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理解凝胶化为非平衡自组装过程。

Understanding Gelation as a Nonequilibrium Self-Assembly Process.

机构信息

Department of Chemistry, Science Faculty , Universidad Nacional de Colombia , Calle 59A No. 63-20, Bloque 21, Núcleo El Volador , Medellín 050034 , Colombia.

Department of Condensed Matter Physics, Faculty of Physics , University of Barcelona , Avinguda Diagonal 647 , 08028 Barcelona , Spain.

出版信息

J Phys Chem B. 2018 May 10;122(18):4937-4945. doi: 10.1021/acs.jpcb.8b02320. Epub 2018 Apr 30.

Abstract

Gel formation is described by a nonequilibrium self-assembly (SA) mechanism which considers the presence of precursors. Assuming that nonequilibrium structures appear and are maintained by entropy production, we developed a mesoscopic nonequilibrium thermodynamic model that describes the dynamic assembly of the structures. In the model, the evolution of the structures from the initially inactivated building blocks to the final agglomerates is governed by kinetic equations of the Fokker-Planck type. From these equations, we get the probability densities which enable one to know the measurable quantities such as the concentrations of the different components and the dynamic structure factor obtained in light-scattering experiments. Our results obtained are in very good agreement with the experiments. The model proposed can in general be used to analyze the kinetics of formation of nonequilibrium SA structures usually found in biomedicine and advanced materials.

摘要

凝胶的形成是由非平衡自组装(SA)机制来描述的,该机制考虑了前体的存在。假设非平衡结构的出现和维持是由熵产生的,我们开发了一个介观非平衡热力学模型,该模型描述了结构的动态组装。在该模型中,结构从最初的失活构建块到最终聚集体的演变由福克-普朗克(Fokker-Planck)类型的动力学方程控制。从这些方程中,我们得到了概率密度,从而可以知道可测量的量,如不同成分的浓度和在光散射实验中获得的动态结构因子。我们得到的结果与实验非常吻合。所提出的模型通常可用于分析在生物医学和先进材料中通常发现的非平衡 SA 结构形成的动力学。

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