, Volume 26, Issue 10, pp 5959–5979 | Cite as

Extraction and characterization of nanocellulose crystals from cotton gin motes and cotton gin waste

  • Jacobs H. Jordan
  • Michael W. EassonEmail author
  • Bruce Dien
  • Stephanie Thompson
  • Brian D. Condon
Original Research


Cellulose nanocrystals (CNC) have attracted a great deal of attention as an environmentally-friendly biorenewable resource for use as reinforcing agents in nanocomposites, polymers, gels, and emulsions. CNCs are typically prepared from extracted cellulose or highly refined cellulose products. The chemical refining process can alter the chemical and physical properties of the cellulose fibers prior to extraction of CNCs. Moreover, the method of isolation can also insert various functional groups onto the nanocellulose, affecting thermal stability and imparting different physical properties. Herein, two byproducts of the cotton industry, cotton gin motes and cotton gin waste, are investigated for the preparation of nanocelluloses. Cellulose was purified from these two post-process agroindustrial by-products and CNCs subsequently produced by sulfuric acid hydrolysis. Additionally, two acid hydrolysis methods were utilized to successfully extract CNCs from gin motes without chemical pretreatment. CNCs were obtained with diameters < 10 nm and lengths of ca. 100–300 nm resulting in high aspect ratios (12–33). Incorporating CNCs with these dimensions impart increased hydrophilicity to a substrate. The effect of post-extraction chemical treatments on crystallinity and morphology are discussed. The extracted nanocellulose derivatives were additionally characterized by FTIR, AFM, TGA, DLS, XRD and XPS. Differences in extraction method and chemical treatment resulted in different thermal properties and colloidal stability. Furthermore, this work provides a means of producing a high value commodity from inexpensive source materials such as cotton gin motes and cotton gin waste.


Agroindustrial waste Cellulose nanocrystals (CNC) Cotton Cellulose Nanocellulose Bioproducts 



The authors would like to thank Al French for assistance with analysis of XRD patterns, and Dongmei Cao at the LSU Shared Instrument Facility for data collection. Additionally, the authors would like to thank the National Program Staff, the Mid-South Area Director, and the Center Director of the Agricultural Research Service of the U.S. Department of Agriculture for providing the necessary support for the study presented here. The Southern Regional Research Center is a federal research facility of the U.S. Department of Agriculture in New Orleans, LA. The names of the companies and/or their products are mentioned solely for the purpose of providing information and do not in any way imply their recommendation or endorsement by the USDA over others.

Supplementary material

10570_2019_2533_MOESM1_ESM.docx (618 kb)
Supplementary material 1 (DOCX 618 kb)


