journal article·2021-03-27Open access

Cold Crystallization Kinetics and Thermal Degradation of PLA Composites with Metal Oxide Nanofillers

Evangelia Tarani, Klementina Pušnik Črešnar, Lidija Fras Zemljič, Konstantinos Chrissafis, George Z. Papageorgiou, Dimitra Lambropoulou, Alexandra Zamboulis, Dimitrios N. Bikiaris, Zoi Terzopoulou

Applied Sciences· Volume 11· Issue 7

Abstract

Poly(lactic acid) (PLA) nanocomposites with antimicrobial fillers have been increasingly explored as food packaging materials that are made of a biobased matrix and can minimize food loss due to spoilage. Some of the most commonly studied fillers are zinc oxide (ZnO), titanium dioxide (TiO2), and silver nanoparticles (AgNPs). In this work, nanocomposites with 1 wt.% of each filler were prepared by melt mixing. An extensive study of thermally stimulated processes such as crystallization, nucleation, degradation, and their kinetics was carried out using Differential Scanning Calorimetry (DSC) and Thermogravimetric Analysis (TGA). In detail, non-isothermal cold crystallization studies were performed with DSC and polarized light microscopy (PLM), and kinetics were analyzed with multiple equations. The activation energy of the non-isothermal cold crystallization was calculated with the methods of Kissinger and Friedman. The latter was used to also determine the Hoffman–Lauritzen parameters (Kg and U*) by applying the Vyazovkin method. Additionally, effective activation energy and kinetic parameters of the thermal decomposition process were determined by applying the isoconversional differential method and multivariate non-linear regression method. According to TGA results, metal oxide nanofillers affected the thermal stability of PLA and caused a decrease in the activation energy values. Moreover, the fillers acted as heterogenous nucleating agents, accelerating the non-isothermal crystallization of PLA, thus reducing its activation energy. It can be concluded that metal oxide nanofillers catalytically affect the thermal degradation and crystallization of PLA samples.
Source: crossref · Quality: baseline

Research context

OpenAlex topics: biodegradable polymer synthesis and properties · Microplastics and Plastic Pollution · Polymer crystallization and properties

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Department of Physics, Aristotle University of Thessaloniki, GR54124 Thessaloniki, Greece

Faculty of Mechanical Engineering, University of Maribor, 2000 Maribor, Slovenia

Department of Chemistry, University of Ioannina, P.O. Box 1186, GR45110 Ioannina, Greece

Laboratory of Environmental Pollution Control, Department of Chemistry, Aristotle University of Thessaloniki, GR54124 Thessaloniki, Greece

Laboratory of Chemistry and Technology of Polymers and Dyes, Department of Chemistry, Aristotle University of Thessaloniki, GR54124 Thessaloniki, Greece

References (83)

