Journal of Polymers and the Environment

, Volume 27, Issue 2, pp 395–404 | Cite as

Biodegradable Linseed Oil-Based Cross-Linked Polymer Composites Filled with Industrial Waste Materials for Mulching Coatings

  • Justina Vaicekauskaite
  • Jolita OstrauskaiteEmail author
  • Jolanta Treinyte
  • Violeta Grazuleviciene
  • Danguole Bridziuviene
  • Egidija Rainosalo
Original Paper


The aim of this work was preparation and initial investigation of biodegradable polymer composites from renewable recourses filled with industrial waste materials for potential application as mulching coatings. Crosslinked polymer of epoxidized linseed oil and 1-hydroxyethane-1,1-diphosphonic acid was used as polymeric binder in the prepared composites. The following industrial waste materials of natural origin were used as fillers: horn meal, phosphogypsum, rapeseed cake, pine needles, pine bark, grain mill waste, and mix of grain waste and weeds. The composite films can be formed in one day at (20–25) °C. The curing time was increased with an increase of dilution and amount of filler, as well as with reduction of temperature. Mechanical and thermal properties, moisture permeability, surface wetting, swelling in water, combustibility, and biodegradability of the formed polymer composite films were evaluated. It was found that mechanical characteristics of the prepared polymer composites deteriorated with increase of amount of filler. Tensile strength, Young modulus, and elongation at break of composite films were in the range of (0.3–1.8) MPa, (0.8–6.8) MPa, and (17–51) %, respectively. The values of wetting angle varied from 71° to 90° and were lower than that of commercial agrofoil. Swelling values were in the range of (2–22) % and depended on type and amount of filler, particle size, and hydrophobicity. The samples with lower amounts and less hydrophobic fillers having the higher particle size exhibited higher swelling values. Prepared composite films were found to be able to retain moisture in soil in 2–2.5 times more than soil without coating after 1 month, they were by ca. (4–20) % less flammable than conventional synthetic polymer films, biodegradable (their mass loss was (36–60) % during 6 months exposition in soil), and therefore could be applied as sprayable or pre-cured mulching films in agriculture and forestry.


Polymer composites Biopolymers and renewable polymers Crosslinking Biodegradable 



This work was supported by the Research Council of Lithuania [Grant Number MIP-066/2015]. José Antonio Reina form the University Rovira i Virgily, Spain, is gratefully acknowledged for the possibility to perform the limiting oxygen index test in his laboratory.


