, Volume 26, Issue 18, pp 9567–9581 | Cite as

Production of cellulose nanofibrils from alfa fibers and its nanoreinforcement potential in polymer nanocomposites

  • Zineb Kassab
  • Assya Boujemaoui
  • Hicham Ben Youcef
  • Abdelghani Hajlane
  • Hassan Hannache
  • Mounir El AchabyEmail author
Original Research


Alfa fibers (Stipa Tenacissima) were effectively utilized in this study as a promising cellulose source for isolation of carboxy-functionalized cellulose nanofibrils (CNFs) using multiple treatments. Pure cellulose microfibers (CMFs) were firstly extracted by alkali and bleaching treatments. CNFs with an average nanofibrils diameter ranging from 1.4 to 4.6 nm and a crystallinity of 89% were isolated from CMFs by a combination of TEMPO-oxidation and mechanical disintegration processes. The morphology and physico-chemical properties of cellulosic materials were evaluated at different stages of treatments using several characterization techniques. Various CNF loadings (5–15 wt%) were incorporated into PVA polymer to evaluate the nanoreinforcement ability of CNFs and to produce CNF-filled PVA nanocomposite materials. The tensile and optical transmittance properties, as well as the morphological and thermal properties of the as-produced CNF-filled PVA nanocomposite films were investigated. It was found that the tensile modulus and strength of nanocomposites were gradually increased with increasing of CNF loadings, with a maximum increase of 90% and 74% was observed for a PVA nanocomposite containing 15 wt% CNFs, respectively. The optical transmittance was reduced from 91% (at 650 nm) for neat PVA polymer to 88%, 82% and 76% for PVA nanocomposites containing 5, 10 and 15 wt% CNFs, respectively. It was also found that the glass transition temperature was gradually increased from 76 °C for neat PVA to 89 °C for PVA nanocomposite containing 15 wt%. This study demonstrates the importance of Alfa fibers as annual renewable lignocellulosic material to produce CNFs with good morphology and excellent properties. These newly developed carboxy-functionalized CNFs could be considered as a potential nanofiller candidate for the preparation of nanocomposite materials of high transparency and good mechanical properties.

Graphic abstract


Alfa fibers Cellulose nanofibrils Polymer nanocomposites Mechanical properties 



The financial assistance of the Office Chérifien des Phosphates (OCP S.A.) in the Moroccan Kingdom toward this research is hereby acknowledged. The authors would like to thank the Swedish Foundation for Strategic Research (SSF, Project Number 63634) and the Wallenberg Wood Science Centre (WWSC) for the financial support particularly during Kassab’s stay in KTH. Discussions with Prof L Berglund at KTH are gratefully acknowledged.


