Superior Toughened Biodegradable Poly(L-lactic acid)-based Blends with Enhanced Melt Strength and Excellent Low-temperature Toughness <italic style="font-style: italic">via</italic> <italic style="font-style: italic">In situ</italic> Reaction Compatibilization

Shi-Ling Jia; Xiang-Yu Wang; Ye Zhang; Xiang-Yu Yan; Hong-Wei Pan; Yan Zhao; Li-Jing Han; Hui-Liang Zhang; Li-Song Dong; Hui-Xuan Zhang

doi:10.1007/s10118-022-2862-6

Your Location：

Home >

Browse articles >

Superior Toughened Biodegradable Poly(L-lactic acid)-based Blends with Enhanced Melt Strength and Excellent Low-temperature Toughness via In situ Reaction Compatibilization

RESEARCH ARTICLE | Updated：2023-01-18

- Superior Toughened Biodegradable Poly(L-lactic acid)-based Blends with Enhanced Melt Strength and Excellent Low-temperature Toughness via In situ Reaction Compatibilization
- Chinese Journal of Polymer Science Vol. 41, Issue 3, Pages: 373-385(2023)
- Affiliations：
  
  a.Key Laboratory of Polymer Ecomaterials, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun130022, China
  b.School of Materials Science and Engineering, Changchun University of Technology, Changchun 130012, China
- Author bio：
  
  ljhan@ciac.ac.cn
- Funds：
- DOI：10.1007/s10118-022-2862-6
  CLC：
- Received：16 June 2022，
  
  Revised：2022-7-20，
  
  Accepted：22 August 2022，
  
  Online First：20 October 2022，
  
  Published：01 March 2023
- Accepted：
Scan QR Code
Jia, S. L.; Wang, X. Y.; Zhang, Y.; Yan, X. Y.; Pan, H. W.; Zhao, Y.; Han, L. J.; Zhang, H. L.; Dong, L. S.; Zhang, H. X. Superior toughened biodegradable poly(L-lactic acid)-based blends with enhanced melt strength and excellent low-temperature toughness via in situ reaction compatibilization. Chinese J. Polym. Sci. 2023, 41, 373–385

Shi-Ling Jia, Xiang-Yu Wang, Ye Zhang, et al. Superior Toughened Biodegradable Poly(L-lactic acid)-based Blends with Enhanced Melt Strength and Excellent Low-temperature Toughness via In situ Reaction Compatibilization[J]. Chinese Journal of Polymer Science, 2023, 41(3): 373-385. DOI: 10.1007/s10118-022-2862-6.
Jia, S. L.; Wang, X. Y.; Zhang, Y.; Yan, X. Y.; Pan, H. W.; Zhao, Y.; Han, L. J.; Zhang, H. L.; Dong, L. S.; Zhang, H. X. Superior toughened biodegradable poly(L-lactic acid)-based blends with enhanced melt strength and excellent low-temperature toughness via in situ reaction compatibilization. Chinese J. Polym. Sci. 2023, 41, 373–385 DOI： 10.1007/s10118-022-2862-6.

Shi-Ling Jia, Xiang-Yu Wang, Ye Zhang, et al. Superior Toughened Biodegradable Poly(L-lactic acid)-based Blends with Enhanced Melt Strength and Excellent Low-temperature Toughness via In situ Reaction Compatibilization[J]. Chinese Journal of Polymer Science, 2023, 41(3): 373-385. DOI: 10.1007/s10118-022-2862-6. DOI：

摘要

In this study

PBST and PLLA were melt blended

and ADR was added to improve the compatibility of the blends. As the formation of PLLA-g-PBST copolymer improves the interfacial bonding of the blends

biodegradable materials with excellent mechanical properties at both room temperature and low temperature are prepared.