Show source-provided references
1. European Bioplastics e.V (2021, February 10). (EUBP), Bioplastics Market Development Update 2020. Available online: https://www.european-bioplastics.org/news/publications/#MarketData.
2. The development and challenges of poly (lactic acid) and poly (glycolic acid)
3. Biobased Building Blocks and Polymers—Global Capacities, Production and Trends, 2018–202310.1089/ind.2019.29179.rch ↗
4. Physical and mechanical properties of PLA, and their functions in widespread applications—A comprehensive review10.1016/j.addr.2016.06.012 ↗
5. Additive manufacturing (3D printing): A review of materials, methods, applications and challenges10.1016/j.compositesb.2018.02.012 ↗
6. Banerjee, R., and Ray, S.S. (2021). An overview of the recent advances in polylactide-based sustainable nanocomposites. Polym. Eng. Sci.10.1002/pen.25623 ↗
7. Effect of rigid nanoparticles and preparation techniques on the performances of poly(lactic acid) nanocomposites: A review10.1002/pat.5104 ↗
8. Rigid amorphous fraction and segmental dynamics in nanocomposites based on poly(L–lactic acid) and nano-inclusions of 1–3D geometry studied by thermal and dielectric techniques10.1016/j.eurpolymj.2016.07.002 ↗
9. Glass transition and segmental dynamics in poly(l-lactic acid)/graphene oxide nanocomposites10.1016/j.tca.2015.08.020 ↗
10. In situ prepared poly(DL-lactic acid)/silica nanocomposites: Study of molecular composition, thermal stability, glass transition and molecular dynamics10.1016/j.tca.2018.08.025 ↗
11. Rational design of two-dimensional nanofillers for polymer nanocomposites toward multifunctional applications10.1016/j.pmatsci.2020.100708 ↗
12. Biodegradable polymers and green-based antimicrobial packaging materials: A mini-review
13. Sarfraz, J., Gulin-Sarfraz, T., Nilsen-Nygaard, J., and Pettersen, M.K. (2021). Nanocomposites for food packaging applications: An overview. Nanomaterials, 11.10.3390/nano11010010 ↗
14. Metal oxide-based nanocomposites in food packaging: Applications, migration, and regulations10.1016/j.tifs.2018.09.021 ↗
15. Liao, C., Li, Y., and Tjong, S.C. (2019). Antibacterial activities of aliphatic polyester nanocomposites with silver nanoparticles and/or graphene oxide sheets. Nanomaterials, 9.10.3390/nano9081102 ↗
16. Nanocomposites for food packaging applications10.1016/j.foodres.2009.03.019 ↗
17. ZnO-PLA nanocomposite coated paper for antimicrobial packaging application10.1016/j.lwt.2016.12.024 ↗
18. Incorporation of zinc oxide nanoparticles improved the mechanical, water vapor barrier, UV-light barrier, and antibacterial properties of PLA-based nanocomposite films10.1016/j.msec.2018.08.002 ↗
19. González, E.A.S., Olmos, D., Lorente, M.Á., Vélaz, I., and González-Benito, J. (2018). Preparation and characterization of polymer composite materials based on PLA/TiO2 for antibacterial packaging. Polymers, 10.10.3390/polym10121365 ↗
20. PLA-ZnO nanocomposite films: Water vapor barrier properties and specific end-use characteristics10.1016/j.eurpolymj.2013.08.005 ↗
21. Poly(lactic acid)/graphene oxide-ZnO nanocomposite films with good mechanical, dynamic mechanical, anti-UV and antibacterial properties10.1002/jctb.4476 ↗
22. Chu, Z., Zhao, T., Li, L., Fan, J., and Qin, Y. (2017). Characterization of antimicrobial poly (lactic acid)/nano-composite films with silver and zinc oxide nanoparticles. Materials, 10.10.3390/ma10060659 ↗
23. Antimicrobial activity of poly(l-lactide acid)/silver nanocomposite fibers10.1177/0040517513481875 ↗
24. ZnO deposited/encapsulated halloysite-poly (lactic acid) (PLA) nanocomposites for high performance packaging films with improved mechanical and antimicrobial properties10.1016/j.clay.2015.03.024 ↗
25. Sirotkin, N.A., Gurina, D.L., Khlyustova, A.V., Costerin, D.Y., Naumova, I.K., Titov, V.A., and Agafonov, A.V. (2020). Experimental and computational investigation of polylactic acid/silver-NP nanocomposite with antimicrobial activity prepared by plasma in liquid. Plasma Process. Polym.10.1002/ppap.202000169 ↗