  1. 1.
    Hayes DG, Dharmalingam S, Wadsworth LC, Leonas KK, Miles C, Inglis DA (2012) Biodegradable agricultural mulches derived from biopolymers. In: Khemani K, Scholz C (eds) Degradable polymers and materials: principles and practice, 2nd edn. American Chemical Society, Washington, DCGoogle Scholar
  2. 2.
    Gurunathan T, Mohanty S, Nayak SK (2015) A review of the recent developments in biocomposites based on natural fibres and their application perspectives. Compos Part A 77:1–25CrossRefGoogle Scholar
  3. 3.
    Brodhagen M, Peyron M, Miles C, Inglis DA (2015) Biodegradable plastic agricultural mulches and key features of microbial degradation. Appl Microbiol Biotechnol 99:1039–1056CrossRefGoogle Scholar
  4. 4.
    Kasirajan S, Ngouajio M (2012) Polyethylene and biodegradable mulches for agricultural applications: a review. Agron Sustain Dev 32:501–529CrossRefGoogle Scholar
  5. 5.
    Yang N, Sun ZX, Feng LS, Zheng MZ, Chi DC, Meng WZ, Hou ZY, Bai W, Li KY (2015) Plastic film mulching for water-efficient agricultural applications and degradable films materials development research. Mater Manuf Process 30:143–154CrossRefGoogle Scholar
  6. 6.
    Steinmetz Z, Wollmann C, Schaefer M, Buchmann C, David J, Troeger J, Munoz K, Froer O, Schaumann GE (2016) Plastic mulching in agriculture. Trading short-term agronomic benefits for long-term soil degradation? Sci Total Environ 550:690–705CrossRefGoogle Scholar
  7. 7.
    Sartore L, Vox G, Schettini E (2013) Preparation and performance of novel biodegradable polymeric materials based on hydrolyzed proteins for agricultural application. J Polym Environ 21:718–725CrossRefGoogle Scholar
  8. 8.
    Vox G, Santagata G, Malinconico M, Immirzi B, Mugnozza GS, Schettini E (2013) Biodegradable films and spray coatings as eco-friendly alternative to petro-chemical derived mulching films. J Agr Eng 2013:e44Google Scholar
  9. 9.
    Immirzia B, Santagataa G, Vox G, Schettini E (2009) Preparation, characterisation and field-testing of a biodegradable sodium alginate-based spray mulch. Biosyst Eng 102:461–472CrossRefGoogle Scholar
  10. 10.
    Väisänen T, Haapala A, Lappalainen R, Tomppo L (2016) Utilization of agricultural and forest industry waste and residues in natural fiber-polymer composites: a review. Waste Manag 54:62–73CrossRefGoogle Scholar
  11. 11.
    Virtanen S, Chowreddy RR, Irmak S, Honkapaa K, Isom L (2016) Food industry co-streams: potential raw materials for biodegradable mulch film applications. J Polym Environ 25:1110–1130CrossRefGoogle Scholar
  12. 12.
    Bashir ASM, Manusamy Y (2015) Recent developments in biocomposites reinforced with natural biofillers from food waste. Polym-Plast Technol 54:87–99CrossRefGoogle Scholar
  13. 13.
    Saba N, Jawaid M, Alothman OY, Paridah MT, Hassan A (2016) Recent advances in epoxy resin, natural fiber-reinforced epoxy composites and their application. ‎J Reinf Plast Compos 35(6):447–470CrossRefGoogle Scholar
  14. 14.
    Zhang CH, Garrison TF, Madbouly SA, Kessler MR (2017) Recent advances in vegetable oil-based polymers and their composites. Prog Polym Sci 71:91–143CrossRefGoogle Scholar
  15. 15.
    Saba N, Tahir PM, jawaid M (2014) A review on potentiality of nano filler/natural fiber filled polymer hybrid composites. Polymers 6:2247–2273CrossRefGoogle Scholar
  16. 16.
    Samper MD, Petrucci R, Sanchez-Nacher L, Balart R, Kenny JM (2015) New environmentally friendly composite laminates with epoxidized linseed oil (ELO) and slate fiber fabrics. Compos B 71:203–209CrossRefGoogle Scholar
  17. 17.
    Ngo TT, Lambert CA, Kohl JG (2014) Characterization of compostability and mechanical properties for linseed oil resin composites reinforced with natural fibers. Polym Plast Technol Eng 53:1215–1222CrossRefGoogle Scholar
  18. 18.
    Pfister DP, Larock RC (2012) Cationically cured natural oil-based green composites: effect of the natural oil and the agricultural fiber. J Appl Polym Sci 123:1392–1400CrossRefGoogle Scholar
  19. 19.
    Rueda MM, Auscher MC, Fulchiron R, Perie T, Martin G, Sonntag P, Cassagnau P (2017) Rheology and applications of highly filled polymers: a review of current understanding. Prog Polym Sci 66:22–53CrossRefGoogle Scholar
  20. 20.
    Sobczak L, Bruggemann O, Putz RF (2013) Polyolefin composites with natural fibers and wood-modification of the fiber-filler-matrix interaction. J Appl Polym Sci 127:1–17CrossRefGoogle Scholar
  21. 21.
    Sartore L, Bignotti F, Pandini S, D’Amore A, Di Landro L (2016) Green composites and blends from leather industry waste. Polym Compos 37(12):3416–3422CrossRefGoogle Scholar
  22. 22.
    Adhikari R, Bristow KL, Casey PS, Freischmidt G, Hornbuckle JW, Adhikari B (2016) Preformed and sprayable polymeric mulch film to improve agricultural water use efficiency. Agr Water Manag 169:1–13CrossRefGoogle Scholar
  23. 23.
    Santagata G, Malinconico M, Immirzi B, Schettini E, Scarascia Mugnozza G, Vox G (2014) An overview of biodegradable films and spray coatings as sustainable alternative to oil-based mulching films. Acta Hortic 1037:921–928CrossRefGoogle Scholar
  24. 24.
    Johnston P, Freischmidt G, Easton CD, Greaves M, Casey PS, Bristow KL, Gunatillake PA, Adhikari R (2016) Hydrophobic-hydrophilic surface switching properties of nonchain extended poly(urethane)s for use in agriculture to minimize soil water evaporation and permit water infiltration. J Appl Polym Sci. Google Scholar
