化学反应和老化大分子混合物 II:相分离和粗化

Ruoyao Zhang, Sheng Mao, Mikko P. Haataja
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摘要

在另一篇论文中,我们提出了一个通过涉及多种大分子的化学反应进行复合物形成的热力学模型,该模型随后可能发生液-液相分离,并进一步转变为凝胶状。在本研究中,我们提出了一个热力学一致的动力学框架,以研究空间不均匀大分子混合物中的相分离、化学反应和老化之间的相互作用。同时还提出了一种数值算法,用于模拟液态和凝胶态在二维和三维空间中通过被动布朗运动碰撞产生的态域增长。我们的研究结果表明,凝胶化程度和布朗运动对凝聚行为有显著影响。凝结物内部凝胶相的存在极大地限制了扩散传输过程,而在凝胶状凝结物面积/体积分数较高的系统中,布朗运动凝聚控制了凝聚过程,从而形成了相互连接的畴,其非典型畴增长率受尺寸相关的平移和旋转扩散率控制。
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Chemically reactive and aging macromolecular mixtures II: Phase separation and coarsening
In a companion paper, we put forth a thermodynamic model for complex formation via a chemical reaction involving multiple macromolecular species, which may subsequently undergo liquid-liquid phase separation and a further transition into a gel-like state. In the present work, we formulate a thermodynamically consistent kinetic framework to study the interplay between phase separation, chemical reaction and aging in spatially inhomogeneous macromolecular mixtures. A numerical algorithm is also proposed to simulate domain growth from collisions of liquid and gel domains via passive Brownian motion in both two and three spatial dimensions. Our results show that the coarsening behavior is significantly influenced by the degree of gelation and Brownian motion. The presence of a gel phase inside condensates strongly limits the diffusive transport processes, and Brownian motion coalescence controls the coarsening process in systems with high area/volume fractions of gel-like condensates, leading to formation of interconnected domains with atypical domain growth rates controlled by size-dependent translational and rotational diffusivities.
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