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(12) United States Patent (10) Patent No.: US 9,670,344 B2 Favis Et Al

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(12) United States Patent (10) Patent No.: US 9,670,344 B2 Favis Et Al USOO967034.4B2 (12) United States Patent (10) Patent No.: US 9,670,344 B2 Favis et al. (45) Date of Patent: Jun. 6, 2017 (54) POLYMERIC MATERIAL AND PROCESS (56) References Cited FOR RECYCLING PLASTC BLENDS U.S. PATENT DOCUMENTS (71) Applicant: POLYVALOR, LIMITED 6,077.904 A * 6, 2000 Dalgewicz. III ... B29C 49,0005 PARTNERSHIP, Montreal (CA) W algeW1CZ, III .... 524/401 2005, OO381.85 A1* 2, 2005 Sullivan ................... CO8J 3,005 (72) Inventors: Basil D. Favis, Kirkland (CA); Pierre 525,63 Le Corroller, Montreal (CA) 2009 OO18248 A1* 1/2009 Piriri ......................... CO8K9/08 524/425 (73) Assignee: POLYVALOR, LIMITED PARTNERSHIP, Montreal (CA) OTHER PUBLICATIONS (*) Notice: Subject to any disclaimer, the term of this Virgilio et al. Macromolecules, 2009, 42, 7518-7529.* patent is extended or adjusted under 35 Valera et al., Macromolecules 2006, 39, 2663-2675. U.S.C. 154(b) by 0 days. Bhadane, P. A. et al., “Continuity development in polymer blends of very low interfacial tension.” Polymer, vol. 47, pp. 2760-2771, 2006. (21) Appl. No.: 14/360,360 Chen, H. Y., et al., “Olefin Block Copolymers as Polyolefin Blend Compatibilizer.” Antec, 2008. (22) PCT Filed: Nov. 22, 2012 Dai, C. A., et al., “Reinforcement of Polymer Interfaces with Random Copolymers'. The American Physical Society: Physical (86). PCT No.: PCT/CA2O12/050839 Review Letters, vol. 73, No. 18, pp. 2472-2475, 1994. D'Orazio, L., et al., “Effect of Addition of Ethylene-Propylene S 371 (c)(1), Random Copolymers on the Properties of High Density Polyethyl (2) Date: May 23, 2014 ene/Isotactic Polypropylene Blends: Part1. Morphology and Impact Behaviour of Moulded Samples.” Polymer Engineering Science, (87) PCT Pub. No.: WO2013/075241 vol. 22, pp. 536-544, 1982. EPA. U.S Environment Protection Agency, “Municipal Solid Waste PCT Pub. Date: May 30, 2013 Generation, Recycling, and Disposal in the United States: Facts and Figures for 2008.” Washington DC2009. (65) Prior Publication Data Kamdar, A. R. et al., “Effect of Chain Blockiness on the Phase Behavior of Ethylene-Octene Copolymer Blends,” Journal of Physi US 2015/OO31837 A1 Jan. 29, 2015 cal Science part B: Polymer Physics, vol. 47, pp. 1554-1572, 2009. Le Corroller, P. and B. D. Favis, “Droplet-in-Droplet Polymer Blend Related U.S. Application Data Microstructures: a Potential Route Toward the Recycling of Co mingled Plastics', Macromolecule Chemistry and Physics, vol. 213, (60) Provisional application No. 61/563,202, filed on Nov. pp. 2062-2074, 2012. 23, 2011. Lee, M. S., et al., “Can Random Copolymers Serve as Effective Polymeric Compatibilizers?,” Journal of Polymer Science part B. (51) Int. Cl. Polymer Physics, vol. 35, pp. 2835-2842, 1998. COSL23/00 (2006.01) (Continued) COSL 23/2 (2006.01) C08L 23/6 (2006.01) Primary Examiner — Irina Krylova COSL23/04 (2006.01) (74) Attorney, Agent, or Firm — Isabelle Pelletier COSL 2.3/10 (2006.01) C08. II/06 (2006.01) (57) ABSTRACT B29B 9/00 (2006.01) There is provided a polymeric material comprising: a co C83/100 (2006.01) continuous or highly-continuous blend of polyethylene and C08L 23/06 (2006.01) polypropylene, the blend comprising a polyethylene phase B29K IOI/12 (2006.01) and a polypropylene phase separated by a polyethylene? B29K 105/26 (2006.01) polypropylene interface; and one or more thermoplastics (52) U.S. Cl. other than polyethylene and polypropylene, the one or more CPC ................ C08L 23/12 (2013.01); B29B 9/00 thermoplastics each having an interfacial tension with poly (2013.01); C08J 3/005 (2013.01); C08J II/06 propylene higher than the interfacial tension of the polyeth (2013.01); C08L 23/04 (2013.01); C08L 23/06 ylene/polypropylene interface, wherein the one or more (2013.01); C08L 23/10 (2013.01); C08L 23/16 thermoplastics form discrete phases that are encapsulating (2013.01); B29K 2101/12 (2013.01); B29K each other, and wherein said discrete phases are comprised 2105/26 (2013.01); C08.J 2323/06 (2013.01); within the polypropylene phase of the co-continuous or C08.J 2323/10 (2013.01); C08J 2323/12 highly-continuous blend or are located at the polyethylene/ (2013.01); C08J 2423/12 (2013.01); C08.J polypropylene interface. There is also provided a process for 2423/16 (2013.01); C08J 2425/06 (2013.01); recycling a blend of thermoplastics comprising polyethyl C08.J. 2433/12 (2013.01); C08J 2469/00 ene, polypropylene and one or more other thermoplastics, (2013.01); C08L 2205/035 (2013.01); C08L the process comprising the step of melting and mixing the 2207/53 (2013.01); Y02W 30/701 (2015.05) polyethylene, the polypropylene and the one or more other (58) Field of Classification Search thermoplastics, thereby producing a polymeric material. CPC ....................................................... CO8L 23/12 See application file for complete search history. 