Skip to main content
SpringerLink
Log in

Biosourced epoxidized neem oil toughened poly(lactic acid) for agricultural applications: mechanical, thermal and compostability properties

  • Original Research
  • Published:
Iranian Polymer Journal Aims and scope Submit manuscript

Abstract

Poly(lactic acid) (PLA) is a stupendous alternative to conventional plastics in several applications such as packaging, cutlery, etc., although biodegradable PLA has drawbacks such as brittleness, poor processability and low thermal resistance. This study focuses on impact modification of PLA through melt blending with epoxidized neem oil (ENO), a cost effective, non-edible oil-based plasticizer with diversified properties as an anti-microbial and bio-pesticide. Neem oil was subjected to epoxidation and blended with virgin PLA (VPLA) using a twin-screw extruder at different weight ratios of 95/5, 92.5/7.5, 90/10 and 85/15. The fully green PLA/ENO blends were observed to have significant increase in impact strength and elongation-at-break with drop in glass transition (Tg), melting (Tm) and crystallization (Tc) temperatures. SEM images revealed good interfacial adhesion, to the extent of 10% (by weight) of ENO, which could be attributed to the enhancement of mechanical properties in the blends. The blend PLA/ENO10 showed maximum impact strength of 66 J/m (413% increase), elongation-at-break of 78% (VPLA: 3.5%) and higher heat deflection temperature of 90 °C (VPLA: 55 °C). Aerobic biodegradation study of PLA/ENO10 blend as per ISO 14855-1 indicated that 90% biodegradability was achieved within 96 days under controlled composting conditions and the obtained compost was non-toxic and supported plant growth. The ENO-modified PLA is a promising eco-friendly candidate for agricultural applications, such as nursery bags.

Graphical abstract

This is a preview of subscription content, log in via an institution to check access.

Access this article

Log in via an institution

Price excludes VAT (USA)
Tax calculation will be finalised during checkout.

Instant access to the full article PDF.

Institutional subscriptions

Fig. 1
Fig. 2
Scheme 1
Fig. 3
Fig. 4
Fig. 5
Fig. 6
Fig. 7
Fig. 8
Fig. 9
Fig. 10

Similar content being viewed by others

Data availability

The data that support the findings of this study are available from the corresponding author, [K. A. Rajesh], upon reasonable request.

References

  1. Bandopadhyay S, Martin-Closas L, Pelacho AM, DeBruyn JM (2018) Biodegradable plastic mulch films: impacts on soil microbial communities and ecosystem functions. Front Microbiol 9:819. https://doi.org/10.3389/fmicb.2018.00819

    Article  PubMed  PubMed Central  Google Scholar 

  2. Chieng B, Ibrahim N, Then Y, Loo Y (2014) Epoxidized vegetable oils plasticized poly (lactic acid) biocomposites: mechanical, thermal and morphology properties. Molecules 19:16024–16038. https://doi.org/10.3390/molecules191016024

    Article  CAS  PubMed  PubMed Central  Google Scholar 

  3. Ali F, Chang YW, Kang SC, Yoon JY (2009) Thermal, mechanical and rheological properties of poly(lactic acid)/epoxidized soybean oil blends. Polym Bull 62:91–98. https://doi.org/10.1007/s00289-008-1012-9

    Article  CAS  Google Scholar 

  4. Tang Z, Zhang C, Liu X, Zhu J (2012) The crystallization behavior and mechanical properties of polylactic acid in the presence of a crystal nucleating agent. J Appl Polym Sci 125:1108–1115. https://doi.org/10.1002/app.34799

    Article  CAS  Google Scholar 

  5. Rajesh KA, Panicker AM, Varghese TO (2022) Effect of compatibilization of thermoplastic polyurethane with poly(lactic acid) for the preparation of sustainable blends. Polym Sci Ser A 63:S46-57. https://doi.org/10.1134/S0965545X22030087

    Article  Google Scholar 

  6. Baiardo M, Frisoni G, Scandola M, Rimelen M, Lips D, Ruffieux K, Wintermantel E (2003) Thermal and mechanical properties of plasticized poly(L-lactic acid). J Appl Polym Sci 90:1731–1738. https://doi.org/10.1002/app.12549

    Article  CAS  Google Scholar 

  7. Labrecque LV, Kumar RA, Davé V, Gross RA, McCarthy SP (1997) Citrate esters as plasticizers for poly(lactic acid). J Appl Polym Sci 66:1507–1513. https://doi.org/10.1002/(SICI)1097-4628(19971121)66:8%3c1507::AID-APP11%3e3.0.CO;2-0

