Abstract
Poly(glycolic acid) (PGA) is derived from glycolide obtained by fermenting pineapples or sugarcane, which has excellent gas barrier properties and a small carbon footprint. PGA is a potential substitute for the current aluminum-plastic composite films used in high barrier packaging applications. However, its poor ductility and narrow processing window limit its application in food packaging. Herein, poly(butylene succinate-co-butylene adipate) (PBSA) was used to fabricate PGA/PBSA blend films through an in situ fibrillation technique and blown film extrusion. Under the elongational flow field used during the extrusion process, a unique hierarchical structure based on the PBSA nanofibrils and interfacially oriented PGA crystals was obtained. This structure enhances the strength, ductility and gas barrier properties of the PGA/PBSA blend film. In addition, an epoxy chain extender (ADR4468) was used as a compatibilizer to further enhance the interfacial adhesion between PGA and PBSA. 70PGA/0.7ADR exhibited a very low oxygen permeability (2.34×10−4 Barrer) with significantly high elongating at break (604.4%), tensile strength (47.4 MPa), and transparency, which were superior to those of petroleum-based polymers. Thus, the 70PGA/0.7ADR blown films could satisfy the requirements for most instant foods such as coffee, peanuts, and fresh meat.
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References
Hudson, M. J.; Aoyama, M.; Hoover, K. C.; Uchiyama, J. Prospects and challenges for an archaeology of global climate change. Wiley Interdiscip. Rev. Clim. Change 2012, 3, 313–328.
Zhao, X.; Ma, X.; Chen, B.; Shang, Y.; Song, M. Challenges toward carbon neutrality in China: strategies and countermeasures. Resour. Conserv. Recycl. 2022, 176, 105959.
Okura, M.; Takahashi, S.; Kobayashi, T.; Saijo, H.; Takahashi, T. In Improvement of impact strength of polyglycolic acid for self-degradable tools for low-temperature wells, SPE Middle East Unconventional Resources Conference and Exhibition, OnePetro: 2015.
Yamane, K.; Sato, H.; Ichikawa, Y.; Sunagawa, K.; Shigaki, Y. Development of an industrial production technology for high-molecular-weight polyglycolic acid. Polym. J. 2014, 46, 769–775.
Valderrama, M. A. M.; van Putten, R. J.; Gruter, G. J. M. The potential of oxalic-and glycolic acid based polyesters (review). Towards CO2 as a feedstock (Carbon Capture and Utilization-CCU). Eur. Polym. J. 2019, 119, 445–468.
Li, J. X.; Niu, D. Y.; Xu, P. W.; Sun, Z. Y.; Yang, W. J.; Ji, Y.; Ma, P. M. Tailoring the crystallization behavior and mechanical property of poly(glycolic acid) by self-nucleation. Chinese J. Polym. Sci. 2022, 40, 365–372.
Xu, P.; Tan, S.; Niu, D.; Yang, W.; Ma, P. Highly toughened sustainable green polyglycolic acid/polycaprolactone blends with balanced strength: morphology evolution, interfacial compatibilization, and mechanism. ACS Appl. Polym. Mater. 2022, 4, 5772–5780.
Samantaray, P. K.; Little, A.; Haddleton, D. M.; McNally, T.; Tan, B.; Sun, Z.; Huang, W.; Ji, Y.; Wan, C. Poly(glycolic acid) (PGA): a versatile building block expanding high performance and sustainable bioplastic applications. Green Chem. 2020, 22, 4055–4081.
Kuredux Polyglycolic Acid (PGA) Resin, A New Polymer Option. http://www.kureha.com/product-groups/pga.htm.
Shunsuke, A. Successively biaxially stretched polyglycolic acid film, process for producing the successively biaxially stretched polyglycolic acid film, and multilayered film. WO: 2010.
Kawakami, Y.; Sato, N.; Hoshino, M.; Kouyama, T.; Shiiki, Z. Polyglycolic acid sheet and production process thereof. Google Patents: 1999.
Lin, Y.; Bilotti, E.; Bastiaansen, C. W.; Peijs, T. Transparent semi-crystalline polymeric materials and their nanocomposites: a review. Polym. Eng. Sci. 2020, 60, 2351–2376.