  1. Abitbol T, Johnstone T, Quinn TM, Gray DG (2011) Reinforcement with cellulose nanocrystals of poly(vinyl alcohol) hydrogels prepared by cyclic freezing and thawing. Soft Matter 7:2373–2379. CrossRefGoogle Scholar
  2. Belouadah Z, Ati A, Rokbi M (2015) Characterization of new natural cellulosic fiber from Lygeum spartum L. Carbohydr Polym 134:429–437. CrossRefPubMedGoogle Scholar
  3. Borchani KE, Carrot C, Jaziri M (2015) Untreated and alkali treated fibers from Alfa stem: effect of alkali treatment on structural, morphological and thermal features. Cellulose 22:1577–1589. CrossRefGoogle Scholar
  4. Boufi S, Kaddami H, Dufresne A (2014) Mechanical performance and transparency of nanocellulose reinforced polymer nanocomposites. Macromol Mater Eng 299:560–568. CrossRefGoogle Scholar
  5. Brinchi L, Cotana F, Fortunati E, Kenny JM (2013) Production of nanocrystalline cellulose from lignocellulosic biomass: technology and applications. Carbohydr Polym 94:154–169CrossRefGoogle Scholar
  6. Cao X, Ding B, Yu J, Al-Deyab SS (2012) Cellulose nanowhiskers extracted from TEMPO-oxidized jute fibers. Carbohydr Polym 90:1075–1080. CrossRefPubMedGoogle Scholar
  7. Chen YW, Lee HV, Abd Hamid SB (2017) Facile production of nanostructured cellulose from Elaeis guineensis empty fruit bunch via one pot oxidative-hydrolysis isolation approach. Carbohydr Polym 157:1511–1524. CrossRefPubMedGoogle Scholar
  8. Cho MJ, Park BD (2011) Tensile and thermal properties of nanocellulose-reinforced poly(vinyl alcohol) nanocomposites. J Ind Eng Chem 17:36–40. CrossRefGoogle Scholar
  9. Collazo-Bigliardi S, Ortega-Toro R, Chiralt Boix A (2018) Isolation and characterisation of microcrystalline cellulose and cellulose nanocrystals from coffee husk and comparative study with rice husk. Carbohydr Polym 191:205–215. CrossRefPubMedGoogle Scholar
  10. Curvello R, Raghuwanshi VS, Garnier G (2019) Engineering nanocellulose hydrogels for biomedical applications. Adv Colloid Interface Sci 267:47–61. CrossRefPubMedGoogle Scholar
  11. Dong H, Sliozberg YR, Snyder JF et al (2015) Highly transparent and toughened poly(methyl methacrylate) nanocomposite films containing networks of cellulose nanofibrils. ACS Appl Mater Interfaces 7:25464–25472. CrossRefPubMedGoogle Scholar
  12. El Achaby M, El Miri N, Snik A et al (2016) Mechanically strong nanocomposite films based on highly filled carboxymethyl cellulose with graphene oxide. J Appl Polym Sci 133:1–11. CrossRefGoogle Scholar
  13. El Achaby M, El Miri N, Hannache H et al (2018a) Cellulose nanocrystals from Miscanthus fibers: insights into rheological, physico-chemical properties and polymer reinforcing ability. Cellulose 25:6603–6619. CrossRefGoogle Scholar
  14. El Achaby M, El Miri N, Hannache H et al (2018b) Production of cellulose nanocrystals from vine shoots and their use for the development of nanocomposite materials. Int J Biol Macromol 117:592–600. CrossRefPubMedGoogle Scholar
  15. El Achaby M, Kassab Z, Aboulkas A et al (2018c) Reuse of red algae waste for the production of cellulose nanocrystals and its application in polymer nanocomposites. Int J Biol Macromol 106:681–691. CrossRefPubMedGoogle Scholar
  16. El Achaby M, Kassab Z, Barakat A, Aboulkas A (2018d) Alfa fibers as viable sustainable source for cellulose nanocrystals extraction: application for improving the tensile properties of biopolymer nanocomposite films. Ind Crops Prod 112:499–510. CrossRefGoogle Scholar
  17. El Miri N, Abdelouahdi K, Zahouily M et al (2015) Bio-nanocomposite films based on cellulose nanocrystals filled polyvinyl alcohol/chitosan polymer blend. J Appl Polym Sci 132:1–13. CrossRefGoogle Scholar
  18. Endo R, Saito T, Isogai A (2013) TEMPO-oxidized cellulose nanofibril/poly(vinyl alcohol) composite drawn fibers. Polymer (Guildf) 54:935–941. CrossRefGoogle Scholar
  19. Ferrer A, Pal L, Hubbe M (2017) Nanocellulose in packaging: advances in barrier layer technologies. Ind Crops Prod 95:574–582. CrossRefGoogle Scholar
  20. Fortunati E, Puglia D, Luzi F et al (2013) Binary PVA bio-nanocomposites containing cellulose nanocrystals extracted from different natural sources: part I. Carbohydr Polym 97:825–836. CrossRefPubMedGoogle Scholar
  21. French AD (2014) Idealized powder diffraction patterns for cellulose polymorphs. Cellulose 21:885–896. CrossRefGoogle Scholar
