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Toward Solution Syntheses of the Tetrahedral Au20 Pyramid and Atomically Precise Gold Nanoclusters with Uncoordinated Sites
Accounts of Chemical Research ( IF 16.4 ) Pub Date : 2018-08-02 00:00:00 , DOI: 10.1021/acs.accounts.8b00257
Qian-Fan Zhang 1 , Xuenian Chen 2 , Lai-Sheng Wang 1
Affiliation  

A long-standing objective of cluster science is to discover highly stable clusters and to use them as models for catalysts and building blocks for cluster-assembled materials. The discovery of catalytic properties of gold nanoparticles (AuNPs) has stimulated wide interests in gaseous size-selected gold clusters. Ligand-protected AuNPs have also been extensively investigated to probe their size-dependent catalytic and optical properties. However, the need to remove ligands can introduce uncertainties in both the structures and sizes of ligand-protected AuNPs for catalytic applications. Ideal model catalysts should be atomically precise AuNPs with well-defined structures and uncoordinated surface sites as in situ active centers. The tetrahedral (Td) Au20 pyramidal cluster, discovered to be highly stable in the gas phase, provided a unique opportunity for such an ideal model system. The Td-Au20 consists of four Au(111) faces with all its atoms on the surface. Bulk synthesis of Td-Au20 with appropriate ligands would allow its catalytic and optical properties to be investigated and harnessed. The different types of its surface atoms would allow site-specific chemistry to be exploited. It was hypothesized that if the four corner atoms of Td-Au20 were coordinated by ligands the cluster would still contain 16 uncoordinated surface sites as potential in situ catalytically active centers.

中文翻译:

四面体Au 20金字塔和原子精确的具有不协调位点的金纳米团簇的溶液合成

团簇科学的长期目标是发现高度稳定的团簇,并将其用作团簇组装材料的催化剂和结构单元的模型。金纳米颗粒(AuNPs)催化性能的发现激发了人们对气态大小选择的金团簇的广泛兴趣。还对配体保护的AuNPs进行了广泛研究,以探究其尺寸依赖性的催化和光学性质。然而,需要去除配体会在用于催化应用的配体保护的AuNPs的结构和尺寸上引入不确定性。理想的模型催化剂应该是原子精确的AuNPs,具有定义明确的结构和不协调的表面位点作为原位活性中心。四面体(T d)Au 20被发现在气相中高度稳定的金字塔状簇为这种理想的模型系统提供了独特的机会。所述Ť d -Au 20由四个AU(111)的面与所有其表面上的原子。具有适当配体的T d -Au 20的本体合成将允许研究和利用其催化和光学性质。其表面原子的不同类型将允许利用位点特异性化学。假设如果T d -Au 20的四个角原子被配体配位,则该簇仍将包含16个未配位的表面位点作为原位电势 催化活性中心。
更新日期:2018-08-02
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