Abstract

The toughened poly(L-lactic acid)/poly(butylene succinate-butylene terephthalate) (PLLA/PBST) blend with enhanced melt strength and excellent low temperature toughness and strength was prepared by melt compounding through

in situ

compatibilization reaction in presence of multifunctional epoxy compound (ADR). The PLLA/PBST blend was an immiscible system

and the compatibility of the PLLA/PBST blend was improved after adding ADR. FTIR and GPC curves confirmed the formation of the PLLA-

-PBST copolymer

which improved the interfacial bonding of the blend and therefore the PLLA/PBST/ADR blend showed excellent melt strength and mechanical properties. For the PLLA/PBST/ADR blend with 70/30 PLLA/PBST content

the complex viscosity increased significantly with increasing ADR content. Moreover

the tensile strength

elongation at break and impact strength all increased obviously with increasing the ADR content. The elongation at break of the blend reached the maximum value of 392.7%

which was 93.2 times that of neat PLLA. And the impact strength of the blend reached the maximum value of 74.7 kJ/m

which was 21.3 times that of neat PLLA. Interestingly

the PLLA/PBST/ADR blend exhibited excellent low-temperature toughness and strength. At –20 °C

the elongation at break of the PLLA/PBST/ADR blend was as high as 93.2%

and the impact strength reached 18.8 kJ/m

. Meanwhile

the tensile strength of the blend at low temperature was also high (64.7 MPa)

which was beneficial to the application of PLA in the low temperature field. In addition

the PLLA/PBST/ADR blend maintaind good biodegradability

which was of great significance to the wide application of PLLA.

关键词

Keywords

references

Garlotta, D . A literature review of poly(lactic acid) . J. Polym. Environ. , 2001 . 9 63 - 84 . DOI: 10.1023/A:1020200822435 http://doi.org/10.1023/A:1020200822435 .

Sodergard, A.; Stolt, M . Properties of lactic acid based polymers and their correlation with composition . Prog. Polym. Sci. , 2002 . 27 1123 - 1163 . DOI: 10.1016/S0079-6700(02)00012-6 http://doi.org/10.1016/S0079-6700(02)00012-6 .

Lim, L . T.; Auras, R.; Rubino, M. Processing technologies for poly(lactic acid) . Prog. Polym. Sci. , 2008 . 33 820 - 852 . DOI: 10.1016/j.progpolymsci.2008.05.004 http://doi.org/10.1016/j.progpolymsci.2008.05.004 .

Ho, C. H.; Wang, C. H.; Lin, C. I.; Lee, Y. D . Synthesis and characterization of TPO-PLA copolymer and its behavior as compatibilizer for PLA/TPO blends . Polymer , 2008 . 49 3902 - 3910 . DOI: 10.1016/j.polymer.2008.06.054 http://doi.org/10.1016/j.polymer.2008.06.054 .

Anderson, K. S.; Hillmyer, M. A . The influence of block copolymer microstructure on the toughness of compatibilized polylactide/polyethylene blends . Polymer , 2004 . 45 8809 - 8823 . DOI: 10.1016/j.polymer.2004.10.047 http://doi.org/10.1016/j.polymer.2004.10.047 .

Ma, P.; Hristova-Bogaerds, D. G.; Goossens, J. G. P.; Spoelstra, A. B.; Zhang, Y.; Lemstra, P. J . Toughening of poly(lactic acid) by ethylene- co -vinyl acetate copolymer with different vinyl acetate contents . Eur. Polym. J. , 2012 . 48 146 - 154 . DOI: 10.1016/j.eurpolymj.2011.10.015 http://doi.org/10.1016/j.eurpolymj.2011.10.015 .

Gajria, A. M.; Dave, V.; Gross, R. A.; McCarthy, S. P . Miscibility and biodegradability of blends of poly(lactic acid) and poly(vinyl acetate) . Polymer , 1996 . 37 437 - 444 . DOI: 10.1016/0032-3861(96)82913-2 http://doi.org/10.1016/0032-3861(96)82913-2 .

Eguiburu, J. L.; Iruin, J. J.; Fernandez-Berridi, M. J.; Roman, J. S . Blends of amorphous and crystalline polylactides with poly(methyl methacrylate) and poly(methyl acrylate): a miscibility study . Polymer , 1998 . 39 6891 - 6897 . DOI: 10.1016/S0032-3861(98)00182-7 http://doi.org/10.1016/S0032-3861(98)00182-7 .