  1. Agarwal UP, Ralph SA, Reiner RS, Hunt CG, Baez C, Ibach R, Hirth KC (2018) Production of high lignin-containing and lignin-free cellulose nanocrystals from wood. Cellulose 25:5791–5805. CrossRefGoogle Scholar
  2. Agblevor FA, Batz S, Trumbo J (2003) Composition and ethanol production potential of cotton gin residues. Appl Biochem Biotechnol 105–108:219–230CrossRefGoogle Scholar
  3. Alemdar A, Sain M (2008) Isolation and characterization of nanofibers from agricultural residues: wheat straw and soy hulls. Biores Technol 99:1664–1671. CrossRefGoogle Scholar
  4. Araki J, Wada M, Kuga S, Okano T (1998) Flow properties of microcrystalline cellulose suspension prepared by acid treatment of native cellulose. Colloids Surf A 142:75–82. CrossRefGoogle Scholar
  5. Bajwa SG, Bajwa DS, Holt G, Coffelt T, Nakayama F (2011) Properties of thermoplastic composites with cotton and guayule biomass residues as fiber fillers. Ind Crops Prod 33:747–755. CrossRefGoogle Scholar
  6. Baumann H, Richter A, Klemm D, Faust V (2000) Concepts for preparation of novel regioselective modified cellulose derivatives sulfated, aminated, carboxylated and acetylated for hemocompatible ultrathin coatings on biomaterials. Macromol Chem Phys 201:1950–1962.;2-3 CrossRefGoogle Scholar
  7. Ben Ayed E, Cochereau R, Dechance C, Capron I, Nicolai T, Benyahia L (2018) Water-In-Water Emulsion Gels Stabilized by Cellulose Nanocrystals. Langmuir 34:6887–6893. CrossRefGoogle Scholar
  8. Bhattacharjee S (2016) DLS and zeta potential – What they are and what they are not? J Controlled Release 235:337–351. CrossRefGoogle Scholar
  9. Boluk Y, Danumah C (2013) Analysis of cellulose nanocrystal rod lengths by dynamic light scattering and electron microscopy. J Nanopart Res 16:2174. CrossRefGoogle Scholar
  10. Brinchi L, Cotana F, Fortunati E, Kenny JM (2013) Production of nanocrystalline cellulose from lignocellulosic biomass: technology and applications. Carbohyd Polym 94:154–169. CrossRefGoogle Scholar
  11. Camarero Espinosa S, Kuhnt T, Foster EJ, Weder C (2013) Isolation of thermally stable cellulose nanocrystals by phosphoric acid hydrolysis. Biomacromol 14:1223–1230. CrossRefGoogle Scholar
  12. de Campos A et al (2013) Obtaining nanofibers from curaua and sugarcane bagasse fibers using enzymatic hydrolysis followed by sonication. Cellulose 20:1491–1500. CrossRefGoogle Scholar
  13. de Morais Teixeira E, Corrêa AC, Manzoli A, de Lima Leite F, de Oliveira CR, Mattoso LHC (2010) Cellulose nanofibers from white and naturally colored cotton fibers. Cellulose 17:595–606. CrossRefGoogle Scholar
  14. Dufresne A (2017) Cellulose nanomaterial reinforced polymer nanocomposites. Curr Opin Colloid Interface Sci 29:1–8. CrossRefGoogle Scholar
  15. Edwards V et al (2015) An assessment of surface properties and moisture uptake of nonwoven fabrics from ginning by-products. In: 2015. InTech, pp 45–61.
  16. Flauzino Neto WP et al (2016) Mechanical properties of natural rubber nanocomposites reinforced with high aspect ratio cellulose nanocrystals isolated from soy hulls. Carbohydr Polym 153:143–152. CrossRefGoogle Scholar
  17. Foster EJ et al (2018) Current characterization methods for cellulose nanomaterials. Chem Soc Rev 47:2609–2679. CrossRefGoogle Scholar
  18. French AD (2014) Idealized powder diffraction patterns for cellulose polymorphs. Cellulose 21:885–896. CrossRefGoogle Scholar
  19. Hamad WY, Hu TQ (2010) Structure-process-yield interrelations in nanocrystalline cellulose extraction. Can J Chem Eng 88:392–402. Google Scholar
  20. Han J, Zhou C, Wu Y, Liu F, Wu Q (2013) Self-assembling behavior of cellulose nanoparticles during freeze-drying: effect of suspension concentration, particle size, crystal structure, and surface charge. Biomacromol 14:1529–1540. CrossRefGoogle Scholar
  21. Hasani M, Cranston ED, Westman G, Gray DG (2008) Cationic surface functionalization of cellulose nanocrystals. Soft Matter 4:2238–2244. CrossRefGoogle Scholar
