, Volume 25, Issue 10, pp 5751–5768 | Cite as

Dispersion, stability and size measurements for cellulose nanocrystals by static multiple light scattering

  • Mahyar Mazloumi
  • Linda J. JohnstonEmail author
  • Zygmunt J. Jakubek
Original Paper


Static multiple light scattering (SMLS) is used to provide qualitative information on cellulose nanocrystal (CNC) suspensions as a function of the methods used to disperse the dry CNCs and, in some cases, to estimate the equivalent size for primary particles and their aggregates. The methods were validated by measuring the mean diameter of several sizes and concentrations of silica particles which are approximately monodisperse and spherical, both of which significantly simplify the analysis of SMLS data. The results indicate that uncertainty in the silica density contributes to differences between the estimated SMLS diameters and those determined by dynamic light scattering. Suspension stability, sedimentation kinetics, and particle size as a function of dispersion method were evaluated for CNC suspensions by measuring the intensity profiles of light transmitted through the sample as a function of time, and applying sedimentation or light scattering theories. The results demonstrate that SMLS is a useful method for monitoring CNC dispersion for samples that are too concentrated to study by DLS. The sedimentation analysis provides qualitative information on the presence and size (equivalent diameter) of CNC aggregates/agglomerates and evidence for formation of a stable phase that forms during concurrent sedimentation and dispersion of CNC aggregates for unsonicated suspensions and is hypothesized to be a gel phase.


Cellulose nanocrystals Dispersion Static multiple light scattering 



We thank Formulaction staff for helpful discussions on the Turbiscan instrument and software.

Supplementary material

10570_2018_1961_MOESM1_ESM.pdf (576 kb)
Additional figures with SMLS results for silica and CNCs. (PDF 575 kb)


