The compatibilization of PLA-g-TPU graft copolymer on polylactide/thermoplastic polyurethane blends

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The insufficient compatibility between poly(lactic acid) (PLA) and thermoplastic polyurethane (TPU) phase leads to some disadvantages such as extrudate swell and poor mechanical properties of PLA/TPU blends. Therefore, to improve the compatibility is an essential work of modifying the blends. In this study, PLA, dicumyl peroxide (DCP), glycidyl methacrylate (GMA) and TPU were added to torque rheometer in sequence to synthesize PLA-g-TPU graft copolymer, and the synthetic products were characterized by nuclear magnetic resonance (NMR) spectroscopy and Fourier transform infrared (FTIR) spectra. Subsequently, binary blends (PLA /TPU blends) and ternary blends (PLA/TPU/PLA-g-TPU blends) were prepared via melt blending in twin screw extruder. The compatibility, the extrusion behavior, thermal stabilities and mechanical properties of binary blends and ternary blends were studied, respectively. The results showed that the graft copolymer played a crucial role in improving the compatibility of PLA/TPU blends. In comparison to binary blends, the ternary blends exhibited better extrusion behavior and higher thermal stabilities. In addition, the notched impact strength and elongation at break of blends improved under the effect of the graft copolymer. Interestingly, the tensile strength also strengthened with incorporation of the graft copolymer, which indicated that the interfacial adhesion between PLA phase and TPU phase had been enhanced.

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  1. 1.

    Ata S, Basak S, Mal D et al (2017) Synthesis and self-assembly behavior of POSS tethered amphiphilic polymer based on poly(caprolactone) (PCL) grafted with poly(acrylic acid) (PAA) via ROP, ATRP, and CuAAC reaction. J Polym Res 24(2):19

  2. 2.

    Li CT, Zhang M, Weng YX et al (2018) Influence of ether bond on degradation property of PBS-based copolymers at molecular level using molecular simulations. J Polym Res 25(7):161

  3. 3.

    Woo HJ, Chiam-Wen L, Majid SR, Arof AK (2014) Poly(ε-caprolactone)-based polymer electrolyte for electrical double-layer capacitors. High perform polym 26(6):637–640

  4. 4.

    Lin L, Deng C, Lin G, Wang Y (2015) Super toughened and high heat-resistant poly(lactic acid) (PLA)-based blends by enhancing interfacial bonding and PLA phase crystallization. Ind Eng Chem Res 54(21):5643–5655

  5. 5.

    Ji LJ, Gong MD, Qiao W et al (2018) A gelatin/PLA-b-PEG film of excellent gas barrier and mechanical properties. J Polym Res 25:10

  6. 6.

    Meng X, Nguyen NA, Tekinalp H, Lara-Curzio E, Ozcan S (2017) Supertough PLA-Silane Nanohybrids by in situ condensation and grafting. ACS sustainable Chem Eng: 7b03650

  7. 7.

    Yang X, Clénet J, Xu H, Odelius K, Hakkarainen M (2015) Two step extrusion process: from thermal recycling of PHB to plasticized PLA by reactive extrusion grafting of PHB degradation products onto PLA chains. Macromolecules 48(8):2509–2518

  8. 8.

    Wu N, Zhang H, Fu G (2017) Super-tough poly(lactide) thermoplastic Vulcanizates based on modified natural rubber. ACS Sustain Chem Eng 5(1):78–84

  9. 9.

    Oliaei E, Kaffashi B, Davoodi S (2016) Investigation of structure and mechanical properties of toughened poly(l-lactide)/thermoplastic poly(ester urethane) blends. J Appl Polym Sci 133(15):43104

  10. 10.

    Li Y, Shimizu H (2007) Toughening of polylactide by melt blending with a biodegradable poly(ether)urethane elastomer. Macromol Biosci 7(7):921–928

  11. 11.

    Zheng X, Zhang C, Luo C, Tian G, Wang L, Li Y (2016) TPU inclusion complex modified POM: fabrication of high performance POM composites with both excellent stiffness–toughness balance and Thermostability. Ind Eng Chem Res:5b04544

  12. 12.

    Lai SM, Wu WL, Wang YJ (2016) Annealing effect on the shape memory properties of polylactic acid (PLA)/thermoplastic polyurethane (TPU) bio-based blends. J Polym Res 23(5):99

  13. 13.

    Lai SM, You PY, Yu TC et al (2017) Triple-shape memory properties of thermoplastic polyurethane/olefin block copolymer/polycaprolactone blends. J Polym Res 24(10):161

  14. 14.

    Dogan SK, Reyes EA, Rastogi S, Ozkoc G (2014) Reactive compatibilization of PLA/TPU blends with a diisocyanate. J Appl Polym Sci 131(10):n/a-n/a

  15. 15.

    Reulier M, Avérous L (2015) Elaboration, morphology and properties of renewable thermoplastics blends, based on polyamide and polyurethane synthesized from dimer fatty acids. Eur Polym J 67:418–427

  16. 16.

    Hong H, Wei J, Yuan Y, Chen FP, Wang J, Qu X, Liu CS (2011) A novel composite coupled hardness with flexibleness—polylactic acid toughen with thermoplastic polyurethane. J Appl Polym Sci 121(2):855–861

  17. 17.