Zhang, W.; Chen, L.; Zhang, Y . Surprising shape-memory effect of polylactide resulted from toughening by polyamide elastomer . Polymer , 2009 . 50 1311 - 1315 . DOI: 10.1016/j.polymer.2009.01.032 http://doi.org/10.1016/j.polymer.2009.01.032 .

Feng, F.; Zhao, X. W.; Ye, L . Structure and Properties of Ultradrawn Polylactide/Thermoplastic Polyurethane Elastomer Blends . J. Macromol. Sci., Part B-Phys. , 2011 . 50 1500 - 1507 . DOI: 10.1080/00222348.2010.518889 http://doi.org/10.1080/00222348.2010.518889 .

Han, L. J.; Han, C. Y.; Zhang, H. L.; Chen, S.; Dong, L. S . Morphology and properties of biodegradable and biosourced polylactide blends with poly(3-hydroxybutyrate- co -4-hydroxybutyrate) . Polym. Compos. , 2012 . 33 850 - 859 . DOI: 10.1002/pc.22213 http://doi.org/10.1002/pc.22213 .

Zhao, H. W.; Bian, Y. J.; Li, Y.; Dong, Q. L.; Han, C. Y.; Dong, L. S . Bioresource-based blends of poly(3-hydroxybutyrate- co -4-hydroxybutyrate) and stereocomplex polylactide with improved rheological and mechanical properties and enzymatic hydrolysis . J. Mater. Chem. A , 2014 . 2 8881 - 8892 . DOI: 10.1039/c4ta01194e http://doi.org/10.1039/c4ta01194e .

Jiang, L.; Wolcott, M. P.; Zhang, J. W . Study of biodegradable polyactide/poly(butylene adipate- co -terephthalate) blends . Biomacromolecules , 2006 . 7 199 - 207 . DOI: 10.1021/bm050581q http://doi.org/10.1021/bm050581q .

Ma, P.; Cai, X.; Zhang, Y.; Wang, S.; Dong, W.; Chen, M.; Lemstra, P. J . In-situ compatibilization of poly(lactic acid) and poly(butylene adipate- co -terephthalate) blends by using dicumyl peroxide as a free-radical initiator . Polym. Degrad. Stabil. , 2014 . 102 145 - 151 . DOI: 10.1016/j.polymdegradstab.2014.01.025 http://doi.org/10.1016/j.polymdegradstab.2014.01.025 .

Zhang, K. Y.; Mohanty, A. K.; Misra, M . Fully biodegradable and biorenewable ternary blends from polylactide, poly(3-hydroxybutyrate- co -hydroxyvalerate) and poly(butylene succinate) with balanced properties . ACS Appl. Mater. Interfaces , 2012 . 4 3091 - 3101 . DOI: 10.1021/am3004522 http://doi.org/10.1021/am3004522 .

Supthanyakul, R.; Kaabbuathong, N.; Chirachanchai, S . Random poly(butylene succinate- co -lactic acid) as a multi-functional additive for miscibility, toughness, and clarity of PLA/PBS blends . Polymer , 2016 . 105 1 - 9 . DOI: 10.1016/j.polymer.2016.10.006 http://doi.org/10.1016/j.polymer.2016.10.006 .

Chuayjuljit, S.; Wongwaiwattanakul, C.; Chaiwutthinan, P.; Prasassarakich, P . Biodegradable poly(lactic acid)/poly(butylene succinate)/wood flour composites: physical and morphological properties . Polym. Compos. , 2017 . 38 2841 - 2851 . DOI: 10.1002/pc.23886 http://doi.org/10.1002/pc.23886 .

Zhao, X. P.; Zhang, D. F.; Yu, S. T.; Zhou, H. Y.; Peng, S. X . Recent advances in compatibility and toughness of poly(lactic acid)/poly(butylene succinate) blends . e-Polymers , 2021 . 21 793 - 810 . DOI: 10.1515/epoly-2021-0072 http://doi.org/10.1515/epoly-2021-0072 .

