Interfacial shear and elongational rheology of immiscible multi-micro-nanolayered polymers: contribution for probing the effect of highly mismatched viscoelastic properties and modeling interfacial tension properties

The present work explores the shear and extensional rheology of immiscible multi-micro/nanolayered systems comprising low-density polyethylene (LDPE) paired with polystyrene (PS) and polycarbonate (PC) obtained from forced-assembly multilayer coextrusion. Firstly, miscible multilayer references based on LDPE/LLDPE layers were prepared with their miscibility characterized by shear and elongational measurements. Their strain hardening behaviors were found to be intricately linked to the number of layers and confinement. Secondly, for immiscible LDPE/PS and LDPE/PC multilayers with symmetric (50/50) and asymmetric (10/90) compositions, negative deviation of complex viscosities from neat polymers was highlighted because of the heightened confinement of LDPE chains by PS or PC and reduced entanglements at polymer–polymer interfaces. Intriguingly, LDPE/PC systems exhibited no strain hardening irrespective of layer configuration, while the geometric confinement imposed by PS layers facilitated interactions between single chains with long-chain branching (LCB), leading to strain hardening under specific conditions. Furthermore, the extensional viscosities were predicted using the Macosko model (C.W. Macosko et al. Journal of Rheology. 63 2019), accurately describing the behavior of 1024 layered films for both asymmetric (10/90) LDPE/PS and LDPE/PC systems, but not for 32 layers due to a limited number of interfaces. This study provides insights into quantifying interfacial tension properties in micro/nano-layered systems with high mismatched viscoelastic polymers, shedding light on their strain hardening properties in the presence of increased interfacial area.

Graphical abstract