  22. Holt G, Simonton MG, Canto A (2004) Utilization of cotton gin by-products for the manufacturing of fuel pellets: an economic perspective. Appl Eng Agric 20:423–430Google Scholar
  23. Johar N, Ahmad I, Dufresne A (2012) Extraction, preparation and characterization of cellulose fibers and nanocrystals from rice husk. Ind Crops Prod 37:93–99. CrossRefGoogle Scholar
  24. Kargarzadeh H, Ahmad I, Abdullah I, Dufresne A, Zainudin SY, Sheltami RM (2012) Effects of hydrolysis conditions on the morphology, crystallinity, and thermal stability of cellulose nanocrystals extracted from kenaf bast fibers. Cellulose 19:855–866. CrossRefGoogle Scholar
  25. Kargarzadeh H et al (2018) Advances in cellulose nanomaterials. Cellulose 25:2151–2189. CrossRefGoogle Scholar
  26. Klemm D et al (2018) Nanocellulose as a natural source for groundbreaking applications in materials science. Today’s State Mater Today 21:720–748. CrossRefGoogle Scholar
  27. Kloser E, Gray DG (2010) Surface Grafting of Cellulose Nanocrystals with Poly(ethylene oxide) in Aqueous Media. Langmuir 26:13450–13456. CrossRefGoogle Scholar
  28. Kontturi E et al (2018) Advanced Materials through Assembly of Nanocelluloses. Adv Mater 30:e1703779CrossRefGoogle Scholar
  29. Lin N, Dufresne A (2014) Surface chemistry, morphological analysis and properties of cellulose nanocrystals with gradiented sulfation degrees. Nanoscale 6:5384–5393. CrossRefGoogle Scholar
  30. Ling Z et al (2018) Structural variations of cotton cellulose nanocrystals from deep eutectic solvent treatment: micro and nano scale. Cellulose. (Ahead of Print) Google Scholar
  31. (2018) Nanocellulose market by type, application, and region—global forecast to 2023. MarketsandMarketsGoogle Scholar
  32. Morais JP, de Freitas Rosa M, Nascimento LD, do Nascimento DM, Cassales AR (2013) Extraction and characterization of nanocellulose structures from raw cotton linter. Carbohyd Polym 91:229–235. CrossRefGoogle Scholar
  33. Nam S, French AD, Condon BD, Concha M (2016) Segal crystallinity index revisited by the simulation of X-ray diffraction patterns of cotton cellulose Iβ and cellulose II. Carbohyd Polym 135:1–9. CrossRefGoogle Scholar
  34. Nascimento DM et al (2018) Nanocellulose nanocomposite hydrogels: technological and environmental issues. Green Chem 20:2428–2448. CrossRefGoogle Scholar
  35. (2019) Current lumber, pulp and panel prices. Natural Resources Canada.
  36. Ortega A, Torre JG (2003) Hydrodynamic properties of rodlike and disklike particles in dilute solution. J Chem Phys 119:9914–9919. CrossRefGoogle Scholar
  37. Oun AA, Rhim J-W (2015) Effect of post-treatments and concentration of cotton linter cellulose nanocrystals on the properties of agar-based nanocomposite films. Carbohydr Polym 134:20–29. CrossRefGoogle Scholar
  38. Reid MS, Villalobos M, Cranston ED (2017) Benchmarking Cellulose Nanocrystals: From the Laboratory to Industrial Production. Langmuir 33:1583–1598. CrossRefGoogle Scholar
  39. Rösslein M, Wick P, Prina-Mello A (2018) Characterisation of particles in solution—a perspective on light scattering and comparative technologies. Sci Technol Adv Mater 19:732–745. CrossRefGoogle Scholar
  40. Sacui IA et al (2014) Comparison of the properties of cellulose nanocrystals and cellulose nanofibrils isolated from bacteria, tunicate, and wood processed using acid, enzymatic, mechanical, and oxidative methods. ACS Appl Mater Interfaces 6:6127–6138. CrossRefGoogle Scholar
  41. Saito T, Isogai A (2004) TEMPO-Mediated Oxidation of Native Cellulose. The Effect of Oxidation Conditions on Chemical and Crystal Structures of the Water-Insoluble Fractions. Biomacromol 5:1983–1989. CrossRefGoogle Scholar
  42. Saito T, Nishiyama Y, Putaux J-L, Vignon M, Isogai A (2006) Homogeneous Suspensions of Individualized Microfibrils from TEMPO-Catalyzed Oxidation of Native Cellulose. Biomacromol 7:1687–1691. CrossRefGoogle Scholar
