个Au _4单元。第三个 2 e ^-跳跃步骤导致二十面体单元的形成。目前的研究为含有二十面体核的配体保护金纳米团簇的形成和尺寸转换机制提供了新的见解。

更新日期：2023-04-10

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