    Article  CAS  Google Scholar 

  8. Kulinski Z, Piorkowska E, Gadzinowska K, Stasiak M (2006) Plasticization of poly(L-lactide) with poly(propylene glycol). Biomacromol 7:21282135. https://doi.org/10.1021/bm060089m

    Article  CAS  Google Scholar 

  9. Pluta M, Piorkowska E (2015) Tough and transparent blends of polylactide with block copolymers of ethylene glycol and propylene glycol. Polym Test 41:209–218. https://doi.org/10.1016/j.polymertesting.2014.11.011

    Article  CAS  Google Scholar 

  10. Harada M, Ohya T, Iida K, Hayashi H, Hirano K, Fukuda H (2007) Increased impact strength of biodegradable poly(lactic acid)/poly(butylene succinate) blend composites using isocyanate as a reactive processing agent. J Appl Polym Sci 106:1813–1820. https://doi.org/10.1002/app.26717

    Article  CAS  Google Scholar 

  11. Fenollar O, García D, Sánchez L, López J, Balart R (2009) Optimization of the curing conditions of PVC plastisols based on the use of an epoxidized fatty acid ester plasticizer. Eur Polym J 45:2674–2684. https://doi.org/10.1016/j.eurpolymj.2009.05.029

    Article  CAS  Google Scholar 

  12. Tee YB, Talib RA, Abdan K, Chin NL, Basha RK, Yunos KF (2016) Comparative study of chemical, mechanical, thermal, and barrier properties of poly(lactic acid) plasticized with epoxidized soybean oil and epoxidized palm oil. BioResources 11:1518–1540. https://doi.org/10.15376/biores.11.1.1518-1540

  13. Bouti M, Irinislimane R, Belhaneche-Bensemra N (2022) Properties investigation of epoxidized sunflower oil as bioplasticizer for poly(lactic acid). J Polym Environ 30:232–245. https://doi.org/10.1007/s10924-021-02194-3

    Article  CAS  Google Scholar 

  14. Silverajah VSG, Ibrahim NA, Zainuddin N, Yunus W, Hassan HA (2012) Mechanical, thermal and morphological properties of poly(lactic acid)/epoxidized palm olein blend. Molecules 17:11729–11747. https://doi.org/10.3390/molecules171011729

    Article  CAS  PubMed  PubMed Central  Google Scholar 

  15. Murariu M, Da Silva FA, Alexandre M, Dubois P (2008) Polylactide (PLA) designed with desired end-use properties: 1. PLA compositions with low molecular weight ester-like plasticizers and related performances. Polym Adv Technol 19:636–646. https://doi.org/10.1002/pat.1131

    Article  CAS  Google Scholar 

  16. Isman MB, Koul O, Luczynski A, Kaminski J (1990) Insecticidal and antifeedant bioactivities of neem oils and their relationship to azadirachtin content. J Agric Food Chem 38:1406–1411. https://doi.org/10.1021/jf00096a024

    Article  CAS  Google Scholar 

  17. Koley R, Kasilingam R, Sahoo S, Chattopadhyay S, Bhowmick AK (2021) Synthesis and characterization of epoxidized neem oil: a bio-derived natural processing aid for elastomer. J Appl Polym Sci 138:50440. https://doi.org/10.1002/app.50440

    Article  CAS  Google Scholar 

  18. Pascoli M, Jacques MT, Agarrayua DA, Avila DS, LimaR FLF (2019) Neem oil based nanopesticide as an environmentally-friendly formulation for applications in sustainable agriculture: an ecotoxicological perspective. Sci Total Environ 677:57–67. https://doi.org/10.1016/j.scitotenv.2019.04.345

    Article  CAS  PubMed  Google Scholar 

  19. Derahman A, Abidin ZZ, Cardona F, Biak DRA, Tahir PMD, Abdan K, Liew KE (2019) Epoxidation of jatropha methyl esters via acidic ion exchange resin: optimization and characterization. Braz J Chem Eng 36:959–968. https://doi.org/10.1590/0104-6632.20190362s20180326

    Article  CAS  Google Scholar 

  20. Hamadou B, Djomdi D, Falama RZ, Delattre C, Pierre G, Dubessay P, Michaud P (2020) Influence of physicochemical characteristics of neem seeds (Azadirachta indica A. Juss) on biodiesel production. Biomolecules 10:616. https://doi.org/10.3390/biom10040616

  21. Orue A, Eceiza A, Arbelaiz A (2018) Preparation and characterization of poly(lactic acid) plasticized with vegetable oils and reinforced with sisal fibers. Ind Crops Prod 112:170–180. https://doi.org/10.1016/j.indcrop.2017.11.011

