A grand unified model for liganded gold clusters.
A grand unified model for liganded gold clusters.
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配位金簇的大统一模型
DOI：
10.1038/ncomms13574
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发表时间：
2016-12-02
影响因子：
16.6
通讯作者：
Gao, Yi
中科院分区：
文献类型：
--
作者：
Xu, Wen Wu;Zhu, Beien;Zeng, Xiao Cheng;Gao, Yi
一个大统一模型（GUM）的发展，以实现丰富的结构的所有71个配体金团簇的基本理解。受夸克模型的启发，复合粒子（例如质子和中子）是由三个夸克（或味道）组合而成的，这里金原子被分配了三种“味道”（即底部，中间和顶部）来代表三种可能的价态。GUM中的“复合粒子”被分为两类：三角形基本块Au 3（2e）和四面体基本块Au 4（2e）的变体，它们都满足价层的duet规则（2e），类似于普通化学中的八隅体规则。当这些基本块堆积在一起时，就形成了配位金簇的核心。利用该模型，可以解释71个金团簇的结构和生长机制。虽然GUM是一个预测性的启发式，可能不一定反映实际的电子结构，几个高度稳定的配体金簇的预测，从而提供GUM引导的配体金簇的合成设计。 没有一个理论模型可以解释所有已知的配体金簇的稳定性。在这里，作者提出了一个受粒子物理学夸克模型启发的大统一模型，该模型将金团簇描述为由金原子“基本粒子”构建的稳定三角形Au 3（2e）和四角形Au 4（2e）“复合粒子”的组合。
A grand unified model (GUM) is developed to achieve fundamental understanding of rich structures of all 71 liganded gold clusters reported to date. Inspired by the quark model by which composite particles (for example, protons and neutrons) are formed by combining three quarks (or flavours), here gold atoms are assigned three ‘flavours' (namely, bottom, middle and top) to represent three possible valence states. The ‘composite particles' in GUM are categorized into two groups: variants of triangular elementary block Au3(2e) and tetrahedral elementary block Au4(2e), all satisfying the duet rule (2e) of the valence shell, akin to the octet rule in general chemistry. The elementary blocks, when packed together, form the cores of liganded gold clusters. With the GUM, structures of 71 liganded gold clusters and their growth mechanism can be deciphered altogether. Although GUM is a predictive heuristic and may not be necessarily reflective of the actual electronic structure, several highly stable liganded gold clusters are predicted, thereby offering GUM-guided synthesis of liganded gold clusters by design. There is no one theoretical model that can explain the stability of all known liganded gold clusters. Here, the authors present a grand unified model, inspired by the quark model of particle physics, which describes gold clusters as combinations of stable triangular Au3(2e) and tetragonal Au4(2e) ‘composite particles' built from gold atom ‘elementary particles'.
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