  25. 25.
    Adhikari R, Bristow KL, Casey PS, Freischmidt G, Hornbuckle JW (2015) Novel sprayable biodegradable polymer membrane to minimise soil evaporation. In: International Conference on Technologies for Sustainable Development (ICTSD 2015). Don Bosco Inst Technol DBIT, MumbaiGoogle Scholar
  26. 26.
    Malinconico M, Immirzi B, Santagata G, Schettini E, Vox G, Scarascia Mugnozza G (2008) An overview on innovative biodegradable materials for agricultural applications. In: Moeller HW (ed) Progress in polymer degradation and stability research. Nova Science, New YorkGoogle Scholar
  27. 27.
    Mosiewicki MA, Aranguren MI (2013) A short review on novel biocomposites based on plant oil precursors. Eur Polym J 49:1243–1256CrossRefGoogle Scholar
  28. 28.
    Biermann U, Bornscheuer U, Meier MAR, Metzger JO, Schafer HJ (2011) Oils and fats as renewable raw materials in chemistry. Angew Chem Int Ed 50:3854–3871CrossRefGoogle Scholar
  29. 29.
    Montero de Espinosa L, Meier MAR (2011) Plant oils: the perfect renewable resource for polymer science ? Eur Polym J 47:837–852CrossRefGoogle Scholar
  30. 30.
    Huang SW, Zhuo RX (2008) Recent advances in polyphosphoester and polyphosphoramidate-based biomaterials. Phosphorus Sulfur 183:340–348CrossRefGoogle Scholar
  31. 31.
    Wang YC, Yuan YY, Du JZ, Yang XZ, Wang J (2009) Recent progress in polyphosphoesters: from controlled synthesis to biomedical applications. Macromol Biosci 9:1154–1164CrossRefGoogle Scholar
  32. 32.
    Kasetaite S, Ostrauskaite J, Grazuleviciene V, Svediene J, Bridziuviene D (2014) Camelina oil- and linseed oil-based polymers with bisphosphonate crosslinks. J Appl Polym Sci. Google Scholar
  33. 33.
    ISO 846 (1997) Plastics—evaluation of the action of microorganismsGoogle Scholar
  34. 34.
    Chandra R, Rustgi R (1998) Biodegradable polymers. Prog Polym Sci 23:1273–1335CrossRefGoogle Scholar
  35. 35.
    Llevot A, Meier MAR (2016) Renewability—a principle of utmost importance! Green Chem 18:4800–4803CrossRefGoogle Scholar
  36. 36.
    Brown JE, Channell-Butcher C (2001) Black plastic mulch and drip irrigation affect growth and performance of bell pepper. J Veg Crop Prod 7:109–112CrossRefGoogle Scholar
  37. 37.
    Chalker-Scott L (2007) Impact of mulches on landscape plants and the environment—a review. J Environ Hortic 25:239–249Google Scholar
  38. 38.
    Mahmoudpour MA, Stapleton JJ (1997) Influence of sprayable mulch color on yield of eggplant (Solanum melongena L. cv. Millionaire). Sci Hortic 70:331–338CrossRefGoogle Scholar
  39. 39.
    Vox G, Scarascia Mugnozza G, Schettini E, de Palma L, Tarricone L, Gentilesco G, Vitali M (2012) Radiometric properties of plastic films for vineyard covering and their influence on vine physiology and production. Acta Hortic 956:465–472CrossRefGoogle Scholar
  40. 40.
    Schettini E, De Salvador FR, Scarascia-Mugnozza G, Vox G (2011) Radiometric properties of photoselective and photoluminescent greenhouse plastic films and their effects on peach and cherry tree growth. J Hortic Sci Biotechnol 86(1):79–83CrossRefGoogle Scholar
  41. 41.
    Schettini E, Vox G, De Lucia B (2007) Effects of the radiometric properties of innovative biodegradable mulching materials on snapdragon cultivation. Sci Hortic 112:456–461CrossRefGoogle Scholar
  42. 42.
    Tarara JM (2000) Microclimate modification with plastic mulch. Hortscience 35:169–180CrossRefGoogle Scholar
  43. 43.
    Mngomezulu ME, John MJ, Jacobs V, Luyt AS (2014) Review on flammability of biofibres and biocomposites. Carbohydr Polym 111:149–182CrossRefGoogle Scholar
  44. 44.
    Idumah CI, Hassan A (2016) Emerging trends in flame retardancy of biofibers, biopolymers, biocomposites, and bionanocomposites. Rev Chem Eng 32(1):115–148CrossRefGoogle Scholar
  45. 45.
    Younis AA (2017) Flammability properties of polypropylene containing montmorillonite and some of silicon compounds. Egypt J Petrol 26:1–7CrossRefGoogle Scholar
  46. 46.
    Merlini C, Soldi V, Barra GMO (2011) Influence of fiber surface treatment and length on physico-chemical properties of short random banana fiber-reinforced castor oil polyurethane composites. Polym Test 30:833–840CrossRefGoogle Scholar
  47. 47.
    Khot SN, Lascala JJ, Can E, Morye SS, Williams GI, Palmese GR, Kusefoglu SH, Wool RP (2001) Development and application of triglyceride-based polymers and composites. J Appl Polym Sci 82:703–723CrossRefGoogle Scholar
  48. 48.
    Casado U, Marcovich NE, Aranguren MI, Mosiewicki MA (2009) High strength composites based on tung oil polyurethane and wood flour: effect of the filler concentration on the mechanical properties. Polym Eng Sci 49(4):713–721CrossRefGoogle Scholar

Copyright information

© Springer Science+Business Media, LLC, part of Springer Nature 2018

Authors and Affiliations

  • Justina Vaicekauskaite
    • 1
  • Jolita Ostrauskaite
    • 1
    Email author
  • Jolanta Treinyte
    • 2
  • Violeta Grazuleviciene
    • 2
  • Danguole Bridziuviene
    • 3
  • Egidija Rainosalo
    • 4
  1. 1.Department of Polymer Chemistry and TechnologyKaunas University of TechnologyKaunasLithuania
  2. 2.Department of ChemistryAleksandras Stulginskis UniversityAkademijaLithuania
  3. 3.Biodeterioration Research LaboratoryNature Research CenterVilniusLithuania
  4. 4.Centria University of Applied SciencesKokkolaFinland

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