    Han JJ, Huang HX (2011) Preparation and characterization of biodegradable polylactide/thermoplastic polyurethane elastomer blends. J Appl Polym Sci 120(6):3217–3223

  18. 18.

    Jonoobi M, Harun J, Mathew AP et al (2010) Mechanical properties of cellulose nanofiber (CNF) reinforced polylactic acid (PLA) prepared by twin screw extrusion. Compos Sci Technol 70(12):1742–1747

  19. 19.

    Torres J, Cotelo J, Karl J et al (2015) Mechanical property optimization of FDM PLA in shear with multiple objectives. JOM 67(5):1183–1193

  20. 20.

    Afrose MF, Masood SH, Iovenitti P et al (2016) Effects of part build orientations on fatigue behaviour of FDM-processed PLA material. Progress in Additive Manufacturing 1(1–2):21–28

  21. 21.

    Afrose MF, Masood SH, Nikzad M et al (2014) Effects of build orientations on tensile properties of PLA material processed by FDM. Adv Mater Res 1044-1045:31–34

  22. 22.

    Zhansitov Azamat A, Khashirova Svetlana Y et al (2017) Development of technology of polysulfone production for 3D printing. High perform polym 29(6):724–729

  23. 23.

    Feng F, Ye L (2011) Morphologies and mechanical properties of polylactide/thermoplastic polyurethane elastomer blends. J Appl Polym Sci 119(5):2778–2783

  24. 24.

    Bher A, Auras R, Schvezov CE (2018) Improving the toughening in poly(lactic acid)-thermoplastic cassava starch reactive blends MDI. Appl Polym Sci 135:46140

  25. 25.

    Zhao F, Huang HX, Zhang SD (2015) Largely toughening biodegradable poly(lactic acid)/thermoplastic polyurethane blends by adding MDI. Appl Polym Sci 132(48):42511

  26. 26.

    Zhao X, Ding Z, Lin Q, Peng S, Fang P (2017) Toughening of polylactide viain situ formation of polyurethane crosslinked elastomer during reactive blending. J Appl Polym Sci 134(2):44383

  27. 27.

    Ji DY, Liu ZY, Lan XR et al (2012) Study on the crystallization behavior of PLA/PBS/DCP reactive blends. Acta Polym Sin 012:694–697

  28. 28.

    Zhao Z, Yang Q, Coates P, Whiteside B, Kelly A, Huang Y, Wu P (2018) Structure and property of microinjection molded poly(lactic acid) with high degree of long chain branching. Ind Eng Chem Res 57:11312–11322

  29. 29.

    Liu W, Liu T, Liu T, Liu T, Xin J, Hiscox WC, Liu H, Liu L, Zhang J (2017) Improving grafting efficiency of Dicarboxylic anhydride monomer on Polylactic acid by manipulating monomer structure and using Comonomer and reducing agent. Ind Eng Chem Res 56(14):3920–3927

  30. 30.

    Liu J, Jiang H, Chen L (2012) Grafting of Glycidyl methacrylate onto poly(lactide) and properties of PLA/starch blends Compatibilized by the grafted copolymer. J Polym Environ 20(3):810–816

  31. 31.

    Guo R, Ren Z, Bi H, Song Y, Xu M (2018) Effect of toughening agents on the properties of poplar wood flour/poly (lactic acid) composites fabricated with fused deposition modeling. Eur Polym J 107:34–45

  32. 32.

    Dong W, Wang H, He M, Ren F, Wu T, Zheng Q, Li Y (2015) Synthesis of reactive comb polymers and their applications as a highly efficient Compatibilizer in immiscible polymer blends. Ind Eng Chem Res 54(7):2081–2089

  33. 33.

    Fischer EW, Sterzel HJ, Wegner G (1973) Investigation of the structure of solution grown crystals of lactide c opolymers by means of chemical reactions. Kolloid-Z U Z Polymere 251(11):980–990

  34. 34.

    Holland-Moritz K, Siesler HW (1981) Characterization of deformation phenomena in polymers by rapid-scanning fourier transform IR (FTIR) spectroscopy and mechanical measurements: 4. Uniaxial deformation of amorphous poly(butylene terephthalate). Polym Bull 4(3):165–170

  35. 35.

    Liu RYF, Bernal-Lara TE, Hiltner A (2005) Baer E. polymer interphase materials by forced assembly. Macromolecules 38(11):4819–4827

  36. 36.

    Kratochvíl J, Kelnar I (2017) Non-isothermal kinetics of cold crystallization in multicomponent PLA/thermoplastic polyurethane/nanofiller system. Journal of Thermal Analysis & Calorimetry 130(2):1–10

  37. 37.

    Magalhaes AML, Borggreve RJM (1995) Contribution of the crazing process to the toughness of rubber-modified polystyrene. Macromolecules 28(17):5841–5851

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Correspondence to Xian-Zhong Mo.

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Mo, X., Wei, F., Tan, D. et al. The compatibilization of PLA-g-TPU graft copolymer on polylactide/thermoplastic polyurethane blends. J Polym Res 27, 33 (2020).

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  • PLA
  • TPU
  • GMA
  • PLA-g-GMA
  • PLA-g-TPU
  • Compatibility