Tsuji, H.; Ikada, Y . Blends of aliphatic polyesters .2. Hydrolysis of solution-cast blends from poly(L-lactide) and poly(epsilon-caprolactone) in phosphate-buffered solution . J. Appl. Polym. Sci. , 1998 . 67 405 - 415 . DOI: 10.1002/(SICI)1097-4628(19980118)67:3<405::AID-APP3>3.0.CO;2-Q http://doi.org/10.1002/(SICI)1097-4628(19980118)67:3<405::AID-APP3>3.0.CO;2-Q .

Garcia-Campo, M . J.; Boronat, T.; Quiles-Carrillo, L.; Balart, R.; Montanes, N. Manufacturing and characterization of toughened poly(lactic acid) (PLA) formulations by ternary blends with biopolyesters . Polymers , 2018 . 10 15 .

Si, W. J.; Zhang, H.; Li, Y. D.; Huang, C. L.; Weng, Y. X.; Zeng, J. B . Highly toughened and heat resistant poly(L-lactide)/poly( ε -caprolactone) blends via engineering balance between kinetics and thermodynamics of phasic morphology with stereocomplex crystallite . Compos. Part B-Eng. , 2020 . 197 11 .

Zhao, T. H.; Yuan, W. Q.; Li, Y. D.; Weng, Y. X.; Zeng, J. B . Relating chemical structure to toughness via morphology control in fully sustainable sebacic acid cured epoxidized soybean oil toughened polylactide blends . Macromolecules , 2018 . 51 2027 - 2037 . DOI: 10.1021/acs.macromol.8b00103 http://doi.org/10.1021/acs.macromol.8b00103 .

Wang, M.; Wu, Y.; Li, Y. D.; Zeng, J. B . Progress in toughening poly(lactic acid) with renewable polymers . Polym. Rev. , 2017 . 57 557 - 593 . DOI: 10.1080/15583724.2017.1287726 http://doi.org/10.1080/15583724.2017.1287726 .

Zhao, X. P.; Hu, H.; Wang, X.; Yu, X. L.; Zhou, W. Y.; Peng, S. X . Super tough poly(lactic acid) blends: a comprehensive review . RSC Adv. , 2020 . 10 13316 - 13368 . DOI: 10.1039/D0RA01801E http://doi.org/10.1039/D0RA01801E .

Zuo, H. J.; Liu, J. Y.; Huang, D.; Bai, Y. B.; Cui, L.; Pan, L.; Zhang, K. Y.; Wang, H. Y . Sustainable and high-performance ternary blends from polylactide, CO 2 -based polyester and microbial polyesters with different chemical structure . J. Polym. Sci. , 2021 . 59 1578 - 1595 . DOI: 10.1002/pol.20210175 http://doi.org/10.1002/pol.20210175 .

Li, R.; Wu, L.; Li, B. G . Poly(L-lactide)/PEG-mb-PBAT blends with highly improved toughness and balanced performance . Eur. Polym. J. , 2018 . 100 178 - 186 . DOI: 10.1016/j.eurpolymj.2018.01.037 http://doi.org/10.1016/j.eurpolymj.2018.01.037 .

Pan, H. W.; Li, Z. L.; Yang, J.; Li, X.; Ai, X.; Hao, Y. P.; Zhang, H. L.; Dong, L. S . 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 . DOI: 10.1039/C7RA10745E http://doi.org/10.1039/C7RA10745E .

Zhao, Y.; Zhang, Y.; Li, Z. L.; Pan, H. W.; Dong, Q. L.; Han, L. J.; Zhang, H. L.; Dong, L. S . Rheology, mechanical properties and crystallization behavior of glycidyl methacrylate grafted poly(ethylene octene) toughened poly(lactic acid) blends . Korean J. Chem. Eng. , 2016 . 33 1104 - 1114 . DOI: 10.1007/s11814-015-0202-z http://doi.org/10.1007/s11814-015-0202-z .

