, Volume 24, Issue 6, pp 2455–2468 | Cite as

Preparation and property assessment of neat lignocellulose nanofibrils (LCNF) and their composite films

  • Thomas Horseman
  • Mehdi TajvidiEmail author
  • Cherif I. K. Diop
  • Douglas J. Gardner
Original Paper


Lignocellulose nanofibrils (LCNF) were produced from thermo-mechanical pulp (TMP) using a micro-grinder and were characterized with respect to fiber diameter and thermal stability. The initial water content in the TMP affected the defibrillation process and longer grinding time was necessary for the air-dried TMP, resulting in LCNF with higher fibril diameter. As compared to the reference cellulose nanofibrils (CNF) produced through a refining process, LCNF was less thermally stable and started to degrade at a temperature that was 30 °C lower than that of CNF. LCNF obtained from the never-dried TMP was combined with various additives (10 wt%) to produce composite films. The neat LCNF and composite films did not reach the mechanical properties of the neat CNF film that was evaluated as reference. However, the addition of poly(vinyl alcohol) (PVA) at 10 wt% on a dry basis did cause a 46 and 25% increase in tensile strength and elastic modulus, respectively. Other additives including cellulose nanocrystals, bentonite and CNF were also found to increase to some extent the Young’s modulus and ductility of the LCNF composite films whereas the addition of talc did not improve the film performance. Water absorption of neat LCNF films was lower than the reference CNF and was negatively affected by the addition of PVA.


Mechanical fibrillation Lignocellulose nanofibrils Composite films Mechanical properties Thermal stability 



Funding for this research was provided by National Science Foundation (NSF) Grant # EEC-1461116 awarded to University of Maine Forest Bioproducts Research Institute (FBRI). The project was also partially funded by the University of Maine System Research Reinvestment Fund and Maine Economic Improvement Fund (MEIF).