Wang, R.; Sun, X.; Chen, L.; Liang, W. Morphological and mechanical properties of biodegradable poly(glycolic acid)/poly(butylene adipate-co-terephthalate) blends with in situ compatibilization. RSC Adv. 2021, 11, 1241–1249.
Niu, D.; Xu, P.; Sun, Z.; Yang, W.; Dong, W.; Ji, Y.; Liu, T.; Du, M.; Lemstra, P. J.; Ma, P. Superior toughened bio-compostable poly(glycolic acid)-based blends with enhanced melt strength via selective interfacial localization of in-situ grafted copolymers. Polymer 2021, 235, 124269.
Ellingford, C.; Samantaray, P. K.; Farris, S.; McNally, T.; Tan, B.; Sun, Z.; Huang, W.; Ji, Y.; Wan, C. Reactive extrusion of biodegradable PGA/PBAT blends to enhance flexibility and gas barrier properties. J. Appl. Polym. Sci. 2021, 139, 51617.
Magazzini, L.; Grilli, S.; Fenni, S. E.; Donetti, A.; Cavallo, D.; Monticelli, O. The blending of poly(glycolic acid) with polycaprolactone and poly(l-lactide): promising combinations. Polymers 2021, 13, 2780.
Wang, K.; Shen, J.; Ma, Z.; Zhang, Y.; Xu, N.; Pang, S. Preparation and properties of poly(ethylene glycol-co-cyclohexane-1,4-dimethanol terephthalate)/polyglycolic acid (PETG/PGA) blends. Polymers 2021, 13, 452.
Chang, L. F.; Zhou, Y. G.; Ning, Y.; Zou, J. Toughening effect of physically blended polyethylene oxide on polyglycolic acid. J. Polym. Environ. 2020, 28, 2125–2136.
Vartiainen, J.; Shen, Y.; Kaljunen, T.; Malm, T.; Vähä-Nissi, M.; Putkonen, M.; Harlin, A. Bio-based multilayer barrier films by extrusion, dispersion coating and atomic layer deposition. J. Appl. Polym. Sci. 2016, 133, 42260.
Samantaray, P. K.; Ellingford, C.; Farris, S.; Tan, B.; Sun, Z.; Mcnally, T.; Wan, C. Electron beam-mediated cross-linking of blown film-extruded biodegradable PGA/PBAT blends toward high toughness and low oxygen permeation. ACS Sustainable Chem. Eng. 2022, 10, 1267–1276.
Yang, F.; Zhang, C.; Ma, Z.; Weng, Y. In situ formation of microfibrillar PBAT in PGA films: an effective way to robust barrier and mechanical properties for fully biodegradable packaging films. ACS Omega 2022, 7, 21280–21290.
Zhou, S. Y.; Huang, H. D.; Ji, X.; Yan, D. X.; Zhong, G. J.; Hsiao, B. S.; Li, Z. M. Super-robust polylactide barrier films by building densely oriented lamellae incorporated with ductile in situ nanofibrils of poly(butylene adipate-co-terephthalate). ACS Appl. Mater. Interfaces 2016, 8, 8096–109.
Yousfi, M.; Dadouche, T.; Chomat, D.; Samuel, C.; Soulestin, J.; Lacrampe, M. F.; Krawczak, P. Development of nanofibrillar morphologies in poly(L-lactide)/poly (amide) blends: role of the matrix elasticity and identification of the critical shear rate for the nodular/fibrillar transition. RSC Adv. 2018, 8, 22023–22041.
Wang, G.; Zhao, J.; Wang, G.; Zhao, H.; Lin, J.; Zhao, G.; Park, C. B. Strong and super thermally insulating in situ nanofibrillar PLA/PET composite foam fabricated by high-pressure microcellular injection molding. Chem. Eng. J. 2020, 390, 124520.
Chomat, D.; Soulestin, J.; Lacrampe, M. F.; Sclavons, M.; Krawczak, P. In situ fibrillation of polypropylene/polyamide 6 blends: Effect of organoclay addition. J. Appl. Polym. Sci. 2015, 132, 41680.
