Linking Models of Polymerization and Dynamics to Predict Branched Polymer Structure and Flow

Read, Daniel J.; Auhl, Dietmar; Das, Chinmay; den Doelder, Jaap; Kapnistos, Michael; Vittorias, Iakovos; McLeish, Tom C.B.

Abstract

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.

Citation

Read, D. J., Auhl, D., Das, C., den Doelder, J., Kapnistos, M., Vittorias, I., & McLeish, T. C. (2011). Linking Models of Polymerization and Dynamics to Predict Branched Polymer Structure and Flow. Science, 333(6051), 1871-1874. https://doi.org/10.1126/science.1207060

• Journal Article Type: Article
• Publication Date: Sep 1, 2011
• Deposit Date: Jan 21, 2013
• Publicly Available Date: Jan 23, 2013
• Journal: Science
• Print ISSN: 0036-8075
• Electronic ISSN: 1095-9203
• Publisher: American Association for the Advancement of Science
• Peer Reviewed: Peer Reviewed
• Volume: 333
• Issue: 6051
• Pages: 1871-1874
• DOI: https://doi.org/10.1126/science.1207060
• Public URL: https://durham-repository.worktribe.com/output/1490522