, Volume 26, Issue 7, pp 4357–4369 | Cite as

Prevention of cellulose nanofibril agglomeration during dehydration and enhancement of redispersibility by hydrophilic gelatin

  • Hyo Won Kwak
  • Jinhwa You
  • Min Eui Lee
  • Hyoung-Joon JinEmail author
Original Research


Recently, nanocellulose has been used as a bio-polymer reinforcing agent. It is environment-friendly and has excellent performance owing to its unique nanostructure. However, during the drying and redispersion processes of nanocellulose, agglomeration of the nanocellulose occurs, which makes it difficult to store and transport. In this study, a nanocellulose drying system with an excellent redispersion rate and stability was prepared using fish-derived gelatin as a green, bio-polymer capping agent. The dispersion rate and stability of the nanocellulose, according to the ratio of gelatin and nanocellulose, were examined. After the dispersion, the removal of the gelatin was confirmed by FT-IR, TGA, and XRD. When 20% or more of the fish gelatin was added to the nanocellulose, the dried nanocellulose was redispersed within 30 min, and its stability was maintained for a long storage period. The gelatin was easily removed by washing with distilled water and filtrating, and the obtained nanocellulose recovered its original properties. The results herein revealed that the hydrophilic gelatin prevented the agglomeration of the nanocellulose during dehydration, and its redispersibility was enhanced. The drying method of the nanocellulose using the fish gelatin could contribute to the expansion of the nanocellulose applications by facilitating storage and transportation.

Graphical abstract


Fish gelatin Cellulose nanofibril (CNF) Redispersion 



This research was a part of the project titled ‘Performance improvement of Biodegradable fishing net and standardization’, funded by the Ministry of Oceans and Fisheries, Korea. This work was supported by a grant from the National Institute of Fisheries Science (R2019036). This study was also supported by a Basic Science Research Program through the National Research Foundation of Korea (NRF) funded by the Ministry of Education (NRF-2016R1A6A3A03008834).

Supplementary material

10570_2019_2387_MOESM1_ESM.docx (2 mb)
Supplementary material 1 (DOCX 2006 kb)


