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首页> 外文期刊>Chemistry: A European journal >Mechanism of Crystalline Self-Assembly in Aqueous Medium: A Combined Cryo-TEM/Kinetic Study
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Mechanism of Crystalline Self-Assembly in Aqueous Medium: A Combined Cryo-TEM/Kinetic Study

机译：水性介质中晶体自组装的机理：低温-TEM /运动学联合研究

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摘要

Understanding the crystallization of organic molecules is a long-standing challenge. Herein, a mechanistic study on the self-assembly of crystalline arrays in aqueous solution is presented. The crystalline arrays are assembled from perylene diimide (PDI) amphiphiles bearing a chiral Nacetyltyrosine side group connected to the PDI aromatic core. A kinetic study of the crystallization process was performed using circular dichroism spectroscopy combined with time-resolved cryogenic transmission electron microscopy (cryo-TEM) imaging of key points along the reaction coordinate, and molecular dynamics simulation of the initial stages of the assembly. The study reveals a complex self-assembly process starting from the formation of amorphous aggregates that are transformed into crystalline material through a nucleation–growth process. Activation parameters indicate the key role of desolvation along the assembly pathway. The insights from the kinetic study correlate well with the structural data from cryo-TEM imaging. Overall, the study reveals four stages of crystalline self-assembly: 1) collapse into amorphous aggregates; 2) nucleation as partial ordering; 3) crystal growth; and 4) fusion of smaller crystalline aggregates into large crystals. These studies indicate that the assembly process proceeds according to a two-step crystallization model, whereby initially formed amorphous material is reorganized into an ordered system. This process follows Ostwald’s rule of stages, evolving through a series of intermediate phases prior to forming the final structure, thus providing an insight into the crystalline self-assembly process in aqueous medium.
机译：了解有机分子的结晶是一项长期的挑战。本文介绍了水溶液中晶体阵列自组装的机理研究。所述晶体阵列由带有手性N乙酰基酪氨酸侧基的per二酰亚胺（PDI）两亲物组装而成，所述手性N乙酰基酪氨酸侧基连接到PDI芳族核。使用圆二色光谱结合时间分辨的低温透射电子显微镜（cryo-TEM）沿反应坐标对关键点进行成像的动力学研究，以及装配初期的分子动力学模拟。这项研究揭示了一个复杂的自组装过程，该过程从形成无定形聚集体开始，然后通过成核-生长过程转化为结晶材料。激活参数表明去溶剂化沿组装路径的关键作用。动力学研究的见解与冷冻TEM成像的结构数据密切相关。总的来说，该研究揭示了晶体自组装的四个阶段：1）塌陷为无定形聚集体; 2）成核为部分有序; 3）晶体生长; 4）将较小的晶体聚集体融合成大晶体。这些研究表明，组装过程按照两步结晶模型进行，从而将最初形成的非晶材料重新组织为有序系统。此过程遵循Ostwald的阶段法则，在形成最终结构之前经历了一系列中间阶段的发展，从而提供了对水性介质中晶体自组装过程的了解。

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