26. Catalytic effect of nanosized ZnO and TiO2 on thermal degradation of poly(lactic acid) and isoconversional kinetic analysis10.1016/j.tca.2018.12.008 ↗
27. Synergistic Effect of Talc and Titanium Dioxide on Poly(lactic acid) Crystallization: An Investigation on the Injection Molding Cycle Time Reduction10.1007/s10924-019-01396-0 ↗
28. Use of chemically modified titanium dioxide particles to mediate the non-isothermal cold crystallization of poly(latic acid)
29. Nomai, J., Suksut, B., and Karl Schlarb, A. (2015). Crystallization Behavior of Poly(lactic acid)/Titanium Dioxide Nanocomposites. KMUTNB Int. J. Appl. Sci. Technol., 1–8.10.14416/j.ijast.2015.10.003 ↗
30. Influence of TiO2 Nanoparticles on the Crystallization Behaviour and Tensile Properties of Biodegradable PLA and PCL Nanocomposites10.1007/s10924-017-1142-y ↗
31. Effect of ZnO nanofillers treated with triethoxy caprylylsilane on the isothermal and non-isothermal crystallization of poly(lactic acid)10.1039/c2cp41574g ↗
32. Poly(lactic acid) crystallization10.1016/j.progpolymsci.2012.07.005 ↗
33. (1970, January 01). NatureWorks, Crystallizing and Drying of PLA, Tech. Resour. Available online: http://www.natureworksllc.com/Technical-Resources/4-Series.aspx.
34. Magnetically recoverable photocatalytic nanocomposite particles for water treatment10.1016/j.matchemphys.2011.03.059 ↗
35. ICTAC Kinetics Committee recommendations for performing kinetic computations on thermal analysis data10.1016/j.tca.2011.03.034 ↗
36. (2021, February 18). Kinetics Neo; How Fast Are Your Chemical Reactions?. Available online: https://kinetics.netzsch.com/en/.
37. Crystallization behavior of poly(lactic acid) filled with modified carbon black10.1080/00222340902837238 ↗
38. Microstructure and nonisothermal cold crystallization of PLA composites based on silver nanoparticles and nanocrystalline cellulose10.1016/j.polymdegradstab.2012.03.027 ↗
39. Effect of polymers on nucleation and crystal growth of amorphous acetaminophen10.1039/c2ce25374g ↗
40. Evaluation of the formed interface in biodegradable poly(l-lactic acid)/graphene oxide nanocomposites and the effect of nanofillers on mechanical and thermal properties10.1016/j.tca.2014.10.007 ↗
41. The synergistic effect of zinc oxide and phenylphosphonic acid zinc salt on the crystallization behavior of poly (lactic acid)10.1016/j.polymdegradstab.2015.10.014 ↗
42. Non-isothermal cold crystallization kinetics of poly(3-hydoxybutyrate) filled with zinc oxide10.1016/j.tca.2016.06.002 ↗
43. Kinetics of non-isothermal crystallization10.1016/0032-3861(71)90041-3 ↗
44. Nonisothermal crystallization of polymers: Getting more out of kinetic analysis of differential scanning calorimetry data
45. Nonisothermal crystallization kinetics of poly(lactic acid) formulations comprising talc with poly(ethylene glycol)10.1002/pen.21755 ↗
46. Isothermal and non-isothermal crystallization kinetics of PLA/PBS blends with talc as nucleating agent10.1007/s10973-019-08631-9 ↗
47. Isothermal and nonisothermal cold crystallization kinetics of poly(l-lactide)/functionalized eggshell powder composites10.1007/s10973-017-6783-5 ↗
48. An investigation of PLA/Babassu cold crystallization kinetics10.1007/s10973-019-09062-2 ↗
49. Nonisothermal cold crystallization behavior and kinetics of polylactide/clay nanocomposites10.1002/polb.21154 ↗
50. Isothermal melt and cold crystallization kinetics of poly(aryl ether ether ketone ketone) (PEEKK)10.1016/S0014-3057(97)00016-5 ↗
51. Nonisothermal crystallization kinetics of poly (ethylene terephthalate)/clay nanocomposites prepared by melt processing10.1002/pc.20892 ↗
52. Non-isothermal crystallization kinetics of syndiotactic polystyrene–polystyrene functionalized SWNTs nanocomposites
53. Homer Kissinger and the Kissinger equation10.1016/j.tca.2012.04.008 ↗
54. On the Kissinger equation and the estimate of activation energies for non-isothermal cold crystallization of PET10.1016/j.polymertesting.2014.08.008 ↗
55. Vyazovkin, S. (2020). Kissinger Method in Kinetics of Materials: Things to Beware and Be Aware of. Molecules, 25.10.3390/molecules25122813 ↗
