Linking models of polymerization and dynamics to predict branched polymer structure and flow.
Linking models of polymerization and dynamics to predict branched polymer structure and flow.
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连接聚合和动力学模型来预测支化聚合物结构和流动。
DOI：
10.1126/science.1207060
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发表时间：
2011
期刊：
影响因子：
--
通讯作者：
Read DJ
中科院分区：
文献类型：
--
作者：
Read DJ
我们提出了一种预测方案，将具有工业水平复杂性的高分支纠缠聚合物的拓扑结构与聚合物熔体的紧急粘弹性联系起来。该方案能够计算随机支链“高压自由基”聚合物熔体的线性和非线性粘弹性及其形成化学动力学的函数。该方法将聚合的数值模拟与聚合物动力学的管/缠结物理扩展到完全非线性响应相结合。我们将一系列低密度聚乙烯的计算与结构和粘弹性性能的实验进行了比较。该方法为这些熔体优化流变性的分子过程提供了一个窗口，将基础科学与复杂流动的过程联系起来，并开辟了新材料的计算机设计。
We present a predictive scheme connecting the topological structure of highly branched entangled polymers, with industrial-level complexity, to the emergent viscoelasticity of the polymer melt. The scheme is able to calculate the linear and nonlinear viscoelasticity of a stochastically branched “high-pressure free radical” polymer melt as a function of the chemical kinetics of its formation. The method combines numerical simulation of polymerization with the tube/entanglement physics of polymer dynamics extended to fully nonlinear response. We compare calculations for a series of low-density polyethylenes with experiments on structural and viscoelastic properties. The method provides a window onto the molecular processes responsible for the optimized rheology of these melts, connecting fundamental science to process in complex flow, and opens up the in silico design of new materials.