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Mechanistic exploration and controlled synthesis of precise thiolate-gold nanoclusters

机译：精确硫醇盐-金纳米团簇的机理探索与受控合成

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摘要

Well-defined thiolate-gold nanoclusters (generally described as Au-n(SR)(m), NCs, where "n" and "m" are the numbers of gold atoms and thiolate ligands ( SR), respectively), comprise a family of ultrasmall particles (<2 nm), which are distinctly different from their large counterparts, plasmonic gold nanoparticles (NPs, >2 nm). They are attracting increasing attention in various areas, including biomedicine, optoelectronics, catalysis, and analytical science, mainly because of their unique molecular-like properties, such as HOMO-LUMO (highest occupied and lowest unoccupied molecular orbital) transitions, quantized charging, and photoluminescence. All of these physicochemical properties are highly sensitive to the size and composition of Au NCs, and thus the ability to control these variables during synthesis is highly important. This review describes recent advances in the precise control of these features during Au NC synthesis, typically via the reduction of Au(I)-SR complexes. First, the formation mechanisms for atomically precise Au-n(SR)(m) NCs are explained, which may be decoupled into two stages: 1) generation of intermediate NCs via the reduction of Au(I)-SR complexes (reduction-assisted growth stage), and 2) size evolution of intermediate NCs to form Au NC species with atomic precision (size evolution stage). The size/composition control strategies implemented in the reduction-assisted growth stage are summarized based on this reduction-size evolution mechanism. Details are then given of the regulation strategies with effects in the size evolution stage. Finally, it is shown that balancing the rate of reduction and size evolution may be a unified approach for the facile synthesis (large-scale production, easy preparation, and short reaction time) of Au-n(SR)(m) NCs with high control over their size and composition. This concept may facilitate the design and development of large-scale methods for synthesizing stable well-defined Au NCs with advanced functions for use in a wide range of applications in different domains. (C) 2016 Elsevier B.V. All rights reserved.
机译：定义明确的硫醇盐-金纳米簇（通常称为Au-n（SR）（m），NC，其中“ n”和“ m”分别是金原子数和硫醇盐配体（SR）的数目）组成一个家族超细颗粒（<2 nm）与等离子金纳米颗粒（NPs，> 2 nm）明显不同。它们在生物医学，光电子学，催化和分析科学等各个领域都吸引了越来越多的关注，这主要是由于它们具有独特的类似于分子的特性，例如HOMO-LUMO（最高占据和最低未占据分子轨道）跃迁，定量电荷以及光致发光。所有这些物理化学性质对Au NCs的大小和组成高度敏感，因此在合成过程中控制这些变量的能力非常重要。这篇综述描述了在Au NC合成过程中精确控制这些特征的最新进展，通常是通过还原Au（I）-SR络合物来实现的。首先，说明原子精确的Au-n（SR）（m）NC的形成机理，该机理可分为两个阶段：1）通过还原Au（I）-SR络合物（还原辅助）生成中间NC 2）中间NC的尺寸演化形成具有原子精度的Au NC物种（尺寸演化阶段）。基于这种缩小尺寸演化机制，总结了在缩小辅助生长阶段实施的尺寸/成分控制策略。然后给出了在大小演变阶段具有影响的调节策略的细节。最后，表明在还原速率和尺寸演变之间取得平衡可能是一种统一的方法，可用于高产量的Au-n（SR）（m）NC的简便合成（大规模生产，易于制备，反应时间短）。控制它们的大小和组成。该概念可能有助于大规模方法的设计和开发，这些方法用于合成具有先进功能的稳定，定义明确的Au NC，以便在不同领域的广泛应用中使用。 （C）2016 Elsevier B.V.保留所有权利。

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  • 来源
    《Coordination chemistry reviews》 |2016年第12期|1-15|共15页
  • 作者

    Goswami Nirmal; Yao Qiaofeng; Chen Tiankai; Xie Jianping;

  • 作者单位

    Natl Univ Singapore, Dept Chem & Biomol Engn, 4 Engn Dr 4, Singapore 117585, Singapore;

    Natl Univ Singapore, Dept Chem & Biomol Engn, 4 Engn Dr 4, Singapore 117585, Singapore;

    Natl Univ Singapore, Dept Chem & Biomol Engn, 4 Engn Dr 4, Singapore 117585, Singapore;

    Natl Univ Singapore, Dept Chem & Biomol Engn, 4 Engn Dr 4, Singapore 117585, Singapore;

  • 收录信息 美国《科学引文索引》(SCI);美国《生物学医学文摘》(MEDLINE);
  • 原文格式 PDF
  • 正文语种 eng
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