Jia, S. L.; Chen, Y. J.; Yu, Y. L.; Han, L. J.; Zhang, H. L.; Dong, L. S . Effect of ethylene/butyl methacrylate/glycidyl methacrylate terpolymer on toughness and biodegradation of poly(L-lactic acid) . Int. J. Biol. Macromol. , 2019 . 127 415 - 424 . DOI: 10.1016/j.ijbiomac.2019.01.068 http://doi.org/10.1016/j.ijbiomac.2019.01.068 .

Dong, W. F.; Zou, B. S.; Yan, Y. Y.; Ma, P. M.; Chen, M. Q . Effect of chain-extenders on the properties and hydrolytic degradation behavior of the poly(lactide)/poly(butylene adipate- co -terephthalate) blends . Int. J. Mol. Sci. , 2013 . 14 20189 - 20203 . DOI: 10.3390/ijms141020189 http://doi.org/10.3390/ijms141020189 .

Wang, X.; Peng, S. X.; Chen, H.; Yu, X. L.; Zhao, X. P . Mechanical properties, rheological behaviors, and phase morphologies of high-toughness PLA/PBAT blends by in situ reactive compatibilization . Compos. Part B-Eng. , 2019 . 173 10 .

Zhang, H.; Yuan, W. Q.; Weng, Y. X.; Zeng, J. B.; Li, Y. D . Morphological control and interfacial compatibilization of fully biobased PLA/ENR blends via partial crosslinking ENR with sebacic acid . Ind. Crop. Prod. , 2022 . 180 12 .

Zhao, X. P.; Li, J. C.; Liu, J. C.; Zhou, W. Y.; Peng, S. X . Recent progress of preparation of branched poly(lactic acid) and its application in the modification of polylactic acid materials . Int. J. Biol. Macromol. , 2021 . 193 874 - 892 . DOI: 10.1016/j.ijbiomac.2021.10.154 http://doi.org/10.1016/j.ijbiomac.2021.10.154 .

Zhu, G.; Zhang, W.; Han, L.; Xu, N.; Ji, W . Toughening modification of polylactic acid with biodegradable aliphatic-aromatic copolyester . Petrochem. Technol. , 2014 . 43 561 - 565 . .

Al-Itry, R.; Lamnawar, K.; Maazouz, A . Improvement of thermal stability, rheological and mechanical properties of PLA, PBAT and their blends by reactive extrusion with functionalized epoxy . Polym. Degrad. Stabil. , 2012 . 97 1898 - 1914 . DOI: 10.1016/j.polymdegradstab.2012.06.028 http://doi.org/10.1016/j.polymdegradstab.2012.06.028 .

Zhou, Y.; Wang, J.; Cai, S. Y.; Wang, Z. G.; Zhang, N. W.; Ren, J . Effect of POE- g -GMA on mechanical, rheological and thermal properties of poly(lactic acid)/poly(propylene carbonate) blends . Polym. Bull. , 2018 . 75 5437 - 5454 . DOI: 10.1007/s00289-018-2339-5 http://doi.org/10.1007/s00289-018-2339-5 .

Huang, Y.; Zhang, C. M.; Pan, Y. H.; Wang, W . W.; Jiang, L.; Dan, Y. Study on the effect of dicumyl peroxide on structure and properties of poly(lactic acid)/natural rubber blend . J. Polym. Environ. , 2013 . 21 375 - 387 . DOI: 10.1007/s10924-012-0544-0 http://doi.org/10.1007/s10924-012-0544-0 .

Wu, D. F.; Zhang, Y. S.; Zhang, M.; Zhou, W. D . Phase behavior and its viscoelastic response of polylactide/poly( ε -caprolactone) blend . Eur. Polym. J. , 2008 . 44 2171 - 2183 . DOI: 10.1016/j.eurpolymj.2008.04.023 http://doi.org/10.1016/j.eurpolymj.2008.04.023 .

Singla, R. K.; Zafar, M. T.; Maiti, S. N.; Ghosh, A. K . Physical blends of PLA with high vinyl acetate containing EVA and their rheological, thermo-mechanical and morphological responses . Polym. Test. , 2017 . 63 398 - 406 . DOI: 10.1016/j.polymertesting.2017.08.042 http://doi.org/10.1016/j.polymertesting.2017.08.042 .

