Gradual Solvent Quality Changes Induce Abrupt Changes in Interfacial Layer, Dispersion Structure, and Physical Properties of Polymer Nanocomposites

IF 5.2 1区化学 Q1 POLYMER SCIENCE

Macromolecules Pub Date : 2024-09-20 DOI:10.1021/acs.macromol.4c02103

Tae Yeon Kong, Nicolas R. de Souza, So Youn Kim

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Abstract

The polymer interfacial layer, formed by the polymer adsorption onto the surface of nanoparticles (NPs) due to polymer-NP interactions, is well-known to determine the particle dispersion and resulting physical properties of polymer nanocomposites (PNCs). Given that PNC processing generally occurs in the presence of solvents, understanding the influence of solvent quality on the effective polymer-NP interaction is crucial for controlling the microstructure and properties of PNCs. However, the inherent solubility parameter of solvents imposes limitations on systematic analyses based on gradual solvent quality changes. Here, we systematically investigate the role of solvent quality on PNC by using solvent mixtures. We found that the microstructure and physical properties of PNCs varied with the solubility parameter difference between polymer and solvent mixture, suggesting a critical difference of 5 MPa^1/2. These changes are attributed to the structure, rather than the dynamics, of the interfacial layer, which originates from the polymer–particle effective interaction. This study emphasizes the critical role of solvent quality in achieving desired PNC properties and offers insights for optimizing process solvents in various applications of polymer-NP suspensions.

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溶剂质量的渐变会引起聚合物纳米复合材料界面层、分散结构和物理性质的突变

众所周知，聚合物界面层是由聚合物吸附在纳米粒子（NPs）表面而形成的，它决定了粒子的分散性和聚合物纳米复合材料（PNCs）的物理性质。鉴于 PNC 加工通常是在有溶剂存在的情况下进行的，因此了解溶剂质量对聚合物-NP 有效相互作用的影响对于控制 PNC 的微观结构和性能至关重要。然而，溶剂固有的溶解度参数限制了基于溶剂质量渐变的系统分析。在此，我们使用混合溶剂系统地研究了溶剂质量对 PNC 的作用。我们发现，PNC 的微观结构和物理性质随聚合物和混合溶剂之间的溶解度参数差异而变化，临界差异为 5 MPa1/2。这些变化归因于界面层的结构而非动力学，它源于聚合物与粒子之间的有效相互作用。这项研究强调了溶剂质量在实现所需的 PNC 特性方面的关键作用，并为优化聚合物-NP 悬浮液各种应用中的加工溶剂提供了启示。

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来源期刊

Macromolecules 工程技术-高分子科学

CiteScore

9.30

自引率

16.40%

发文量

942

审稿时长

2 months

期刊介绍： Macromolecules publishes original, fundamental, and impactful research on all aspects of polymer science. Topics of interest include synthesis (e.g., controlled polymerizations, polymerization catalysis, post polymerization modification, new monomer structures and polymer architectures, and polymerization mechanisms/kinetics analysis); phase behavior, thermodynamics, dynamic, and ordering/disordering phenomena (e.g., self-assembly, gelation, crystallization, solution/melt/solid-state characteristics); structure and properties (e.g., mechanical and rheological properties, surface/interfacial characteristics, electronic and transport properties); new state of the art characterization (e.g., spectroscopy, scattering, microscopy, rheology), simulation (e.g., Monte Carlo, molecular dynamics, multi-scale/coarse-grained modeling), and theoretical methods. Renewable/sustainable polymers, polymer networks, responsive polymers, electro-, magneto- and opto-active macromolecules, inorganic polymers, charge-transporting polymers (ion-containing, semiconducting, and conducting), nanostructured polymers, and polymer composites are also of interest. Typical papers published in Macromolecules showcase important and innovative concepts, experimental methods/observations, and theoretical/computational approaches that demonstrate a fundamental advance in the understanding of polymers.