Creating supramolecular semiregular Archimedean tilings via gas-mediated deprotonation of a terminal alkyne derivative
Creating supramolecular semiregular Archimedean tilings via gas-mediated deprotonation of a terminal alkyne derivative
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通过末端炔衍生物的气体介导去质子化创建超分子半规则阿基米德平铺
DOI：
10.1039/d1ce01413g
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发表时间：
2021
期刊：
影响因子：
3.1
通讯作者：
Y. Zhang
中科院分区：
文献类型：
--
作者：
H. Zhang;P. Cheng;L. Chen;Z. Chen;S. Klyatskaya;M. Ruben;J.V. Barth;Y. Zhang
将表面限制反应与超分子自组装相结合，可以将简单的分子前体化学转化为更高级的构造，从而产生具有独特结构和功能特性的复杂镶嵌。利用低温扫描隧道显微镜，我们首次证实了一种新的氧介导的末端炔去质子过程，将乙基-菲（EP）前体转化为吸附在Ag(111)/云母上的双（菲-2-乙基）银（BPE-Ag）配合物的高效化学反应。此外，我们发现BPE-Ag参与了三种不同类型的远程有序纳米孔超分子结构的形成，这些结构可以通过初始电位覆盖来调节。对于这三个相，基本构造都被验证为具有灵活配对结构的BPE-Ag二聚体。有趣的是，我们的平铺分析表明，两个相属于（3.6.3.6）类半正则阿基米德平铺（AT），第三个相表达一个新的（3.4.6.4）AT，不同于之前报道的相关网络。我们的研究结果说明了引入的合成策略在获取结构复杂性增加方面的潜力，并为进一步控制和探索界面半规则at的功能特性铺平了道路。
Combining surface-confined reactions with supramolecular self-assembly allows the chemical transformation of simple molecular precursors into higher-level tectons to generate complex tessellations with unique structural and functional properties. Herein, utilizing low-temperature scanning tunnelling microscopy, we firstly confirm a highly efficient chemical reaction converting ethynyl-phenanthrene (EP) precursors into bis(phenanthren-2-yleythnyl)silver (BPE–Ag) complexes adsorbed on Ag(111)/mica at room temperature via a novel oxygen-gas mediated terminal alkyne deprotonation process. Moreover, we show that the BPE–Ag species engage in the formation of three distinct types of long-range ordered nanoporous supramolecular architectures, which can be tuned by the initial EP coverage. For all three phases, the basic tectons were verified to be BPE–Ag dimers with flexible pairing configurations. Intriguingly, our tiling analysis reveals that two phases belong to the (3.6.3.6) class of semiregular Archimedean tiling (AT) and the third expresses a new (3.4.6.4) AT, different from the previously reported related networks. Our results illustrate the potential of the introduced synthesis strategy towards accessing architectures with increased complexity and pave the way towards further control and exploration regarding functional properties of interfacial semiregular ATs.