Zhang, N. W.; Wang, Q . F.; Ren, J.; Wang, L. Preparation and properties of biodegradable poly(lactic acid)/poly(butylene adipate- co -terephthalate) blend with glycidyl methacrylate as reactive processing agent . J. Mater. Sci. , 2009 . 44 250 - 256 . DOI: 10.1007/s10853-008-3049-4 http://doi.org/10.1007/s10853-008-3049-4 .

Jia, S.; Chen, Y.; Bian, J.; Pan, H.; Wang, X.; Zhao, L.; Han, L.; Zhang, H.; Dong, L.; Zhang, H . Preparation and properties of poly(L-lactic acid) blends with excellent low-temperature toughness by blending acrylic ester based impact resistance agent . Int. J. Biol. Macromol. , 2021 . 183 1871 - 1880 . DOI: 10.1016/j.ijbiomac.2021.05.177 http://doi.org/10.1016/j.ijbiomac.2021.05.177 .

Jia, S.; Zhao, L.; Wang, X.; Chen, Y.; Pan, H.; Han, L.; Zhang, H.; Dong, L.; Zhang, H . Poly(lactic acid) blends with excellent low temperature toughness: a comparative study on poly(lactic acid) blends with different toughening agents . Int. J. Biol. Macromol. , 2022 . 201 662 - 675 . DOI: 10.1016/j.ijbiomac.2022.01.126 http://doi.org/10.1016/j.ijbiomac.2022.01.126 .

Tsuji, H.; Ishizaka, T. Blends of aliphatic polyesters. VI . Lipase-catalyzed hydrolysis and visualized phase structure of biodegradable blends from poly( ε -caprolactone) and poly(L-lactide) . Int. J. Biol. Macromol. , 2001 . 29 83 - 89 . DOI: 10.1016/S0141-8130(01)00158-1 http://doi.org/10.1016/S0141-8130(01)00158-1 .

Views

251

Downloads

CSCD

Alert me when the article has been cited

Submit

Tools

Publicity Resources

Compatibilizer-aided Fabrication of a 'High-entropy Polymer Blend'

Biobased Polyesters Derived from 2-Methoxyhydroquinone: Impact of Cyclic and Alkyl Chain Segments on Their Thermomechanical Properties, Biodegradability, and Ecotoxicity

One-step Preparation of Brush-type Polystyrene (PS)-SiO2-Poly(2-hydroxyethyl methacrylate) Janus Nanoparticle to Compatibilize PS/Poly(methyl methacrylate) Blends

Sliding Dynamics of Ring Chain on a Rod-Coil Block Copolymer in Rotaxane

Molecular Segregation and Melt Memory in Dilute Polycaprolactone with Reduced Entanglements

Related Author

Jia-Nan Du

Wen-Kang Wei

Shi-De Lu

Dong Wang

Hao-Ming Xu

Zheng-Zai Cheng

Zi-Ting Zhou

Lesly Dasilva Wandji Djouonkep

Related Institution

Shandong Runde Composite Materials Co., Ltd.

State Key Laboratory of Organic-Inorganic Composites & Beijing Key Laboratory of Advanced Functional Polymer Composites, Beijing University of Chemical Technology

Institute of Fine Organic Chemicals & Organic Materials, School of Chemistry and Chemical Engineering, Wuhan University of Science and Technology

College of Chemistry and Materials Science, Fujian Key Laboratory of Polymer Materials, Fujian Normal University

School of Chemistry, Key Laboratory of Advanced Technologies of Materials (Ministry of Education), Southwest Jiaotong University

⁰

Superior Toughened Biodegradable Poly(L-lactic acid)-based Blends with Enhanced Melt Strength and Excellent Low-temperature Toughness via In situ Reaction Compatibilization

DOI：10.1007/s10118-022-2862-6

摘要

Abstract

关键词

Keywords

references