WestCHEM, School of Chemistry, University of Glasgow, Glasgow G12 8QQ, UK.
Nat Commun. 2014 Apr 28;5:3715. doi: 10.1038/ncomms4715.
The discovery of gigantic molecular nanostructures like coordination and polyoxometalate clusters is extremely time-consuming since a vast combinatorial space needs to be searched, and even a systematic and exhaustive exploration of the available synthetic parameters relies on a great deal of serendipity. Here we present a synthetic methodology that combines a flow reaction array and algorithmic control to give a chemical 'real-space' search engine leading to the discovery and isolation of a range of new molecular nanoclusters based on Mo(2)O(2)S(2)-based building blocks with either fourfold (C4) or fivefold (C5) symmetry templates and linkers. This engine leads us to isolate six new nanoscale cluster compounds: 1, {Mo(10)(C5)}; 2, {Mo(14)(C4)4(C5)2}; 3, {Mo(60)(C4)10}; 4, {Mo(48)(C4)6}; 5, {Mo(34)(C4)4}; 6, {Mo(18)(C4)9}; in only 200 automated experiments from a parameter space spanning ~5 million possible combinations.
发现像配位和多金属氧酸盐簇这样的巨大分子纳米结构极其耗时，因为需要搜索庞大的组合空间，即使系统地、详尽地探索现有的合成参数也依赖于大量的偶然发现。在这里，我们提出了一种合成方法，将流动反应阵列和算法控制相结合，为化学提供了一个“实空间”搜索引擎，从而发现和分离了一系列基于Mo(2)O(2)S(2) 为基础的构建块的新型分子纳米簇，这些构建块具有四重（C4）或五重（C5）对称模板和连接体。这个引擎使我们能够分离出六种新的纳米级簇化合物：1、{Mo(10)(C5)}；2、{Mo(14)(C4)4(C5)2}；3、{Mo(60)(C4)10}；4、{Mo(48)(C4)6}；5、{Mo(34)(C4)4}；6、{Mo(18)(C4)9}，仅从跨越约 500 万个可能组合的参数空间进行了 200 次自动化实验。
