Abstract
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.
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References
Aulin C, Karabulut E, Tran A et al (2013) Transparent nanocellulosic multilayer thin films on polylactic acid with tunable gas barrier properties. ACS Appl Mater Interfaces 5:7352–7359. https://doi.org/10.1021/am401700n
Borges J, Rodrigues LC, Reis RL, Mano JF (2014) Layer-by-layer assembly of light-responsive polymeric multilayer systems. Adv Func Mater 24:5624–5648. https://doi.org/10.1002/adfm.201401050
Dmochowska A, Peixinho J, Sollogoub C, Miquelard-Garnier G (2023) Extensional viscosity of immiscible polymer multi-nanolayer films: signature of the interphase. Macromolecules 56:6222–6231. https://doi.org/10.1021/acs.macromol.3c00288
Gholami F, Pakzad L, Behzadfar E (2020) Morphological, interfacial and rheological properties in multilayer polymers: a review. Polymer 208:122950. https://doi.org/10.1016/j.polymer.2020.122950
Giumanca R (2002) The Effects of Long Chain Branching on the rheological properties of polymers. The University of British Columbia
He L, Shi Y, Wang Q et al (2020) Strategy for constructing electromagnetic interference shielding and flame retarding synergistic network in poly (butylene succinate) and thermoplastic polyurethane multilayered composites. Compos Sci Technol 199:108324. https://doi.org/10.1016/j.compscitech.2020.108324
Huang Q (2022) When polymer chains are highly aligned: a perspective on extensional rheology. Macromolecules 55:715–727. https://doi.org/10.1021/acs.macromol.1c02262
Janzen J, Colby RH (1999) Diagnosing long-chain branching in polyethylenes. J Mol Struct 485–486:569–583. https://doi.org/10.1016/S0022-2860(99)00097-6
Jordan AM, Lee P, Thurber C, Macosko CW (2018) Adapting a capillary rheometer for research on polymer melt interfaces. Ind Eng Chem Res 57:14106–14113. https://doi.org/10.1021/acs.iecr.8b03674
Jordan AM, Lee B, Kim K et al (2019) Rheology of polymer multilayers: slip in shear, hardening in extension. J Rheol 63:751–761. https://doi.org/10.1122/1.5109788
Kazmierczak T, Song H, Hiltner A, Baer E (2007) Polymeric one-dimensional photonic crystals by continuous coextrusion. Macromol Rapid Commun 28:2210–2216. https://doi.org/10.1002/marc.200700367
Lamnawar K, Zhang H, Maazouz A (2013) Coextrusion of multilayer structures, interfacial phenomena. In: Encyclopedia of Polymer Science and Technology
Lee PC, Park HE, Morse DC, Macosko CW (2009) Polymer-polymer interfacial slip in multilayered films. J Rheol 53:893–915. https://doi.org/10.1122/1.3114370
Levitt L, Macosko CW, Schweizer T, Meissner J (1997) Extensional rheometry of polymer multilayers: a sensitive probe of interfaces. J Rheol 41:671–685. https://doi.org/10.1122/1.550829
Li Z, Olah A, Baer E (2020) Micro- and nano-layered processing of new polymeric systems. Prog Polym Sci 102:101210. https://doi.org/10.1016/j.progpolymsci.2020.101210
Li S, Qian K, Thaiboonrod S et al (2021) Flexible multilayered aramid nanofiber/silver nanowire films with outstanding thermal durability for electromagnetic interference shielding. Compos A Appl Sci Manuf 151:106643. https://doi.org/10.1016/j.compositesa.2021.106643
Li J, Touil I, Sudre G et al (2024) Fabrication of architectured multilayers with mismatched rheological behaviors: layer stability, structure, and confinement dictate polyethylene-based film properties. Ind Eng Chem Res 63:1953–1964. https://doi.org/10.1021/acs.iecr.3c03923
Liu G, Sun H, Rangou S et al (2013) Studying the origin of “strain hardening”: basic difference between extension and shear. J Rheol 57:89–104. https://doi.org/10.1122/1.4763568
Lu B, Lamnawar K, Maazouz A (2017a) Rheological and dynamic insights into an in situ reactive interphase with graft copolymers in multilayered polymer systems. Soft Matter 13:2523–2535. https://doi.org/10.1039/C6SM02658C
Lu B, Lamnawar K, Maazouz A (2017b) Influence of in situ reactive interphase with graft copolymer on shear and extensional rheology in a model bilayered polymer system. Polym Testing 61:289–299. https://doi.org/10.1016/j.polymertesting.2017.05.037
Lu B, Lamnawar K, Maazouz A, Sudre G (2018) Critical role of interfacial diffusion and diffuse interphases formed in multi-micro-/nanolayered polymer films based on poly(vinylidene fluoride) and poly(methyl methacrylate). ACS Appl Mater Interfaces 10:29019–29037. https://doi.org/10.1021/acsami.8b09064
Lu B, Alcouffe P, Sudre G et al (2020a) Unveiling the effects of in situ layer–layer interfacial reaction in multilayer polymer films via multilayered assembly: from microlayers to nanolayers. Macromol Mater Eng 305:2000076. https://doi.org/10.1002/mame.202000076
Lu B, Alcouffe P, Sudre G et al (2020b) Unveiling the effects of in situ layer–layer interfacial reaction in multilayer polymer films via multilayered assembly: from microlayers to nanolayers. Macromol Mater Eng 2000076:1–16. https://doi.org/10.1002/mame.202000076
