Tunability of Self-Organized Structures Based on Thermodynamic Flux

Tunability of Self-Organized Structures Based on Thermodynamic Flux
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基于热力学通量的自组织结构的可调性

DOI:
10.1021/acs.langmuir.2c01602
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发表时间:
2022
期刊:
影响因子:
3.9
通讯作者:
Ban Takahiko
Ban Takahiko
中科院分区:
化学2区
文献类型:
--
作者:
Nabika Hideki;Tsukada Kanta;Itatani Masaki;Ban Takahiko

文献摘要

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大自然通过离子、分子和粒子等成分的自组织来建立结构和功能。了解决定由许多可能的替代方案形成的自组织结构的选择规则在根本上和技术上都很重要。在这项研究中,利用Liesegang现象探索了与反应扩散系统相关的自组织的选择规则,通过该现象形成了周期性沉淀模式作为模型系统。通过系统地改变质量通量来进行实验。在低质量通量时,形成垂直周期性图案,而在高质量通量时,形成水平周期性图案。结果推断,在熵产率反转的交叉通量处,自组织周期结构发生了结构垂直到水平的周期性转变。数值分析将所观察到的通量依赖性结构转变归因于选择具有更高熵产率的自组织模式。这些发现有助于我们理解自然如何控制自组织结构和几何形状,有可能促进新型设计、合成和制造工艺的发展,以实现良好控制的组织功能结构。
Nature establishes structures and functions via self-organization of constituents, including ions, molecules, and particles. Understanding the selection rule that determines the self-organized structure formed from many possible alternatives is fundamentally and technologically important. In this study, the selection rule for the self-organization associated with a reaction–diffusion system was explored using the Liesegang phenomenon, by which a periodic precipitation pattern is formed as a model system. Experiments were conducted by systematically changing the mass flux. At low mass fluxes, a vertically periodic pattern was formed, whereas at high mass fluxes, a horizontally periodic pattern was formed. The results inferred that a structural vertical-to-horizontal periodicity transition occurred in the self-organized periodic structure at the crossover flux at which the entropy production rate reversed. Numerical analyses attributed the as-observed flux-dependent structural transition to the selection of the self-organized pattern with a higher entropy production rate. These findings contribute to our understanding of how nature controls self-organized structures and geometry, potentially facilitating the development of novel designs, syntheses, and fabrication processes for well-controlled organized functional structures.