    Article  CAS  Google Scholar 

  22. Zych A, Perotto G, Trojanowska D, Tedeschi G, Bertolacci L, Francini N, Athanassiou A (2021) Super tough polylactic acid plasticized with epoxidized soybean oil methyl ester for flexible food packaging. ACS Appl Polym Mater 3:5087–5095. https://doi.org/10.1021/acsapm.1c00832

    Article  CAS  Google Scholar 

  23. Burgos N, Martino VP, Jiménez A (2013) Characterization and ageing study of poly(lactic acid) films plasticized with oligomeric lactic acid. Polym Degrad Stab 98:651–658. https://doi.org/10.1016/j.polymdegradstab.2012.11.009

    Article  CAS  Google Scholar 

  24. Nagarajan V, Zhang K, Misra M, Mohanty AK (2015) Overcoming the fundamental challenges in improving the impact strength and crystallinity of PLA biocomposites: influence of nucleating agent and mold temperature. ACS Appl Mater Interfaces 7:11203–11214. https://doi.org/10.1021/acsami.5b01145

  25. Bouchareb B, Benaniba MT (2008) Effects of epoxidized sunflower oil on the mechanical and dynamical analysis of the plasticized poly(vinyl chloride). J Appl Polym Sci 107:3442–3450. https://doi.org/10.1002/app.27458

    Article  CAS  Google Scholar 

  26. Muscat D, Adhikari B, Adhikari R, Chaudhary DS (2012) Comparative study of film forming behaviour of low and high amylose starches using glycerol and xylitol as plasticizers. J Food Eng 109:189–201. https://doi.org/10.1016/j.jfoodeng.2011.10.019

    Article  CAS  Google Scholar 

  27. Mekonnen T, Mussone P, Khalil H, Bressler D (2013) Progress in bio-based plastics and plasticizing modifications. J Mater Chem A 1:13379. https://doi.org/10.1039/c3ta12555f

    Article  CAS  Google Scholar 

  28. Garcia-Garcia D, Ferri JM, Montanes N, Lopez-Martinez J, Balart R (2016) Plasticization effects of epoxidized vegetable oils on mechanical properties of poly(3-hydroxybutyrate). Polym Int 65:1157–1164. https://doi.org/10.1002/pi.5164

    Article  CAS  Google Scholar 

  29. Sahakaro K, Beraheng A (2011) Epoxidized natural oils as the alternative safe process oils in rubber compounds. Rubber Chem Technol 84:200–214. https://doi.org/10.5254/1.3577518

  30. Leejarkpai T, Suwanmanee U, Rudeekit Y, Mungcharoen T (2011) Biodegradable kinetics of plastics under controlled composting conditions. Waste Manag 31:1153–1161. https://doi.org/10.1016/j.wasman.2010.12.011

    Article  CAS  PubMed  Google Scholar 

Download references

Acknowledgements

The authors are thankful to Abin Davis, Aarsha Surendren, and Dr. Neethu Antony, Central Institute of Plastics Engineering and Technology (CIPET) Kochi for their analytical services and technical support provided throughout the research work.

Author information

Authors and Affiliations

  1. Central Institute of Petrochemicals Engineering and Technology (CIPET), Eloor, Udyogamandal P.O., Kochi, Kerala, 683501, India

    K. A. Rajesh, Saranya A. Kartha, Merlin N. Issac & T. O. Varghese

Authors
  1. K. A. Rajesh
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. Saranya A. Kartha
    View author publications

    You can also search for this author in PubMed Google Scholar

  3. Merlin N. Issac
    View author publications

    You can also search for this author in PubMed Google Scholar

  4. T. O. Varghese
    View author publications

    You can also search for this author in PubMed Google Scholar

Corresponding author

Correspondence to K. A. Rajesh.

Ethics declarations

Conflict of interest

All authors declare that they have no conflict of interest.

Rights and permissions

Springer Nature or its licensor (e.g. a society or other partner) holds exclusive rights to this article under a publishing agreement with the author(s) or other rightsholder(s); author self-archiving of the accepted manuscript version of this article is solely governed by the terms of such publishing agreement and applicable law.

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Rajesh, K.A., Kartha, S.A., Issac, M.N. et al. Biosourced epoxidized neem oil toughened poly(lactic acid) for agricultural applications: mechanical, thermal and compostability properties. Iran Polym J 32, 275–285 (2023). https://doi.org/10.1007/s13726-022-01126-9

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s13726-022-01126-9

Keywords

Search

Navigation