Lu B, Bondon A, Touil I et al (2020c) Role of the macromolecular architecture of copolymers at layer-layer interfaces of multilayered polymer films: a combined morphological and rheological investigation. Ind Eng Chem Res 59:22144–22154. https://doi.org/10.1021/acs.iecr.0c04731
Lu B, Zhang H, Maazouz A, Lamnawar K (2021) Interfacial phenomena in multi-micro-/nanolayered polymer coextrusion: a review of fundamental and engineering aspects. Polymers 13. https://doi.org/10.3390/polym13030417
Orwoll RA, Arnold PA (2007) Physical properties of polymers handbook. Mark, JE, Ed 104
Palierne JF (1990) Linear rheology of viscoelastic emulsions with interfacial tension. Rheol Acta 29:204–214. https://doi.org/10.1007/BF01331356
Park HE(박희언), Lee PC, Macosko CW (2010) Polymer-polymer interfacial slip by direct visualization and by stress reduction. J Rheol 54:1207–1218. https://doi.org/10.1122/1.3479389
Ponting M, Burt TM, Korley LTJ et al (2010a) Gradient multilayer films by forced assembly coextrusion. Ind Eng Chem Res 49:12111–12118. https://doi.org/10.1021/ie100321h
Ponting M, Hiltner A, Baer E (2010b) Polymer nanostructures by forced assembly: process, structure, and properties. Macromol Symp 294:19–32. https://doi.org/10.1002/masy.201050803
Qiao H, Zheng B, Zhong G et al (2023) Understanding the rheology of polymer–polymer interfaces covered with janus nanoparticles: polymer blends versus particle sandwiched multilayers. Macromolecules 56:647–663. https://doi.org/10.1021/acs.macromol.2c01973
Sentmanat M, Wang BN, McKinley GH (2005) Measuring the transient extensional rheology of polyethylene melts using the SER universal testing platform. J Rheol 49:585–606. https://doi.org/10.1122/1.1896956
Thompson RL, Oishi CM (2021) Reynolds and Weissenberg numbers in viscoelastic flows. J Nonnewton Fluid Mech 292:104550. https://doi.org/10.1016/j.jnnfm.2021.104550
Wang H, Keum JK, Hiltner A, Baer E (2009) Confined crystallization of PEO in nanolayered films impacting structure and oxygen permeability. Macromolecules 42:7055–7066. https://doi.org/10.1021/ma901379f
Wood-Adams PM, Dealy JM, DeGroot AW, Redwine OD (2000) Effect of molecular structure on the linear viscoelastic behavior of polyethylene. Macromolecules 33:7489–7499. https://doi.org/10.1021/ma991533z
Yang Y-H, Haile M, Park YT et al (2011) Super gas barrier of all-polymer multilayer thin films. Macromolecules 44:1450–1459. https://doi.org/10.1021/ma1026127
Yin G, Wang Y, Wang W, Yu D (2020) Multilayer structured PANI/MXene/CF fabric for electromagnetic interference shielding constructed by layer-by-layer strategy. Colloids Surf, A 601:125047. https://doi.org/10.1016/j.colsurfa.2020.125047
Zhang H, Lamnawar K, Maazouz A (2012) Rheological modeling of the diffusion process and the interphase of symmetrical bilayers based on PVDF and PMMA with varying molecular weights. Rheol Acta 51:691–711. https://doi.org/10.1007/s00397-012-0629-7
Zhang H, Lamnawar K, Maazouz A (2015) Fundamental understanding and modeling of diffuse interphase properties and its role in interfacial flow stability of multilayer polymers. Polym Eng Sci 55:771–791. https://doi.org/10.1002/pen.23945
Zhang H, Lamnawar K, Maazouz A, Maia JM (2016) A nonlinear shear and elongation rheological study of interfacial failure in compatible bilayer systems. J Rheol 60:1–23. https://doi.org/10.1122/1.4926492
Zhang X, Xu Y, Zhang X et al (2019) Progress on the layer-by-layer assembly of multilayered polymer composites: strategy, structural control and applications. Prog Polym Sci 89:76–107. https://doi.org/10.1016/j.progpolymsci.2018.10.002
Zhao R, Macosko CW (2002) Slip at polymer–polymer interfaces: rheological measurements on coextruded multilayers. J Rheol 46:145–167. https://doi.org/10.1122/1.1427912
Zhu Y, Bironeau A, Restagno F et al (2016) Kinetics of thin polymer film rupture: model experiments for a better understanding of layer breakups in the multilayer coextrusion process. Polymer 90:156–164. https://doi.org/10.1016/j.polymer.2016.03.005
Acknowledgements
The authors acknowledge Pierre Alcouffe for kind assistance with microscope observations. Author Jixiang Li also thanks China Scholarship Council for providing the doctoral scholarship.
Funding
This research was funded in part the MESRI (Ministère de l’Enseignement Supérieur, de la Recherche et de l’Innovation) with I.T Grant. The authors thank INSA Lyon of its support through BQR “DEVMAN-2022” grants. K.L thanks the French National Research Agency (ANR, grant no. ANR-11-RMNP-0002, and ANR, grant no. ANR-20-CE06-0003 and ANR-22-PERE-0002-PLASTICS).
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Li, J., Touil, I., Lu, B. et al. 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. Rheol Acta (2024). https://doi.org/10.1007/s00397-024-01445-z
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DOI: https://doi.org/10.1007/s00397-024-01445-z