Ojijo, V.; Ray, S. S. Super toughened biodegradable polylactide blends with non-linear copolymer interfacial architecture obtained via facile in-situ reactive compatibilization. polymer 2015, 80, 1–17.
Sun, Q.; Mekonnen, T.; Misra, M.; Mohanty, A. K. Novel biodegradable cast film from carbon dioxide based copolymer and poly(lactic acid). J. Polym. Environ. 2015, 24, 23–36.
Li, X.; Yan, X.; Yang, J.; Pan, H.; Gao, G.; Zhang, H.; Dong, L. Improvement of compatibility and mechanical properties of the poly(lactic acid)/poly(butylene adipate-co-terephthalate) blends and films by reactive extrusion with chain extender. Polym. Eng. Sci. 2018, 58, 1868–1878.
Messin, T.; Follain, N.; Guinault, A.; Sollogoub, C.; Gaucher, V.; Delpouve, N.; Marais, S. Structure and barrier properties of multinanolayered biodegradable PLA/PBSA films: confinement effect via forced assembly coextrusion. ACS Appl. Mater. Interfaces 2017, 9, 29101–29112.
Chiu, F. C.; Hsieh, Y. C.; Sung, Y. C.; Liang, N. Y. Poly(butylene succinate-co-adipate) green composites with enhanced rigidity: influences of dimension and surface modification of Kenaf fiber reinforcement. Ind. Eng. Chem. Res. 2015, 54, 12826–12835.
Jiang, G.; Yu, L. High strength and barrier properties of biodegradable PPC/PBSA blends prepared by reaction compatibilization for promising application in packaging. Macromol. Mater. Eng. 2021, (306), 2000723.
Purahong, W.; Wahdan, S. F. M.; Heinz, D.; Jariyavidyanont, K.; Sungkapreecha, C.; Tanunchai, B.; Sansupa, C.; Sadubsarn, D.; Alaneed, R.; Heintz-Buschart, A.; Schadler, M.; Geissler, A.; Kressler, J.; Buscot, F. Back to the future: decomposability of a biobased and biodegradable plastic in field soil environments and its microbiome under ambient and future climates. Environ. Sci. Technol. 2021, 55, 12337–12351.
Yousfi, M.; Soulestin, J.; Marcille, S.; Lacrampe, M. F. In-situ nanofibrillation of poly(butylene succinate-co-adipate) in isosorbide-based polycarbonate matrix. Relationship between rheological parameters and induced morphological and mechanical properties. Polymer 2021, 217, 123445.
Nakafuku, C.; Yoshimura, H. Melting parameters of poly(glycolic acid). Polymer 2004, 45, 3583–3585.
Xu, H. S.; Li, Z. M.; Pan, J. L.; Yang, M. B.; Huang, R. Morphology and rheological behaviors of polycarbonate/high density polyethylene in situ microfibrillar blends. Macromol. Mater. Eng. 2004, 289, 1087–1095.
Xia, X. C.; Yang, W.; He, S.; Xie, D. D.; Zhang, R. Y.; Tian, F.; Yang, M. B. Formation of various crystalline structures in a polypropylene/polycarbonate in situ microfibrillar blend during the melt second flow. Phys. Chem. Chem. Phys. 2016, 18, 14030–9.
Evstatiev, M. Manufacturing and characterization of microfibrillar reinforced composites from polymer blends. Polym. Compos. 2005, 149–167.
Gu, S. Y.; Zhang, K.; Ren, J.; Zhan, H. Melt rheology of polylactide/poly(butylene adipate-co-terephthalate) blends. Carbohydr. Polym. 2008, 74, 79–85.
Wang, R.; Sun, X.; Chen, L.; Liang, W. Morphological and mechanical properties of biodegradable poly(glycolic acid)/poly(butylene adipate-co-terephthalate) blends with in situ compatibilization. RSC Adv. 2021, 11, 1241–1249.
