Separation and Reuse of Multilayer Food Packaging in Cellulose Reinforced Polyethylene Composites


The recycling of multilayer packaging is hindered by the problematic separation of the packaging components. Among the numerous multilayer packaging, the ubiquitous 5-layer polyethylene/cardboard/polyethylene/aluminum/polyethylene one is one of the most difficult to recycle. This work examines how the synthetic polymer, cellulose and aluminum components can first be efficiently separated and secondly, how the recovered cellulose and polyethylene can be mixed to produce value-added composites. Size reduction and hydro-mechanical treatment of the packaging enabled the separation of cellulose from the PE and dual PE/aluminum layer. The delamination of the PE from the aluminum required a chemical treatment in an organic acid followed by separation by flotation/sedimentation. Instead of reusing the cellulose directly into a composite, the fibers were fractionated in order to produce fermentable sugars for a bio-refining operation and to recover value-added side-products known as microcrystalline cellulose (MCC). Thus, through the reaction with concentrated sulfuric acid, the recovered cellulose was decrystallized and partially hydrolyzed. It was then precipitated in a non-protic polar anti-solvent, and hydrolyzed in dilute sulfuric acid solution to generate MCC. This MCC was incorporated at levels up to 50 wt% into the recovered polyethylene using a twin-screw extrusion mixing process and then injection-molded. The elastic modulus and tensile strength increased linearly with the MCC content. A polyethylene grafted with maleic anhydride was added as a coupling agent between MCC and polyethylene during the compounding stage to further improve the composite properties. The composites were more homogeneous and the modulus and tensile strength were increased by around 20 % in presence of the coupling agent. Micrographs on rupture surfaces corroborated the improvement of cellulose wettability and interfacial adhesion in presence of the coupling agent.

Graphical Abstract

This is a preview of subscription content, log in to check access.

Fig. 1
Fig. 2
Fig. 3
Fig. 4
Fig. 5
Fig. 6
Fig. 7
Fig. 8


  1. 1.

    Lopes, C.M.A., Felisberti, M.I.: Composite of low-density polyethylene and aluminum obtained from the recycling of postconsumer aseptic packaging. J. Appl. Polym. Sci. 101, 3183–3191 (2006)

    Article  Google Scholar 

  2. 2.

    Korkmaz, A., Yanik, J., Brebu, M., Vasile, C.: Pyrolysis of tetra pack. Waste Manag. 29, 2836–2841 (2009)

    Article  Google Scholar 

  3. 3.

    Tetra Paka. Recycling and recovery a hands-on approach (2014). Last visited 15 Feb 2015

  4. 4.

    Shiba, K., Yano, T., Yamada, M., Yoshino, T.: Packaging material. United States Patent, US 8637152 B2, pp. 1–9 (2014)

  5. 5.

    Olafsson, G., Jägerstad, M., Öste, R., Wessllén, B.: Delamination of polyethylene and aluminum foil layers of laminated packaging material by acetic acid. J. Food Sci. 58(1), 215–219 (1993)

    Article  Google Scholar 

  6. 6.

    Ashutosh, M.: A process of delamination of multi-layer laminated packaging industrial refuse. European Patent Specification, EP 1 352 024 B1, pp. 1–7 (2003)

  7. 7.

    Hidalgo-Salazar, M.A., Mina, J.H., Herena-Franco, P.J.: The effect of interfacial adhesion on the creep behavior of LDPE–Al–Fique composite materials. Compos. B 55, 345–351 (2013)

    Article  Google Scholar 

  8. 8.

    El-Sakhawy, M., Hassan, M.L.: Physical and mechanical properties of microcrystalline cellulose prepared from agricultural residues. Carbohydr. Polym. 67, 1–10 (2007)

    Article  Google Scholar 

  9. 9.

    Nelson, M.L., O’Connor, R.T.: Relation of certain infrared bands to cellulose crystallinity and crystal lattice type. Part I. Spectra of lattice types I, II, III and of amorphous cellulose. J. Appl. Polym. Sci. 8, 1311–1324 (1964)

    Article  Google Scholar 

  10. 10.

    Ambjörnsson, H.A.: Mercerization and Enzymatic Pretreatment of Cellulose in Dissolving Pulps. Doctoral dissertation, Karlstad University, Sweden (2013)

  11. 11.

    Muhammad, N., Man, Z., Khalil, M.A.B., Tan, I.M., Maitra, S.: Studies on the thermal degradation behavior of ionic liquid regenerated cellulose. Waste Biomass Valoriz. 1, 315–321 (2010)

    Article  Google Scholar 

  12. 12.

    Kumar, S.: Hydrothermal Treatment for Biofuels: Lignocellulosic Biomass to Bioethanol, Biocrude, and Biochar. Doctoral Dissertation. Auburn University (2010)

  13. 13.

    Ago, M., Endo, T., Hirotsu, T.: Crystalline transformation of native cellulose from cellulose I to cellulose II polymorph by a ball-milling method with a specific amount of water. Cellulose 11, 164–168 (2004)

    Article  Google Scholar 

  14. 14.

    Yue, Y., Han, G., Wu, Q., Yiying, Y.: Transitional properties of cotton fibers from cellulose I to cellulose II structure. BioResources 8(4), 6460–6471 (2013)

    Article  Google Scholar 

  15. 15.

    Abbott, A., Bismarck, A.: Self-reinforced cellulose nanocomposites. Cellulose 17, 779–791 (2010)

    Article  Google Scholar 

  16. 16.

    Yue, Y.: A Comparative Study of Cellulose I and II Fibers and Nanocrystals. Master Dissertation. Heilongjiang Institute of Science and Technology, P. R. China (2010)

  17. 17.

    Lu, J.Z., Negulescu, I., Wu, Q.: Maleated wood-fiber/high-density-polyethylene composites: coupling mechanisms and interfacial characterization. Compos. Interface 12(1–2), 125–140 (2005)

    Article  Google Scholar 

  18. 18.

    Haafiz, M.K.M., Eichhorn, S.J., Hassan, A., Jawaid, M.: Isolation and characterization of microcrystalline cellulose from oil palm biomass residue. Carbohydr. Polym. 93, 628–634 (2013)

    Article  Google Scholar 

Download references


The authors would like to acknowledge the support of BiofuelNet Canada and of the Industrial Research Chair on Cellulosic Ethanol and Biocommodities of the Université de Sherbrooke. The Chair is financially supported by CRB Innovations, Enerkem and Ethanol Greenfield Québec Inc., as well as by the Ministère de l’énergie et des ressources naturelles du Québec.

Author information



Corresponding author

Correspondence to Michel A. Huneault.

Rights and permissions

Reprints and Permissions

About this article

Verify currency and authenticity via CrossMark

Cite this article

Diop, C.I.K., Lavoie, J. & Huneault, M.A. Separation and Reuse of Multilayer Food Packaging in Cellulose Reinforced Polyethylene Composites. Waste Biomass Valor 8, 85–93 (2017).

Download citation


  • Multilayer packaging
  • Cardboard
  • Polyethylene
  • Recycling
  • Microcrystalline cellulose
  • Composites