  22. French AD, Santiago Cintrón M (2013) Cellulose polymorphy, crystallite size, and the Segal Crystallinity Index. Cellulose 20:583–588. CrossRefGoogle Scholar
  23. Gazzotti S, Rampazzo R, Hakkarainen M et al (2019) Cellulose nanofibrils as reinforcing agents for PLA-based nanocomposites: an in situ approach. Compos Sci Technol 171:94–102. CrossRefGoogle Scholar
  24. Goetz LA, Naseri N, Nair SS et al (2018) All cellulose electrospun water purification membranes nanotextured using cellulose nanocrystals. Cellulose 25:3011–3023. CrossRefGoogle Scholar
  25. Guo C, Zhou L, Lv J (2013) Effects of expandable graphite and modified ammonium polyphosphate on the flame-retardant and mechanical properties of wood flour-polypropylene composites. Polym Polym Compos 21:449–456. CrossRefGoogle Scholar
  26. Hamou KB, Kaddami H, Dufresne A et al (2018) Impact of TEMPO-oxidization strength on the properties of cellulose nanofibril reinforced polyvinyl acetate nanocomposites. Carbohydr Polym 181:1061–1070. CrossRefPubMedGoogle Scholar
  27. Jose J, Thomas V, Vinod V et al (2019) Nanocellulose based functional materials for supercapacitor applications. J Sci Adv Mater Devices. CrossRefGoogle Scholar
  28. Joy J, Jose C, Yu X et al (2017) The influence of nanocellulosic fiber, extracted from Helicteres isora, on thermal, wetting and viscoelastic properties of poly(butylene succinate) composites. Cellulose 24:4313–4323. CrossRefGoogle Scholar
  29. Kadem S, Irinislimane R, Belhaneche-Bensemra N (2018) Novel biocomposites based on sunflower oil and alfa fibers as renewable resources. J Polym Environ 26:3086–3096. CrossRefGoogle Scholar
  30. Kassab Z, Aziz F, Hannache H et al (2019a) Improved mechanical properties of k-carrageenan-based nanocomposite films reinforced with cellulose nanocrystals. Int J Biol Macromol 123:1248–1256. CrossRefPubMedGoogle Scholar
  31. Kassab Z, El Achaby M, Tamraoui Y et al (2019b) Sunflower oil cake-derived cellulose nanocrystals: extraction, physico-chemical characteristics and potential application. Int J Biol Macromol 136:241–252. CrossRefPubMedGoogle Scholar
  32. Kılınç AÇ, Köktaş S, Seki Y et al (2018) Extraction and investigation of lightweight and porous natural fiber from Conium maculatum as a potential reinforcement for composite materials in transportation. Compos Part B Eng 140:1–8. CrossRefGoogle Scholar
  33. Koga H, Saito T, Kitaoka T et al (2013) Transparent, conductive, and printable composites consisting of TEMPO-oxidized nanocellulose and carbon nanotube. Biomacromolecules 14:1160–1165. CrossRefPubMedGoogle Scholar
  34. Kumar A, Negi YS, Choudhary V, Bhardwaj NK (2014) Characterization of cellulose nanocrystals produced by acid-hydrolysis from sugarcane bagasse as agro-waste. J Mater Phys Chem 2:1–8. CrossRefGoogle Scholar
  35. Lam NT, Chollakup R, Smitthipong W et al (2017) Characterization of cellulose nanocrystals extracted from sugarcane bagasse for potential biomedical materials. Sugar Tech 19:539–552. CrossRefGoogle Scholar
  36. Lasseuguette E (2008) Grafting onto microfibrils of native cellulose. Cellulose 15:571–580. CrossRefGoogle Scholar
  37. Li W, Wu Q, Zhao X et al (2014) Enhanced thermal and mechanical properties of PVA composites formed with filamentous nanocellulose fibrils. Carbohydr Polym 113:403–410. CrossRefPubMedGoogle Scholar
  38. Liu D, Sun X, Tian H et al (2013) Effects of cellulose nanofibrils on the structure and properties on PVA nanocomposites. Cellulose 20:2981–2989. CrossRefGoogle Scholar
  39. Liu D, Bian Q, Li Y et al (2016) Effect of oxidation degrees of graphene oxide on the structure and properties of poly (vinyl alcohol) composite films. Compos Sci Technol 129:146–152. CrossRefGoogle Scholar
  40. Mabrouk AB, Kaddami H, Boufi S et al (2012) Cellulosic nanoparticles from alfa fibers (Stipa tenacissima): extraction procedures and reinforcement potential in polymer nanocomposites. Cellulose 19:843–853. CrossRefGoogle Scholar
  41. Mandal A, Chakrabarty D (2011) Isolation of nanocellulose from waste sugarcane bagasse (SCB) and its characterization. Carbohydr Polym 86:1291–1299. CrossRefGoogle Scholar
  42. Panyasiri P, Yingkamhaeng N, Lam NT, Sukyai P (2018) Extraction of cellulose nanofibrils from amylase-treated cassava bagasse using high-pressure homogenization. Cellulose 25:1757–1768. CrossRefGoogle Scholar