14 Claims, 4 Drawing Sheets US 9,670,344 B2 Page 2 (56) References Cited Tchomakov, K. R. et al., “Mechanical Properties and Morphology of Ternary PP/EPDM/PE Blends”. The Canadian Journal of Chemical Engineering, vol. 83, pp. 300-309, 2005. OTHER PUBLICATIONS Teh, J. W. and A. Rudin, “A Review of Polyethylene-Polypropylene Lin, Y., et al., “Comparison of Olefin Copolymers as Compatibiliz Blends and Their Compatibilization.” Advances in Polymer Tech ers for Polypropylene and High-Density Polyethylene,” Journal of nology, vol. 13, pp. 1-23, 1994. Applied Polymer Science, vol. 113, pp. 1945-1952, 2009. Virgilio, N., et al., “Novel Self-Assembling Close-Packed Droplet Lyatskaya, Y., et al., “Designing Compatibilizers to Reduce Inter Array at the Interface internary Polymer Blends.” Macromolecules, facial Tension in Polymer Blends'. J. Phys. Chem. (1996), vol. 100, vol. 42, pp. 3405-3416, 2009. pp. 1449-1458. Virgilio, N., et al., “In Situ Measure of Interfacial Tensions in Reignier, J. and B. D. Favis, “Control of the Subinclusion Micro Ternary and Quaternary Immiscible Polymer Blends Demonstrating structure in HDPE/PS/PMMA Ternary Blends.” Macromolecules, Partial Wetting,” Macromolecules, vol. 42, pp. 7518-7529, 2009. vol. 33, pp. 6998-7008, 2000. Wegner, G. and K. Wagemann, “Polymers and the Environment Sarazin, P. and B. D. Favis, “Morphology Control in a Co-continu Current Problems and Future Research,” Advanced Materials, vol. ous Poly(L-lactide)/Polystyrene blend: A Route Toward Highly 6, pp. 629-634, 1994. Structured and Interconnected porosity in Poly(L-lactide) Materi Zhenhua, Y. and B. D. Favis, "Coarsening of Immiscible Co als.” Biomacromolecules, vol. 4, pp. 1669-1679, 2003. Continuous Blends During Quiescent Annealing.” AICHe Journal, Shashoua, Y. "Saving plastics for posterity.” Nature, vol. 455, pp. vol. 51, pp. 271-280, 2005. 288-289, 2008. International Search Report, Feb. 18, 2013. Souza, A. M. C. and N. R. Demarquette, “Influence of coalescence International Preliminary Report on Patentability, Jun. 5, 2014. and Interfacial Tension on the Morphology of PPHDPE compatibilized blends.” Polymer, vol.43, pp. 3959-3967, 2002. * cited by examiner U.S. Patent Jun. 6, 2017 Sheet 1 of 4 US 9,670,344 B2 - i.e. $83. sia as traigia S. 3 i. SS:S 8 : An s :::$3. Sibi : 3 Ei it 3. it is Figure 1 U.S. Patent Jun. 6, 2017 Sheet 2 of 4 US 9,670,344 B2 Figure 2 U.S. Patent Jun. 6, 2017 Sheet 3 of 4 US 9,670,344 B2 Figure 3 U.S. Patent Jun. 6, 2017 Sheet 4 of 4 US 9,670,344 B2 xis is is s Figure 4 US 9,670,344 B2 1. 2 POLYMERIC MATERAL AND PROCESS 1. A polymeric material comprising: FOR RECYCLING PLASTC BLENDS a co-continuous or highly-continuous blend of polyeth ylene and polypropylene, the blend comprising a poly CROSS-REFERENCE TO RELATED ethylene phase and a polypropylene phase separated by APPLICATIONS a polyethylene/polypropylene interface; and one or more thermoplastics other than polyethylene and This application is a National Entry Application of PCT polypropylene, the one or more thermoplastics each application no PCT/CA2012/050839 filed on Nov. 22, 2012 having an interfacial tension with polypropylene higher and published in English under PCT Article 21(2), which than the interfacial tension of the polyethylene/poly itself claims benefit of U.S. provisional application Ser. No. 10 propylene interface, 61/563,202, filed on Nov. 23, 2011. All documents above are wherein the one or more thermoplastics form discrete incorporated herein in their entirety by reference. phases that are encapsulating each other, and FIELD OF THE INVENTION wherein said discrete phases are comprised within the polypropylene phase of the co-continuous or highly The present invention relates to a process for recycling 15 continuous blend or are located at the polyethylene/ blends of plastics and to a new polymeric material having a polypropylene interface. microstructure where one or more thermoplastics are serially 2. The polymeric material of item 1, wherein the polyeth encapsulated in one phase of a biphasic polymeric blend. ylene/polypropylene interface is compatibilized by an Also, the present invention is concerned with this polymeric interfacial agent and said discrete phases are comprised material when it is produced by the process for recycling within the polypropylene phase of the co-continuous or blends of plastics. highly-continuous blend. 3. The polymeric material of item 2, wherein the interfacial CONTEXT OF THE INVENTION agent is an ethylene-propylene-diene elastomer or a ran domethylene-propylene copolymer. Nowadays, the worldwide plastic production is 230 mil lion tonnes and global sales exceed 300 billion dollars 25 4. The polymeric material of item 3, wherein the interfacial annually. Polyolefins, styrenic resins, PET and PVC repre agent is an unvulcanized random ethylene-propylene sent 90% of the consumer waste plastic stream. In the US diene elastomer. alone, non recyclable PS, PVC and engineering resins 5.
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