56. Non-isothermal crystallization kinetics of ramie fiber-reinforced polylactic acid biocomposite10.1039/C7RA09418C ↗
57. Kinetics of thermal degradation of char-forming plastics from thermogravimetry. Application to a phenolic plastic10.1002/polc.5070060121 ↗
58. Vyazovkin, S. (2020). Activation energies and temperature dependencies of the rates of crystallization and melting of polymers. Polymers, 12.10.3390/polym12051070 ↗
59. Nonisothermal crystallization kinetics of PLA/nanosized YVO4 composites as a novel nucleating agent10.1002/app.48340 ↗
60. Crystallization and enzymatic hydrolysis of PLA grade for orthopedics10.1002/adv.20194 ↗
61. Kinetic modelling of thermal degradation and non-isothermal crystallization of silk nano-discs reinforced poly (lactic acid) bionanocomposites10.1007/s00289-018-2434-7 ↗
62. Crystallization behavior of biodegradable poly (L-lactide)/multiwalled carbon nanotubes nanocomposites from the amorphous state10.1002/pen.21933 ↗
63. Crystallization of poly (butylene succinate) on rapid cooling and heating: Toward enhanced nucleation by graphene nanosheets10.1021/acs.jpcc.7b02887 ↗
64. Effect of molecular weight on the cold-crystallization of biodegradable poly (ethylene succinate)10.1016/j.tca.2007.03.002 ↗
65. Melt and glass crystallization of PDMS and PDMS silica nanocomposites10.1039/C4CP00164H ↗
66. Isoconversional Approach to Evaluating the Hoffman–Lauritzen Parameters (U* and Kg) from the Overall Rates of Nonisothermal Crystallization10.1002/marc.200300295 ↗
67. Isoconversional Kinetic Analysis of Thermally Stimulated Processes in Polymers10.1002/marc.200600404 ↗
68. Thermal properties and cold crystallization kinetics of surface-treated banana fiber (BF)-reinforced poly (lactic acid)(PLA) nanocomposites10.1007/s10973-013-3102-7 ↗
69. Crystallization behavior of vetiver grass fiber-polylactic acid composite10.4028/www.scientific.net/AMR.410.55 ↗
70. Isothermal crystallization behavior of hybrid biocomposite consisting of regenerated cellulose fiber, clay, and poly(lactic acid)10.1002/app.26853 ↗
71. Non-isothermal Crystallization Kinetics of Biobased Poly(ethylene 2,5-furandicarboxylate) Synthesized via the Direct Esterification Process10.1002/macp.201400316 ↗
72. PLA nanocomposites: Effect of filler type on non-isothermal crystallization10.1016/j.tca.2010.08.004 ↗
73. Non-isothermal crystallization kinetics from the melt of nanocomposites based on poly(3-hydroxybutyrate) and modified clays10.1016/j.tca.2014.08.023 ↗
74. Tarani, E., Papageorgiou, G.Z., Bikiaris, D.N., and Chrissafis, K. (2019). Kinetics of crystallization and thermal degradation of an isotactic polypropylene matrix reinforced with graphene/glass-fiber filler. Molecules, 24.10.3390/molecules24101984 ↗
75. Activity of substrates in the catalyzed nucleation of glass-forming melts. II. Experimental evidence10.1016/0022-3093(93)90737-I ↗
76. Activity of substrates in the catalyzed nucleation of glass-forming melts. I. Theory10.1016/0022-3093(93)90736-H ↗
77. Non-isothermal crystallization behaviors and spherulitic morphology of poly(lactic acid) nucleated by a novel nucleating agent10.1007/s10973-015-4677-y ↗
78. Effect of surface functionalization of halloysite nanotubes on synthesis and thermal properties of poly(ε-caprolactone)10.1007/s10853-018-1993-1 ↗
79. Terzopoulou, Z., Tarani, E., Kasmi, N., Papadopoulos, L., Chrissafis, K., Papageorgiou, D.G., Papageorgiou, G.Z., and Bikiaris, D.N. (2019). Thermal decomposition kinetics and mechanism of in-situ prepared bio-based poly(propylene 2,5-furan dicarboxylate)/graphene nanocomposites. Molecules, 24.10.3390/molecules24091717 ↗
80. A New Method of Analyzing Thermogravimetric Data10.1246/bcsj.38.1881 ↗
81. Thermal conductivity and degradation behavior of HDPE/graphene nanocomposites: Pyrolysis, kinetics and mechanism10.1007/s10973-017-6342-0 ↗
82. Detail kinetic analysis of the thermal decomposition of PLA with oxidized multi-walled carbon nanotubes10.1016/j.tca.2010.08.009 ↗
83. Thermal degradation of poly(lactic acid) measured by thermogravimetry coupled to Fourier transform infrared spectroscopy10.1007/s10973-009-0121-5 ↗