  1. Agarwal UP, Ralph SA, Baez C et al (2017) Effect of sample moisture content on XRD-estimated cellulose crystallinity index and crystallite size. Cellulose 24:1971–1984. CrossRefGoogle Scholar
  2. Ballesteros JEM, Santos SF, Mármol G et al (2015) Evaluation of cellulosic pulps treated by hornification as reinforcement of cementitious composites. Constr Build Mater 100:83–90. CrossRefGoogle Scholar
  3. Beaumont M, König J, Opietnik M et al (2017) Drying of a cellulose II gel: effect of physical modification and redispersibility in water. Cellulose 24:1199–1209. CrossRefGoogle Scholar
  4. Bruttini R, Crosser OK, Liapis AI (2001) Exergy analysis for the freezing stage of the freeze drying process. Dry Technol 19:2303–2313. CrossRefGoogle Scholar
  5. Butchosa N, Zhou Q (2014) Water redispersible cellulose nanofibrils adsorbed with carboxymethyl cellulose. Cellulose 21:4349–4358. CrossRefGoogle Scholar
  6. Chiou B-S, Avena-Bustillos RJ, Bechtel PJ et al (2009) Effects of drying temperature on barrier and mechanical properties of cold-water fish gelatin films. J Food Eng 95:327–331. CrossRefGoogle Scholar
  7. Favier V, Chanzy H, Cavaille JY (1995) Polymer nanocomposites reinforced by cellulose whiskers. Macromolecules 28:6365–6367. CrossRefGoogle Scholar
  8. Fernandes Diniz JMB, Gil MH, Castro JAAM (2004) Hornification—its origin and interpretation in wood pulps. Wood Sci Technol 37:489–494. CrossRefGoogle Scholar
  9. Ferrer A, Filpponen I, Rodríguez A et al (2012) Valorization of residual empty palm fruit bunch fibers (EPFBF) by microfluidization: production of nanofibrillated cellulose and EPFBF nanopaper. Bioresour Technol 125:249–255. CrossRefGoogle Scholar
  10. Fukuzumi H, Saito T, Isogai A (2013) Influence of TEMPO-oxidized cellulose nanofibril length on film properties. Carbohydr Polym 93:172–177. CrossRefGoogle Scholar
  11. Guo J, Filpponen I, Johansson L-S et al (2018) Micro-patterns on nanocellulose films and paper by photo-induced thiol–yne click coupling: a facile method toward wetting with spatial resolution. Cellulose 25:367–375. CrossRefGoogle Scholar
  12. Han J, Salmieri S, Le Tien C, Lacroix M (2010) Improvement of water barrier property of paperboard by coating application with biodegradable polymers. J Agric Food Chem 58:3125–3131. CrossRefGoogle Scholar
  13. Herrick FW, Casebier RL, Hamilton JK, Sandberg KR (1983) Microfibrillated cellulose: morphology and accessibility. J Appl Polym Sci Appl Polym Symp USA 37:797Google Scholar
  14. Hondros ED, Seah MP (1977) The theory of grain boundary segregation in terms of surface adsorption analogues. Metall Trans A 8:1363–1371. CrossRefGoogle Scholar
  15. Karayannakidis PD, Zotos A (2016) Fish processing by-products as a potential source of gelatin: a review. J Aquat Food Prod Technol 25:65–92. CrossRefGoogle Scholar
  16. Kargarzadeh H, Mariano M, Huang J et al (2017) Recent developments on nanocellulose reinforced polymer nanocomposites: a review. Polymer 132:368–393. CrossRefGoogle Scholar
  17. Ko C-H, Shie M-Y, Lin J-H et al (2017) Biodegradable bisvinyl sulfonemethyl-crosslinked gelatin conduit promotes regeneration after peripheral nerve injury in adult rats. Sci Rep 7:17489. CrossRefGoogle Scholar
  18. Kolman K, Nechyporchuk O, Persson M et al (2018) Combined nanocellulose/nanosilica approach for multiscale consolidation of painting canvases. ACS Appl Nano Mater 1:2036–2040. CrossRefGoogle Scholar
  19. Kruer-Zerhusen N, Cantero-Tubilla B, Wilson DB (2018) Characterization of cellulose crystallinity after enzymatic treatment using Fourier transform infrared spectroscopy (FTIR). Cellulose 25:37–48. CrossRefGoogle Scholar
  20. Kwak HW, Shin M, Lee JY et al (2017a) Fabrication of an ultrafine fish gelatin nanofibrous web from an aqueous solution by electrospinning. Int J Biol Macromol 102:1092–1103. CrossRefGoogle Scholar
  21. Kwak HW, Woo H, Kim I-C, Lee KH (2017b) Fish gelatin nanofibers prevent drug crystallization and enable ultrafast delivery. RSC Adv 7:40411–40417. CrossRefGoogle Scholar
  22. Lee WG, Kim DY, Kang SW (2018) Porous cellulose acetate by specific solvents with water pressure treatment for applications to separator and membranes. Macromol Res 26(7):630–633CrossRefGoogle Scholar
  23. Liapis AI, Pim ML, Bruttini R (1996) Research and development needs and opportunities in freeze drying. Dry Technol 14:1265–1300. CrossRefGoogle Scholar
  24. Lin N, Dufresne A (2014) Nanocellulose in biomedicine: current status and future prospect. Eur Polym J 59:302–325. CrossRefGoogle Scholar
