Gooranorimi Amirhossein, Mousavifard Seyyed Mohammad, Mohseni Mohsen, Yahyaei Hossein, Makki Hesam
Department of Polymer and Color Engineering, Amirkabir University of Technology, 424 Hafez Avenue, Tehran 15875-4413, Iran.
Department of Chemistry and Materials Innovation Factory, University of Liverpool, Liverpool L69 7ZD, U.K.
ACS Appl Polym Mater. 2025 Jul 17;7(14):9034-9044. doi: 10.1021/acsapm.5c01155. eCollection 2025 Jul 25.
The structural complexities of polymer networks, i.e., multiple functional groups, diverse connection sites, and various defects, make it difficult to accurately describe their microstructure using theoretical models and traditional metrics such as the cross-link density (XLD). This study uses multiscale molecular dynamics simulations to construct complex network structures such as acrylic-melamine systems and establish correlations between their microstructure and thermomechanical properties. By accounting for the elastic contribution of each cross-link point within the network, we modified the XLD and introduced effective XLD (XLD). Our findings reveal strong linear correlations between XLD and both elastic modulus and , relationships that conventional XLD could not establish. This demonstrates the robustness of XLD as a predictive metric for thermomechanical properties across diverse cross-linking conversions and prepolymer systems. XLD thus serves as a valuable metric for the in silico design and optimization of thermoset polymers with tailored thermomechanical properties.
聚合物网络的结构复杂性，即多个官能团、多样的连接位点和各种缺陷，使得使用理论模型和传统指标（如交联密度（XLD））准确描述其微观结构变得困难。本研究使用多尺度分子动力学模拟来构建诸如丙烯酸 - 三聚氰胺体系等复杂网络结构，并建立其微观结构与热机械性能之间的相关性。通过考虑网络内每个交联点的弹性贡献，我们修正了XLD并引入了有效XLD（XLD）。我们的研究结果揭示了XLD与弹性模量和 之间都存在很强的线性相关性，而传统XLD无法建立这种关系。这证明了XLD作为预测不同交联转化率和预聚物体系热机械性能指标的稳健性。因此，XLD是用于具有定制热机械性能热固性聚合物计算机辅助设计和优化的有价值指标。
