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Self-assembly of bis-salphen compounds: from semiflexible chains to webs of nanorings†
Soft Matter ( IF 3.4 ) Pub Date : 2018-01-12 00:00:00 , DOI: 10.1039/c7sm02371e
Sergey V. Pyrlin 1, 2, 3, 4, 5 , Nicholas D. M. Hine 6, 7, 8, 9 , Arjan W. Kleij 10, 11, 12, 13, 14 , Marta M. D. Ramos 1, 2, 3, 4, 5
Affiliation  

The recently-observed self-assembly of certain salphen-based compounds into neuron-like networks of microrings interconnected with nano-thin strings may suggest a new highly-potent tool for nanoscale patterning. However, the mechanism behind such phenomena needs to be clarified before they can be applied in materials design. Here we show that, in contrast with what was initially presumed, the emergence of a “rings-and-rods” pattern is unlikely to be explained by merging, collapse and piercing of vesicles as in previously reported cases of nanorings self-assembly via non-bonding interactions. We propose an alternative explanation: the compounds under study form a 1D coordination polymer, the fibres of which are elastic enough to fold into toroidal globules upon solvent evaporation, while being able to link separate chains into extended networks. This becomes possible because the structure of the compound's scaffold is found to adopt a very different conformation from that inferred in the original work. Based on ab initio and molecular dynamics calculations we propose a step-by-step description of self-assembly process of a supramolecular structure which explains all the observed phenomena in a simple and clear way. The individual roles of the compound' s scaffold structure, coordination centres, functional groups and solvent effects are also explained, opening a route to control the morphology of self-assembled networks and to synthesize new compounds exhibiting similar behaviour.

中文翻译:

双沙芬化合物的自组装:从半柔性链到纳米环网

最近观察到的某些基于赛尔芬的化合物自组装成与纳米细线互连的神经环状微环网络,这可能为纳米级图案化提供了一种新的高效工具。但是,在将这种现象应用于材料设计之前,需要弄清楚这种现象的机理。在这里,我们表明,与最初的假设相反,“环和棒”模式的出现不太可能通过囊泡的合并,塌陷和刺穿来解释,就像先前报道的通过环自组装的纳米环的情况一样。非键相互作用。我们提出另一种解释:正在研究的化合物形成一维配位聚合物,其纤维具有足够的弹性,可在溶剂蒸发后折叠成环状小球,同时能够将单独的链连接成扩展的网络。这是可能的,因为发现该化合物支架的结构采用了与原始工作中所推导的构象非常不同的构象。基于从头算和分子动力学计算,我们提出了超分子结构自组装过程的分步描述,以简单明了的方式解释了所有观察到的现象。还解释了该化合物的骨架结构,配位中心,官能团和溶剂作用的各个作用,从而开辟了一条途径来控制自组装网络的形态并合成表现出相似行为的新化合物。
更新日期:2018-01-12
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