Accessible Requires Authentication Published by De Gruyter July 7, 2021

Effect of Uniaxial Stretching on Molecular Orientation, Crystallinity and Oxygen Permeability of Ethylene Vinyl Alcohol

L. Wang, E. Jalali Dil and A. Ajji


This work studies the effects of uniaxial stretching on molecular orientation, crystallinity, crystallography and oxygen permeability of high barrier multilayer films based on EVOH barrier layer. Film samples were prepared using two different blow-up ratios (BUR) of 1 and 3. Uniaxial stretching was applied at 100°C using a tensile machine equipped with an environmental chamber. Fourier transform infrared (FTIR) spectroscopy was used to examine the molecular orientation in the EVOH layer before and after stretching and confirmed a considerable increase in the molecular orientation in the EVOH layer. Dynamic scanning calorimetry (DSC) and wide-angle X-ray diffraction (XRD) results point to the perfection of EVOH crystal structure by applying uniaxial stretching at high temperatures. Oxygen permeability results showed a considerable 25% decrease after stretching of the sample with lower BUR while a significant 80% reduction in oxygen permeability was observed for the sample prepared at higher BUR. The mechanism involved in increasing oxygen permeability due to the uniaxial stretching at high temperature is discussed in detail.

Abdellah Ajji, CREPEC, Chemical Engineering Department, Polytechnique Montreal, Quebec, Canada H3T 1J4


Aktzi, N., Nir, Y., Wang, D., Narkis, M. and Siegmann, A., “EVOH/Clay Nanocomposites Produced by Melt Processing", Polym. Compos., 22, 710–720 (2001), DOI:10.1002/pc.10573 Search in Google Scholar

Aleperstein, D., Artzi, N., Siegmann, A. and Narkis, M., “Experimental and Computational Investigation of EVOH/Clay Nanocomposites”, J. Appl. Polym. Sci., 97, 2060–2066 (2005), DOI:10.1002/app.21937 Search in Google Scholar

Alvarez, V., Ruseckaite, R. and Vázquez, A., “Kinetic Analysis of Thermal Degradation in Poly(ethylene–vinyl alcohol) Copolymers”, J. Appl. Polym. Sci., 90, 3157–3163 (2003), DOI:10.1002/app.13071 Search in Google Scholar

Artzi, N., Nir, Y., Narkis, M. and Siegmann, A., “The Effect of Maleated Compatibilizers on the Structure and Properties of EVOH/Clay Nanocomposites”, Polym. Compos., 24, 627–639 (2003), DOI:10.1002/pc.10058 Search in Google Scholar

Bharadwaj, R. K.,“Modeling the Barrier Properties of Polymer-Layered Silicate Nanocomposites”, Macromolecules, 34, 9189 – 9192 (2001), DOI:10.1021/ma010780b Search in Google Scholar

Butler, T. I., Morris, B. A., “Chapter 15 PE Based Multilayer Film Structures”, in Multilayer Flexible Packaging, Wagner, J. R. (Ed.), William Andrew Publishing, Boston, p. 205–230 (2010), DOI:10.1016/B978-0-8155-2021-4.10015-2 Search in Google Scholar

Cerrada, M. L., Pérez, E., Pereña, J. M. and Benavente, R., “Wide-Angle X-Ray Diffraction Study of the Phase Behavior of Vinyl Alcohol–Ethylene Copolymers”, Macromolecules, 31, 2559–2564 (1998), DOI:10.1021/ma9705127 Search in Google Scholar

Chun, Y.-J., Ahn, T.-K.,“The Thermal and Mechanical Properties of Recycled PP/EVOH/PP Scrap with Compatibilizers”, Journal of The Korea Academia-Industrial Cooperation Society, 9, 176–181 (2008), DOI:10.5762/KAIS. 2008.9.1.176 Search in Google Scholar

Culter, J. D.,“Improving Barrier through Orientation in Processing”, J. Plast. Film Sheeting, 1, 215–225 (1985), DOI:10.1177/875608798500100305 Search in Google Scholar

Dias, P., Lin, Y. J., Hiltner, A., Baer, E., Chen, H. Y. and Chum, S. P., “Effect of Chain Architecture on Biaxial Orientation and Oxygen Permeability of Polypropylene Film”, J. Appl. Polym. Sci., 107, 1730–1736 (2008), DOI:10.1002/app.27197 Search in Google Scholar

Dil, E. J., Dhieb, F. B. and Ajji, A.,“Modeling the Effect of Nanoplate-lets Orientation on Gas Permeability of Polymer Nanocomposites”, Polymer, 168, 126–130 (2019), DOI:10.1016/j.polymer.2019.02.024 Search in Google Scholar

Franco Urquiza, E. A., Santana Pérez, O. O., Gamez-Perez, J., Martínez, A. B., and Maspoch, M. L., “Influence of Processing on the Ethylene-Vinyl Alcohol (EVOH) Properties: Application of the Successive Self-Nucleation and Annealing (SSA) Technique”, eXPRESS Polym. Lett., 4, 153–160 (2010), DOI:10.3144/expresspolymlett.2010.20 Search in Google Scholar