  1. Batchelor GK (1982) Sedimentation in a dilute polydisperse system of interacting spheres. Part 1. General theory. J Fluid Mech 119:379–408CrossRefGoogle Scholar
  2. Batchelor GK, Wen C-S (1982) Sedimentation in a dilute polydisperse system of interacting spheres. Part 2. Numerical results. J Fluid Mech 124:495–528CrossRefGoogle Scholar
  3. Beck S, Bouchard J, Berry R (2011) Controlling the reflection wavelength of iridescent solid films of nanocrystalline cellulose. Biomacromol 12:167–172CrossRefGoogle Scholar
  4. Beck S, Bouchard J, Berry R (2012) Dispersibility in water of dried nanocrystalline cellulose. Biomacromol 13:1486–1494CrossRefGoogle Scholar
  5. Brenner H (1974) Rheology of a dilute suspension of axisymmetric Brownian particles. Int Multiph Flow 1:195–341CrossRefGoogle Scholar
  6. Brinkmann A, Chen M, Couillard M, Jakubek ZJ, Leng T, Johnston LJ (2016) Correlating cellulose nanocrystal particle size and surface area. Langmuir 32:6105–6114CrossRefPubMedGoogle Scholar
  7. Buscall R, White LR (1987) The consolidation of concentrated suspensions. Part 1. The theory of sedimentation. J Chem Soc, Faraday Trans 1(83):873–891CrossRefGoogle Scholar
  8. Buscall R, Mills PD, Goodwin JW, Larson DW (1988) Scaling behaviour of the rheology of aggregate networks formed from colloidal particles. J Chem Soc, Faraday Trans 1(84):4249–4260CrossRefGoogle Scholar
  9. Cherhal F, Cousin F, Capron I (2015) Influence of charge density and ionic strength on the aggregation process of cellulose nanocrystals in aqueous suspension, as revealed by small-angle neutron scattering. Langmuir 31:5596–5602CrossRefPubMedGoogle Scholar
  10. Dong XM, Gray DG (1997) Effect of counterions on ordered phase formation in suspensions of charged rodlike cellulose crystallites. Langmuir 13:2404–2409CrossRefGoogle Scholar
  11. Dong XM, Revol J-F, Gray DG (1998) Effect of microcrystallite preparation conditions on the formation of colloid crystals of cellulose. Cellulose 5:19–32CrossRefGoogle Scholar
  12. Einstein A (1956) A new determination of molecular dimensions. In: Fürth R (ed) Investigations on the theory of the Brownian movement. Dover, New YorkGoogle Scholar
  13. Goscianska J, Olejnik A, Nowak I, Marciniak M, Pietrzak R (2016) Stability analysis of functionalized mesoporous carbon materials in aqueous solution. Chem Eng J 290:209–219CrossRefGoogle Scholar
  14. Hansen S (2004) Translational friction coefficients for cylinders of arbitrary axial ratios estimated by Monte Carlo simulation. J Chem Phys 121:91111–99115CrossRefGoogle Scholar
  15. Haywood AD, Weigandt KM, Saha P, Noor M, Green MJ, Davis VA (2017) New insights into the flow and microstructural relaxation behavior of biphasic cellulose nanocrystal disperisons from RheoSANS. Soft Matter 13:8451–8462CrossRefPubMedGoogle Scholar
  16. Jakubek ZJ, Chen M, Couillard M, Leng T, Liu L, Zou S, Baxa U, Clogston JD, Hamad W, Johnston LJ (2018) Characterization challenges for a cellulose nanocrystal reference material: dispersion and particle size distributions. J Nanopart Res 20:98CrossRefGoogle Scholar
  17. Kangas H, Lahtinen P, Sneck A, Saariaho A-M, Laitenen O, Hellen E (2014) Characterization of fibrillated celluloses. A short review and evaluation of characteristics with a combination of methods. Nord Pulp Paper J 29:129–143CrossRefGoogle Scholar
  18. Kimoto S, Dick WD, Hunt B, Szymanski WW, McMurry PH, Roberts DL, Pui DYH (2017) Characterization of nanosized silica size standards. Aerosol Sci Technol 51:936–945CrossRefGoogle Scholar
  19. Larson RG (1999) The structure and rheology of complex fluids. Oxford University Press, OxfordGoogle Scholar
  20. Lee SY, Widiyastuti W, Tajima N, Iskandar F, Okuyama K (2009) Measurement of the effective density of both spherical aggregated and ordered porous aerosol particles using mobility- and mass-analyzers. Aerosol Sci Technol 43:136–144CrossRefGoogle Scholar
  21. Mengual O, Cayré I, Puech K, Snabre P (1999) TURBISCAN MA 2000: multiple Light scattering measurement for concentrated emulsion and suspension instability analysis. Talanta 50:445–456CrossRefPubMedGoogle Scholar
  22. Mills P, Snabre P (1994) Settling of a suspension of hard spheres. Europhys Lett 25:651–656CrossRefGoogle Scholar
  23. Nordenstrom M, Fall A, Nystrom G, Wagberg L (2017) Formation of colloidal nanocellulose glasses and gels. Langmuir 33:9772–9780CrossRefPubMedGoogle Scholar
  24. Oguzlu H, Danumah C, Boluk Y (2016) The role of dilute and semi-dilute cellulose nanocrystal (CNC) suspensions on the rheology of carboxymethyl cellulose (CMC) solutions. Can J Chem Eng 94:1841–1847CrossRefGoogle Scholar
  25. Oguzlu H, Danumah C, Boluk Y (2017) Colloidal behavior of aqueous cellulose nanocrystal suspensions. Curr Opin Colloid Interface Sci 29:46–56CrossRefGoogle Scholar
  26. Olatunji ON, Du J, Hintz W, Tomas J (2016) Application of particle sedimentation analysis in sterically-stabilized TiO2 particles stability assessment. Adv Powder Technol 27:1325–1336CrossRefGoogle Scholar
  27. Pabst W, Gregorova E, Berthold C (2006) Particle shape and suspension rheology of short-fiber systems. J Eur Ceram Soc 26:149–160CrossRefGoogle Scholar
  28. Paximada P, Dimitrakopoulou EA, Tsouko E, Koutinas AA, Fasseas C, Mandala IG (2016) Structural modification of bacterial cellulose fibrils under ultrasonic irradiation. Carbohydr Polym 150:5–12CrossRefPubMedGoogle Scholar
  29. Peddireddy KR, Capron I, Nicolai T, Benyahia L (2016) Gelation kinetics and network structure of cellulose nanocrystals in aqueous solution. Biomacromol 2016:3298–3304CrossRefGoogle Scholar
  30. Reid MS, Villalobos M, Cranston ED (2016) Cellulose nanocrystal interactions probed by thin film swelling to predict dispersibility. Nanoscale 8:12247–12257CrossRefPubMedGoogle Scholar
  31. Sahlin K, Forsgren L, Moberg T, Bernin D, Rigdahl M, Westman G (2018) Surface treatment of cellulose nanocrystals (CNC): effects on dispersion rheology. Cellulose 25:331–345CrossRefGoogle Scholar
  32. Selim MS, Kothari AC, Turian RM (1983) Sedimentation of multisized particles in concentrated suspensions. AIChE J 29:1029–1038CrossRefGoogle Scholar
  33. Shafiei-Sabet S, Hamad WY, Hatzikiriakos SG (2012) Rheology of nanocrystalline cellulose aqueous suspensions. Langmuir 28:17124–17133CrossRefPubMedGoogle Scholar
  34. Sim K, Lee J, Lee H, Youn HJ (2015) Flocculation behavior of cellulose nanofibrils under different salt conditions and its impact on network strength and dewatering ability. Cellulose 22:3689–3700CrossRefGoogle Scholar
  35. Solomon MJ, Spicer PT (2010) Microstructural regimes of colloidal rod suspensions, gels, and glasses. Soft Matter 6:1391–1400CrossRefGoogle Scholar
  36. Stefaniak AB, Seehra MS, Fix NR, Leonard SS (2014) Lung biodurability and free radical production of cellulose nanomaterials. Inhal Toxicol 26:733–749CrossRefPubMedPubMedCentralGoogle Scholar
  37. Stickland AD, Buscall R (2009) Whither compressional rhelology? J Non-Newtonian Fluid Mech 157:151–157CrossRefGoogle Scholar
  38. Uhlig M, Fall A, Wellert S, Lehmann M, Prévost S, Wågberg L, von Klitzing R, Nyström G (2016) Two-dimensional aggregation and semidilute ordering in cellulose nanocrystals. Langmuir 32:442–450CrossRefPubMedGoogle Scholar
  39. Varanasi S, He R, Batchelor W (2013) Estimation of cellulose nanofibre aspect ratio from measurements of fibre suspension gel point. Cellulose 20:1885–1896CrossRefGoogle Scholar
  40. Yang H, Kang W, Yu Y, Yin X, Wang P, Zhang X (2017) A new approach to evaluate the particle growth and sedimentation of dispersed microsphere profile control system based on multiple light scattering. Powder Technol 315:477–485CrossRefGoogle Scholar

Copyright information

© Crown 2018

Authors and Affiliations

  1. 1.Measurement Science and StandardsNational Research Council CanadaOttawaCanada

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