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非等温体系中由非平衡自组装诱导产生的李赛根环。

Nonequilibrium self-assembly induced Liesegang rings in a non-isothermal system.

作者信息

Arango-Restrepo Andrés, Barragán Daniel, Rubi J Miguel

机构信息

Escuela de Química, Facultad de Ciencias, Universidad Nacional de Colombia, Calle 59A No. 63-30, Bloque 21, Núcleo el volador, Medellín, Colombia.

出版信息

Phys Chem Chem Phys. 2018 Feb 14;20(7):4699-4707. doi: 10.1039/c7cp08469b.

Abstract

We propose a model to show the formation of Liesegang rings under non-isothermal conditions. The model formulates reaction-diffusion equations for all components intervening in the process together with an evolution equation for the temperature. The reactive parts in these equations follow from the analysis of the non-equilibrium self-assembly (NESA) process undergone by the meso-particles which make up the patterns. The solution of these equations enables us to know the concentration of each component, the spherical structures diameter, and the system temperature as a function of time and radial position. The values found for the structures diameter and the rings position are in agreement with the experiments. The results for the system temperature with peaks at the rings positions suggest that heat accumulates at these positions as a consequence of the dissipation inherent to the NESA process. Our model enables us to rationalize how from non-homogeneous initial conditions a transient self-organization process involving formation of self-assembled structures may produce macroscopic patterns. It can, in general, be used to analyze pattern formation due to diffusion-reaction-precipitation processes with potential applications in the design of advanced materials.

摘要

我们提出了一个模型来展示非等温条件下李塞根环的形成。该模型为过程中涉及的所有组分制定了反应扩散方程以及温度演化方程。这些方程中的反应部分源于对构成图案的介观粒子所经历的非平衡自组装(NESA)过程的分析。这些方程的解使我们能够了解各组分的浓度、球形结构直径以及作为时间和径向位置函数的系统温度。所得到的结构直径和环位置的值与实验结果一致。系统温度在环位置出现峰值的结果表明,由于NESA过程固有的耗散,热量在这些位置积累。我们的模型使我们能够解释从非均匀初始条件出发,涉及自组装结构形成的瞬态自组织过程如何产生宏观图案。一般来说,它可用于分析由扩散 - 反应 - 沉淀过程导致的图案形成,在先进材料设计中具有潜在应用。

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