  25. Morán JI, Alvarez VA, Cyras VP, Vázquez A (2008) Extraction of cellulose and preparation of nanocellulose from sisal fibers. Cellulose 15:149–159. CrossRefGoogle Scholar
  26. Ougiya H, Hioki N, Watanabe K et al (1998) Relationship between the physical properties and surface area of cellulose derived from adsorbates of various molecular sizes. Biosci Biotechnol Biochem 62:1880–1884. CrossRefGoogle Scholar
  27. Peng Y, Gardner DJ, Han Y (2012) Drying cellulose nanofibrils: in search of a suitable method. Cellulose 19:91–102. CrossRefGoogle Scholar
  28. Peng Y, Gardner DJ, Han Y et al (2013) Influence of drying method on the material properties of nanocellulose I: thermostability and crystallinity. Cellulose 20:2379–2392. CrossRefGoogle Scholar
  29. Pranoto Y, Lee CM, Park HJ (2007) Characterizations of fish gelatin films added with gellan and κ-carrageenan. LWT Food Sci Technol 40:766–774. CrossRefGoogle Scholar
  30. Qing Y, Sabo R, Wu Y et al (2015) Self-assembled optically transparent cellulose nanofibril films: effect of nanofibril morphology and drying procedure. Cellulose 22:1091–1102. CrossRefGoogle Scholar
  31. Siró I, Plackett D (2010) Microfibrillated cellulose and new nanocomposite materials: a review. Cellulose 17:459–494. CrossRefGoogle Scholar
  32. Spence KL, Venditti RA, Rojas OJ et al (2010) The effect of chemical composition on microfibrillar cellulose films from wood pulps: water interactions and physical properties for packaging applications. Cellulose 17:835–848. CrossRefGoogle Scholar
  33. Sun X, Wu Q, Zhang X et al (2018) Nanocellulose films with combined cellulose nanofibers and nanocrystals: tailored thermal, optical and mechanical properties. Cellulose 25:1103–1115. CrossRefGoogle Scholar
  34. Thimm JC, Burritt DJ, Ducker WA, Melton LD (2000) Celery (Apium graveolens L.) parenchyma cell walls examined by atomic force microscopy: effect of dehydration on cellulose microfibrils. Planta 212:25–32. CrossRefGoogle Scholar
  35. Turbak AF, Snyder FW, Sandberg KR (1983) Microfibrillated cellulose, a new cellulose product: properties, uses, and commercial potential. J Appl Polym Sci Appl Polym Symp USA 37:815Google Scholar
  36. Velásquez-Cock J, Gañán P, Gómez HC et al (2018a) Improved redispersibility of cellulose nanofibrils in water using maltodextrin as a green, easily removable and non-toxic additive. Food Hydrocoll 79:30–39. CrossRefGoogle Scholar
  37. Velásquez-Cock J, Gómez HBE, Posada P et al (2018b) Poly(vinyl alcohol) as a capping agent in oven dried cellulose nanofibrils. Carbohydr Polym 179:118–125. CrossRefGoogle Scholar
  38. Vu CM, Nguyen DD, Sinh LH, Choi HJ, Pham TD (2018) Micro-fibril cellulose as a filler for glass fiber reinforced unsaturated polyester composites: fabrication and mechanical characteristics. Macromol Res 26(1):54–60CrossRefGoogle Scholar
  39. Walton KS, Snurr RQ (2007) Applicability of the BET method for determining surface areas of microporous metal-organic frameworks. J Am Chem Soc 129:8552–8556. CrossRefGoogle Scholar
  40. Wang Q, Zhu JY, Considine JM (2013) Strong and optically transparent films prepared using cellulosic solid residue recovered from cellulose nanocrystals production waste stream. ACS Appl Mater Interfaces 5:2527–2534. CrossRefGoogle Scholar
  41. Wang Z, Yu J, Zhang L et al (2017) Cellulose laurate ester aerogel as a novel absorbing material for removing pollutants from organic wastewater. Cellulose 24:5069–5078. CrossRefGoogle Scholar
  42. Wu W, Dong Z, He J et al (2016) Transparent cellulose/laponite nanocomposite films. J Mater Sci 51:4125–4133. CrossRefGoogle Scholar
  43. Yang Q, Fukuzumi H, Saito T et al (2011) Transparent cellulose films with high gas barrier properties fabricated from aqueous alkali/urea solutions. Biomacromol 12:2766–2771. CrossRefGoogle Scholar
  44. Zhou Y, Jin Q, Zhu T, Akama Y (2011) Adsorption of chromium(VI) from aqueous solutions by cellulose modified with β-CD and quaternary ammonium groups. J Hazard Mater 187:303–310. CrossRefGoogle Scholar
  45. Zhuang C, Tao F, Cui Y (2015) Anti-degradation gelatin films crosslinked by active ester based on cellulose. RSC Adv 5:52183–52193. CrossRefGoogle Scholar

Copyright information

© Springer Nature B.V. 2019

Authors and Affiliations

  • Hyo Won Kwak
    • 1
    • 2
  • Jinhwa You
    • 3
  • Min Eui Lee
    • 3
  • Hyoung-Joon Jin
    • 3
    Email author
  1. 1.Department of Forest SciencesSeoul National UniversitySeoulKorea
  2. 2.Research Institute of Agriculture and Life SciencesSeoul National UniversitySeoulKorea
  3. 3.Department of Polymer Science and EngineeringInha UniversityIncheonKorea

Personalised recommendations