  43. Sawhney P, Allen H, Reynolds M, Slopek R, Condon B, Hui D, Wojkowski S (2012) Effect of web formation on properties of hydroentangled nonwoven fabrics. World J Eng 9:407–416. CrossRefGoogle Scholar
  44. Sawhney P, Allen C, Reynolds M, Slopek R, Condon B (2013) Whiteness and absorbency of hydroentangled cotton-based nonwoven fabrics of different constituent fibers and fiber blends. World J Eng 10:125–132. CrossRefGoogle Scholar
  45. Segal L, Creely JJ, Martin AE, Conrad CM (1959) An Empirical Method for Estimating the Degree of Crystallinity of Native Cellulose Using the X-Ray Diffractometer. Text Res J 29:786–794. CrossRefGoogle Scholar
  46. Sheltami RM, Abdullah I, Ahmad I, Dufresne A, Kargarzadeh H (2012) Extraction of cellulose nanocrystals from mengkuang leaves (Pandanus tectorius). Carbohydr Polym 88:772–779. CrossRefGoogle Scholar
  47. Shimizu M, Fukuzumi H, Saito T, Isogai A (2013) Preparation and characterization of TEMPO-oxidized cellulose nanofibrils with ammonium carboxylate groups. Int J Biol Macromol 59:99–104. CrossRefGoogle Scholar
  48. Siqueira G, Bras J, Dufresne A (2010) Cellulosic bionanocomposites: a review of preparation, properties and applications. Polymers 2:728–765. CrossRefGoogle Scholar
  49. Sluiter A, Hames B, Ruiz R, Scarlata C, Sluiter J, Templeton D, Crocker D (2008) Determination of structural carbohydrates and lignin in biomass. Denver, COGoogle Scholar
  50. Soni B, el Hassan B, Mahmoud B (2015) Chemical isolation and characterization of different cellulose nanofibers from cotton stalks. Carbohyd Polym 134:581–589. CrossRefGoogle Scholar
  51. (2018) Cotton production in the U.S. from 2000 to 2017.
  52. Stewart L (2010) Using cotton byproducts in beef cattle diets. University of GeorgiaGoogle Scholar
  53. Thambiraj S, Ravi Shankaran D (2017) Preparation and physicochemical characterization of cellulose nanocrystals from industrial waste cotton. Appl Surf Sci 412:405–416. CrossRefGoogle Scholar
  54. Theivasanthi T, Anne Christma FL, Toyin AJ, Gopinath SCB, Ravichandran R (2018) Synthesis and characterization of cotton fiber-based nanocellulose. Int J Biol Macromol 109:832–836. CrossRefGoogle Scholar
  55. Valentini L, Cardinali M, Fortunati E, Kenny JM (2014) Nonvolatile memory behavior of nanocrystalline cellulose/graphene oxide composite films. Appl Phys Lett 105:153111. CrossRefGoogle Scholar
  56. Van Hai L, Son HN, Seo YB (2015) Physical and bio-composite properties of nanocrystalline cellulose from wood, cotton linters, cattail, and red algae. Cellulose 22:1789–1798. CrossRefGoogle Scholar
  57. Wang J, Yang Y, Yu M, Hu G, Gan Y, Gao H, Shi X (2018) Diffusion of rod-like nanoparticles in non-adhesive and adhesive porous polymeric gels. J Mech Phys Solids 112:431–457. CrossRefGoogle Scholar
  58. Zainuddin SYZ, Ahmad I, Kargarzadeh H, Abdullah I, Dufresne A (2013) Potential of using multiscale kenaf fibers as reinforcing filler in cassava starch-kenaf biocomposites. Carbohydr Polym 92:2299–2305. CrossRefGoogle Scholar
  59. Zhou L, He H, Li MC, Song K, Cheng HN, Wu Q (2016) Morphological influence of cellulose nanoparticles (CNs) from cottonseed hulls on rheological properties of polyvinyl alcohol/CN suspensions. Carbohyd Polym 153:445–454. CrossRefGoogle Scholar
  60. Zhou S, You T, Zhang X, Xu F (2018) Superhydrophobic Cellulose Nanofiber-Assembled Aerogels for Highly Efficient Water-in-Oil Emulsions Separation. ACS Appl Nano Mater 1:2095–2103. CrossRefGoogle Scholar

Copyright information

© This is a U.S. Government work and not under copyright protection in the US; foreign copyright protection may apply 2019

Authors and Affiliations

  1. 1.The Southern Regional Research Center, Agricultural Research ServiceUSDANew OrleansUSA
  2. 2.The National Center for Agricultural Utilization Research, Agricultural Research ServiceUSDAPeoriaUSA

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