  43. Poyraz B, Tozluoğlu A, Candan Z et al (2017) Influence of PVA and silica on chemical, thermo-mechanical and electrical properties of Celluclast-treated nanofibrillated cellulose composites. Int J Biol Macromol 104:384–392. CrossRefPubMedGoogle Scholar
  44. Puangsin B, Soeta H, Saito T, Isogai A (2017) Characterization of cellulose nanofibrils prepared by direct TEMPO-mediated oxidation of hemp bast. Cellulose 24:3767–3775. CrossRefGoogle Scholar
  45. Qua EH, Hornsby PR, Sharma HSS et al (2009) Preparation and characterization of Poly(vinyl alcohol) nanocomposites made from cellulose nanofibers. J Appl Polym Sci 113:2238–2247. CrossRefGoogle Scholar
  46. Saito T, Kimura S, Nishiyama Y, Isogai A (2007) Cellulose nanofibers prepared by TEMPO-mediated oxidation of native cellulose. Biomacromolecules 8:2485–2491. CrossRefPubMedGoogle Scholar
  47. Singh S, Gaikwad KK, Lee YS (2018) Antimicrobial and antioxidant properties of polyvinyl alcohol bio composite films containing seaweed extracted cellulose nano-crystal and basil leaves extract. Int J Biol Macromol 107:1879–1887. CrossRefPubMedGoogle Scholar
  48. Tadokoro H, Seki S, Nitta I (1956) Some information on the infrared absorption spectrum of poly(vinyl alcohol) from deuteration and pleochroism. J Polym Sci 669:563–566. CrossRefGoogle Scholar
  49. Thomas B, Raj MC, Athira KB et al (2018) Nanocellulose, a versatile green platform: from biosources to materials and their applications. Chem Rev 118:11575–11625. CrossRefPubMedGoogle Scholar
  50. Trache D (2018) Nanocellulose as a promising sustainable material for biomedical applications. AIMS Mater Sci 5:201–205. CrossRefGoogle Scholar
  51. Trache D, Donnot A, Khimeche K et al (2014) Physico-chemical properties and thermal stability of microcrystalline cellulose isolated from Alfa fibres. Carbohydr Polym 104:223–230. CrossRefPubMedGoogle Scholar
  52. Trache D, Hussin MH, Hui Chuin CT et al (2016a) Microcrystalline cellulose: isolation, characterization and bio-composites application—a review. Int J Biol Macromol 93:789–804. CrossRefPubMedGoogle Scholar
  53. Trache D, Khimeche K, Mezroua A, Benziane M (2016b) Physicochemical properties of microcrystalline nitrocellulose from Alfa grass fibres and its thermal stability. J Therm Anal Calorim 124:1485–1496. CrossRefGoogle Scholar
  54. Trache D, Hussin MH, Haafiz MKM, Thakur VK (2017) Recent progress in cellulose nanocrystals: sources and production. Nanoscale 9:1763–1786. CrossRefPubMedGoogle Scholar
  55. Wang Z, Qiao X, Sun K (2018) Rice straw cellulose nanofibrils reinforced poly(vinyl alcohol) composite films. Carbohydr Polym 197:442–450. CrossRefPubMedGoogle Scholar
  56. Wei Q, Tao D, Xu Y (2012) Nanofibers: principles and manufacture. Funct Nanofibers Their Appl. CrossRefGoogle Scholar
  57. Wu J, Du X, Yin Z et al (2019a) Preparation and characterization of cellulose nanofibrils from coconut coir fibers and their reinforcements in biodegradable composite films. Carbohydr Polym 211:49–56. CrossRefPubMedGoogle Scholar
  58. Wu T, Cai B, Wang J et al (2019b) TEMPO-oxidized cellulose nanofibril/layered double hydroxide nanocomposite films with improved hydrophobicity, flame retardancy and mechanical properties. Compos Sci Technol 171:111–117. CrossRefGoogle Scholar
  59. Wu Y, Tang Q, Yang F et al (2019c) Mechanical and thermal properties of rice straw cellulose nanofibrils-enhanced polyvinyl alcohol films using freezing-and-thawing cycle method. Cellulose 26:3193–3204. CrossRefGoogle Scholar
  60. Xiang Z, Gao W, Chen L et al (2016) A comparison of cellulose nanofibrils produced from Cladophora glomerata algae and bleached eucalyptus pulp. Cellulose 23:493–503. CrossRefGoogle Scholar
  61. Zhao Y, Moser C, Lindström ME et al (2017) Cellulose nanofibers from softwood, hardwood, and tunicate: preparation-structure-film performance interrelation. ACS Appl Mater Interfaces 9:13508–13519. CrossRefPubMedGoogle Scholar

Copyright information

© Springer Nature B.V. 2019

Authors and Affiliations

  1. 1.Materials Science and Nanoengineering Department (MSN)Mohammed VI Polytechnic University (UM6P)BenguerirMorocco
  2. 2.Laboratoire d’Ingénierie et Matériaux (LIMAT), Faculté des Sciences Ben M’sikUniversité Hassan II de CasablancaCasablancaMorocco
  3. 3.Wallenberg Wood Science Center, Department of Fiber and Polymer TechnologyKTH Royal Institute of TechnologyStockholmSweden

Personalised recommendations