Global Plastic Packaging Market: Global Plastic Packaging Market 2019 – Industry, Size, Share, Growth, Trends Analysis and Forecast till 2024, Marketwatch, New York (2019) Search in Google Scholar

Global Plastic Packaging Market Research Report, Market Reserach Future, Marketwatch, New York (2020) Search in Google Scholar

Kamal, M. R., Garmabi, Hozhabr, S. and Arghyris, L., “The Development of Laminar Morphology during Extrusion of Polymer Blends”, Polym. Eng. Sci., 35, 41–51 (1995), DOI:10.1002/pen.760350107 Search in Google Scholar

Kamal, M. R., Lohfink, G., Arghyris, L. and Hozhbar-Ghelichi, S., U.S. Patent 5 188 784 (1993) Search in Google Scholar

Lee, S.-Y., Kim, S.-C.,“Morphology and Oxygen Barrier Properties of LDPE/EVOH Blends”, Int. Polym. Proc., 11, 238–247 (1996), DOI:10.3139/217.960238 Search in Google Scholar

López-Rubio, A., Lagaron, J. M., Giménez, E., Cava, D., Hernandez-Muñoz, P., Yamamoto, T. and Gavara, R., “Morphological Alterations Induced by Temperature and Humidity in Ethylene–Vinyl Alcohol Copolymers”, Macromolecules, 36, 9467–9476 (2003), DOI:10.1021/ma035346j Search in Google Scholar

McGonigle, E.-A., Liggat, J. J., Pethrick, R. A., Jenkins, S. D., Daly, J. H. and Hayward, D., “Permeability of N2, Ar, He, O2 and CO2 through Biaxially Oriented Polyester Films–Dependence on Free Volume”, Polymer, 42, 2413–2426 (2001), DOI:10.1016/S0032-3861(00)00615-7 Search in Google Scholar

Morris, B. A.: The Science and Technology of Flexible Packaging: Multilayer Films from Resin and Process to End Use, Elsevier, Boston (2017) Search in Google Scholar

Pazur, R. J., Prud’homme, R. E., “X-Ray Pole Figure and Small Angle Scattering Measurements on Tubular Blown Low-Density Poly (ethylene) Films”, Macromolecules, 29, 119–128 (1996), DOI:10.1021/ma9464229 Search in Google Scholar

Robertson, G. L.: Food Packaging: Principles and Practice, CRC Press, New York (2016) Search in Google Scholar

Sadeghi, F., Ajji, A. and Carreau, P. J.,“Study of Polypropylene Morphology Obtained from Blown and Cast Film Processes: Initial Morphology Requirements for Making Porous Membrane by Stretching”, J. Plast. Film Sheeting, 21, 199–216 (2005), DOI:10.1177/8756087905057085 Search in Google Scholar

Sadeghi, F., Ajji, A. and Carreau, P. J.,“Microporous Membranes Obtained from Polypropylene Blends with Superior Permeability Properties”, J. Polym. Sci. Part B: Polym. Phys., 46, 148–157 (2008), DOI:10.1002/polb.21350 Search in Google Scholar

Shastri, R., Roehrs, H. C., Brown, C. N. and Dollinger, S. E., “Permeability of Competitive Oxygen-Barrier Resins”, in Barrier Polymers and Structures, American Chemical Society, Austin, p. 239– 251 (1990), DOI:10.1021/bk-1990-0423.ch012 Search in Google Scholar

Tabatabaei, S. H., Carreau, P. J. and Ajji, A., “Microporous Membranes Obtained from Polypropylene Blend Films by Stretching”, J. Membr. Sci., 325, 772–782 (2008), DOI:10.1016/j.memsci.2008.09.001 Search in Google Scholar

The Plastics Industry Trade Association: Plastics Packaging Wraps it up, The Plastics Industry Trade Association, Washington (2015) Search in Google Scholar

Weinkauf, D. H., Paul, D. R., “Effects of Structural Order on Barrier Properties”, in Barrier Polymers and Structures, American Chemical Society, Austin, p. 60–91 (1990), DOI:10.1021/bk-1990-0423.ch003 Search in Google Scholar

Yeo, J. H., Lee, C. H., Park, C. S., Lee, K. J., Nam, J. D. and Kim, S. W., “Rheological, Morphological, Mechanical, and Barrier Properties of PP/EVOH Blends”, Adv. Polym. Technol., 20, 191–201 (2001), DOI:10.1002/adv.1015 Search in Google Scholar

Zhang, X., Elkoun, S., Ajji, A. and Huneault, M. A., “Oriented Structure and Anisotropy Properties of Polymer Blown Films: HDPE, LLDPE and LDPE”, Polymer, 45, 217–229 (2004), DOI:10.1016/j.polymer.2003.10.057 Search in Google Scholar

Zhu, Y., Mao, Z. and Gao, C., “Aminolysis-Based Surface Modification of Polyesters for Biomedical Applications”, RSC Adv., 3, 2509–2519 (2013), DOI:10.1039/C2RA22358A Search in Google Scholar

Received: 2020-11-04
Accepted: 2021-03-12
Published Online: 2021-07-07
Published in Print: 2021-07-27

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