  1. Belgacem K, Llewellyn P, NNahdi K, Trabelsi-Ayadi M (2008) Thermal behaviour study of the talc. Optoelectron Adv Mat Rapid Comm 2:332–336Google Scholar
  2. Bharimalla AK, Deshmukh SP, Patil PG, Vigneshwaran N (2015) Energy efficient manufacturing of nanocellulose by chemo- and bio-mechanical processes: a review. World J Nano Sci Eng 5:204–212. doi: 10.4236/wjnse.2015.54021 CrossRefGoogle Scholar
  3. Brebu M, Tamminen T, Spiridon I (2013) Thermal degradation of various lignins by TG-MS/FTIR and Py-GC-MS. J Anal Appl Pyrol 104:531–539CrossRefGoogle Scholar
  4. Carrillo Lugo CA (2014) Application of complex fluids in lignocellulose processing. Dissertation, North Carolina State University, 178 pGoogle Scholar
  5. Chirayil CJ, Mathew L, Thomas S (2014) Review of recent research in nano cellulose preparation from different lignocellulosic fibers. Rev Adv Mater Sci 37:20–28Google Scholar
  6. Diop CIK, Lavoie JM, Huneault MA (2015) Structural changes of Salix miyabeana cellulose fibres during dilute-acid steam explosion: impact of reaction temperature and retention time. Carbohyd Polym 119:8–17CrossRefGoogle Scholar
  7. Dufresne A (ed) (2013) Thermal degradation of cellulose. In: Nanocellulose: from nature to high performance tailored materials, chap 8.4.1. Walter de Gruyter GmbH, Berlin, p 283Google Scholar
  8. Ferrer A, Filpponen I, Rodríguez A, Laine J, Rojas OJ (2012) Valorization of residual Empty Palm Fruit Bunch Fibers (EPFBF) by microfluidization: production of nanofibrillated cellulose and EPFBF nanopaper. Bioresour Technol 125:249–255CrossRefGoogle Scholar
  9. Khalil HA, Davoudpour Y, Islam MN, Mustapha A, Sudesh K, Dungani R, Jawaid M (2014) Production and modification of nanofibrillated cellulose using various mechanical processes: a review. Carbohyd Polym 99:649–665CrossRefGoogle Scholar
  10. Kojima Y, Isa A, Kobori H, Suzuki S, Ito H, Makise R, Okamoto M (2014) Evaluation of binding effects in wood flour board containing ligno-cellulose nanofibers. Materials 7(9):6853–6864CrossRefGoogle Scholar
  11. Li W, Yue J, Liu S (2012) Preparation of nanocrystalline cellulose via ultrasound and its reinforcement capability for poly (vinyl alcohol) composites. Ultrason Sonochem 19(3):479–485CrossRefGoogle Scholar
  12. Liimatainen H, Ezekiel N, Sliz R, Ohenoja K, Sirviö JA, Berglund L, Hormi O, Niinimäki J (2013) High-strength nanocellulose–talc hybrid barrier films. ACS Appl Mater Interfaces 5(24):13412–13418CrossRefGoogle Scholar
  13. Madejova J, Komadel P (2001) Baseline studies of the clay minerals society source clays: infrared methods. Clay Clay Miner 49:410–432CrossRefGoogle Scholar
  14. Naderi A, Lindström T, Sundström J (2015) Repeated homogenization, a route for decreasing the energy consumption in the manufacturing process of carboxymethylated nanofibrillated cellulose. Cellulose 22(2):1147–1157CrossRefGoogle Scholar
  15. Nair SS, Yan N (2015) Effect of high residual lignin on the thermal stability of nanofibrils and its enhanced mechanical performance in aqueous environments. Cellulose 22(5):3137–3150CrossRefGoogle Scholar
  16. Osong SH (2014). Mechanical pulp based nano-ligno-cellulose: production, characterisation and their effect on paper properties. Thesis of the degree of Licentiate of Technology, Mid Sweden University, p 57Google Scholar
  17. Osong SH, Norgren S, Engstrand P (2013) An approach to produce nano-ligno-cellulose from mechanical pulp fine materials. Nord Pulp Pap Res J 28(4):472–479CrossRefGoogle Scholar
  18. Qing Y, Sabo R, Wu Y, Cai Z (2012) High-performance cellulose nanofibril composite films. BioResources 7(3):3064–3075Google Scholar
  19. Rojo E, Peresin MS, Sampson WW, Hoeger IC, Vartiainen J, Laine J, Rojas OJ (2015) Comprehensive elucidation of the effect of residual lignin on the physical, barrier, mechanical and surface properties of nanocellulose films. Green Chem 17(3):1853–1866CrossRefGoogle Scholar
  20. Sjöström E (1993) Wood chemistry: fundamentals and applications. Academic, New YorkGoogle Scholar
  21. Spence KL, Venditti RA, Rojas OJ, Habibi Y, Pawlak JJ (2010) The effect of chemical composition on microfibrillar cellulose films from wood pulps: water interactions and physical properties for packaging applications. Cellulose 17(4):835–848CrossRefGoogle Scholar
  22. Spence KL, Venditti RA, Rojas OJ, Habibi Y, Pawlak JJ (2011) A comparative study of energy consumption and physical properties of microfibrillated cellulose produced by different processing methods. Cellulose 18(4):1097–1111CrossRefGoogle Scholar
  23. Wear D, Prestemon J, Foster MO (2015) US forest products in the global economy. J For 114(4):483–493Google Scholar
  24. Xiao B, Sun X, Sun R (2001) Chemical, structural, and thermal characterizations of alkali-soluble lignins and hemicelluloses, and cellulose from maize stems, rye straw, and rice straw. Polym Degrad Stabil 74(2):307–319CrossRefGoogle Scholar
  25. Yang H, Yan R, Chen H, Lee DH, Zheng C (2007) Characteristics of hemicellulose, cellulose and lignin pyrolysis. Fuel 86(12):1781–1788CrossRefGoogle Scholar
  26. Yee TW, Choy LJ, Rahman WAWA (2011) Mechanical and water absorption properties of poly (vinyl alcohol)/sago pith waste biocomposites. J Compos Mater 45(11):1201–1207CrossRefGoogle Scholar

Copyright information

© Springer Science+Business Media Dordrecht 2017

Authors and Affiliations

  1. 1.Rose-Hulman Institute of TechnologyTerre HauteUSA
  2. 2.School of Forest Resources and Advanced Structures and Composites CenterUniversity of MaineOronoUSA
  3. 3.School of Forest ResourcesUniversity of MaineOronoUSA
  4. 4.School of Forest Resources and Advanced Structures and Composites CenterUniversity of MaineOronoUSA

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