Pan, H.; Li, Z.; Yang, J.; Li, X.; Ai, X.; Hao, Y.; Zhang, H.; Dong, L. The effect of MDI on the structure and mechanical properties of poly(lactic acid) and poly(butylene adipate-co-butylene terephthalate) blends. RSC Adv. 2018, 8, 4610–4623.
Murcia Valderrama, M. A.; van Putten, R. J.; Gruter, G. M. PLGA barrier materials from CO2. The influence of lactide co-monomer on glycolic acid polyesters. ACS Appl. Polym. Mater. 2020, 2, 2706–2718.
Lee, S.; Hongo, C.; Nishino, T. Crystal modulus of poly(glycolic acid) and its temperature dependence. Macromolecules 2017, 50, 5074–5079.
Montes de Oca, H.; Ward, I. M. Structure and mechanical properties of PGA crystals and fibres. Polymer 2006, 47, 7070–7077.
Sato, H.; Yamane, K.; Hokari, Y.; Kobayashi, F.; Kuruhara, N.; Ichikawa, Y.; Oishi, Y. Preparation and characterization of poly(ethylene terephtalate)/polyglycolic acid blends by simple extruding process. KOBUNSHI RONBUNSHU 2011, 68, 719–730.
Robeson, L. M. The upper bound revisited. J. Membr. Sci. 2008, 320, 390–400.
Shen, J.; Wang, K.; Ma, Z.; Xu, N.; Pang, S.; Pan, L. Biodegradable blends of poly(butylene adipate-co-terephthalate) and polyglycolic acid with enhanced mechanical, rheological and barrier performances. J. Appl. Polym. Sci. 2021, 138, e51285.
Wang, J.; Gardner, D. J.; Stark, N. M.; Bousfield, D. W.; Tajvidi, M.; Cai, Z. Moisture and oxygen barrier properties of cellulose nanomaterial-based films. ACS Sustain. Chem. Eng. 2018, 6, 49–70.
Samantaray, P. K.; Ellingford, C.; Farris, S.; O’Sullivan, D.; Tan, B.; Sun, Z.; McNally, T.; Wan, C. Electron beam-mediated cross-linking of blown film-extruded biodegradable PGA/PBAT blends toward high toughness and low oxygen permeation. ACS Sustain. Chem. Eng. 2022, 10, 1267–1276.
Ojijo, V.; Sinha Ray, S.; Sadiku, R. Concurrent enhancement of multiple properties in reactively processed nanocomposites of polylactide/poly[(butylene succinate)-co-adipate] blend and organoclay. Macromol. Mater. Eng. 2014, 299, 596–608.
Suwanamornlert, P.; Kerddonfag, N.; Sane, A.; Chinsirikul, W.; Zhou, W.; Chonhenchob, V. Poly(lactic acid)/poly(butylene-succinate-co-adipate) (PLA/PBSA) blend films containing thymol as alternative to synthetic preservatives for active packaging of bread. Food Packag. Shelf Life 2020, 25, 100515.
Palai, B.; Mohanty, S.; Nayak, S. K. Synergistic effect of polylactic acid (PLA) and poly(butylene succinate-co-adipate) (PBSA) based sustainable, reactive, super toughened eco-composite blown films for flexible packaging applications. Polym. Test. 2020, 83, 106130.
Acknowledgments
This study was financially supported by the National Key Research and Development Program of China (No. 2022YFB3704900), the National Natural Science Foundation of China (No. 52073004) and China National Tobacco Corporation Guizhou Company (No. 2023XM24).
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Generation of Tough Poly(glycolic acid) (PGA)/Poly(butylene succinate-co-butylene adipate) (PBSA) Films with High Gas Barrier Performance through In situ Nanofibrillation of PBSA under an Elongational Flow Field
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Yang, F., Zhang, CL., Han, Y. et al. Generation of Tough Poly(glycolic acid) (PGA)/Poly(butylene succinate-co-butylene adipate) (PBSA) Films with High Gas Barrier Performance through In situ Nanofibrillation of PBSA under an Elongational Flow Field. Chin J Polym Sci 41, 1805–1817 (2023). https://doi.org/10.1007/s10118-023-2972-9
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DOI: https://doi.org/10.1007/s10118-023-2972-9