Springer Nature is making SARS-CoV-2 and COVID-19 research free. View research | View latest news | Sign up for updates

Hydrophobic wood flour derived from a novel p-TsOH treatment for improving interfacial compatibility of wood/HDPE composites

  • 17 Accesses


The interfacial compatibility between wood and polymers of wood/plastic composite (WPC) has been widely investigated. However, the reported methods for improvement of interfacial compatibility almost utilized the compatibilizer. In this work, a compatibilizer-free method was applied to enhance the interfacial compatibility between wood flour (WF) and high-density polyethylene (HDPE). p-toluenesulfonic acid (p-TsOH) was used to selectively remove hemicelulose, which would significantly improve the hydrophobicity of WF. It was found that most hemicellulose (about 91%) and a small amount of lignin were solubilized from WF. The static water contact angle (WCA) of WF sheet was significantly increased from nearly 0° to 135.7°, indicating that the WF was converted from hydrophilic to hydrophobic. Scanning electron microscope (SEM) showed p-TsOH treatment of WF could effectively improve the interfacial bonding between the WF and HDPE. The composite with 50 wt% modified-WF (MWF) showed optimum mechanical properties with an increase of 33.5% and 38.7% in tensile strength and flexural strength, respectively, as compared to those of corresponding WF/HDPE composite.

This is a preview of subscription content, log in to check access.

Fig. 1
Fig. 2
Fig. 3
Fig. 4
Fig. 5
Fig. 6
Fig. 7
Fig. 8
Fig. 9


  1. Ashori A, Nourbakhsh A (2008) Fundamental studies on wood–plastic composites: effects of fiber concentration and mixing temperature on the mechanical properties of poplar/PP composite. Polym Compos 29:569–573

  2. Bao Y, Qian H, Lu Z, Cui S (2015) Revealing the hydrophobicity of natural cellulose by single-molecule experiments. Macromolecules 48:3685

  3. Bengtsson M, Oksman K (2006) The use of silane technology in crosslinking polyethylene/wood flour composites. Compos Part A Appl Sci Manuf 37:752–765. https://doi.org/10.1016/j.compositesa.2005.06.014

  4. Bengtsson M, Gatenholm P, Oksman K (2005) The effect of crosslinking on the properties of polyethylene/wood flour composites. Compos Sci Technol 65:1468–1479. https://doi.org/10.1016/j.compscitech.2004.12.050

  5. Bengtsson M, Stark NM, Oksman K (2007) Durability and mechanical properties of silane cross-linked wood thermoplastic composites. Compos Sci Technol 67:2728–2738. https://doi.org/10.1016/j.compscitech.2007.02.006

  6. Bledzki AK, Gassan J, Theis S (1998) Wood-filled thermoplastic composites. Mech. Compos. Mater. 34:563–568. https://doi.org/10.1007/BF02254666

  7. Cantero G, Arbelaiz A, Llano-Ponte R, Mondragon I (2003) Effects of fibre treatment on wettability and mechanical behaviour of flax/polypropylene composites. Compos Sci Technol 63:1247–1254

  8. Chen T, Liu W, Qiu R (2013) Mechanical properties and water absorption of hemp fibers-reinforced unsaturated polyester composites: effect of fiber surface treatment with a heterofunctional monomer. BioResources 8:2780–2791

  9. Chen L, Dou J, Ma Q, Li N, Wu R, Bian H, Yelle DJ, Vuorinen T, Fu S, Pan X, Zhu JJY (2017) Rapid and near-complete dissolution of wood lignin at ≤ 80 °C by a recyclable acid hydrotrope. Sci Adv 3(9):e1701735. https://doi.org/10.1126/sciadv.1701735

  10. Coloma X, Carrascob F, Pagesc P, Canavate J (2003) Effects of different treatments on the interface of HDPE/lignocellulosic fifiber composites. Compos Sci Technol 63:161–169. https://doi.org/10.1016/S0266-3538(02)00248-8

  11. Croccolo D, Crupi V (2017) Special issue: wood science, engineering and technology. Proc IMechE Part C J Mech Eng Sci 1:3–4. https://doi.org/10.1177/0954406216680882

  12. Dai B, Wang Q, Yan W, Li Z, Guo W (2016) Synergistic compatibilization and reinforcement of HDPE/wood flour composites. J Appl Polym Sci. https://doi.org/10.1002/app.42958

  13. Dányádi L, Renner K, Móczó J (2007) Wood flour filled polypropylene composites: interfacial adhesion and micromechanical deformations. Polym Eng Sci 47:1246–1255. https://doi.org/10.1002/pen.20768

  14. Dong Y, Yan Y, Zhang S, Li J, Wang J (2015) Flammability and physical–mechanical properties assessment of wood treated with furfuryl alcohol and nano-SiO2. Eur J Wood Wood Prod 73:457–464. https://doi.org/10.1007/s00107-015-0896-y

  15. Essabir H, Raji M, Bouh R (2016) Nanoclay reinforced polymer composites. Nanoclay Reinf Polym Compos 1:29–49. https://doi.org/10.1007/978-981-10-1953-1

  16. Fei M, Xie T, Liu W, Chen H, Qiu R (2017) Surface grafting of bamboo fibers with 1,2-epoxy-4-vinylcyclohexane for reinforcing unsaturated polyester. Cellulose 2017(24):5505–5514. https://doi.org/10.1007/s10570-017-1497-1

  17. Frank E, Steudle L, Ingildeev D, Spörl J, Buchmeiser M (2014) Carbon fibers: precursor systems, processing, structure, and properties. Angew Chem Int Ed 53:5262–5298. https://doi.org/10.1002/anie.201306129

  18. Fukuzumi H, Saito T, Iwata T, Kumamoto Y, Isogai A (2009) Transparent and high gas barrier films of cellulose nanofibers prepared by TEMPO-mediated oxidation. Biomacromolecules 10:162–165. https://doi.org/10.1021/bm801065u

  19. Greenfeld I, Zhang W, Sui X, Wagner HD (2018) Intermittent beading in fiber composites. Compos Sci Technol 160:21–31. https://doi.org/10.1016/j.compscitech.2018.03.003

  20. Guimarães JL, Frollini E, Silva CG, Wypych F, Satyanarayana KG (2009) Characterization of banana, sugarcane bagasse and sponge gourd fibers of Brazil. Ind Crops Prod 30:407. https://doi.org/10.1016/j.indcrop.2009.07.013

  21. Haq M, Burgueño R, Mohanty AK, Misra M (2008a) Hybrid biobased composites from blends of unsaturated polyester and soybean oil reinforced with nanoclay and natural fibers. Compos Sci Technol 68:3344–3351. https://doi.org/10.1016/j.compscitech.2008.09.007

  22. Haq M, Burgueño R, Mohanty A, Misra M (2008b) Bio-based unsaturated polyester/layered silicate nanocomposites: characterization and thermo-physical properties. Compos Part A Appl Sci Manuf 40:540–547. https://doi.org/10.1016/j.compositesa.2009.02.008

  23. Hu W, Chen G, Liu Y, Liu Y, Li B, Fang Z (2018) Transparent and hazy all-cellulose composite films with superior mechanical properties. ACS Sustain Chem Eng 6:6974–6980. https://doi.org/10.1021/acssuschemeng.8b00814

  24. Ilona R, Endre A, Mirta IA, Norma EM (2009) Wood flour recycled polyol based polyurethane lightweight composites. J Compos Mater 43:2781–2884. https://doi.org/10.1177/0021998309345308

  25. Islam MS, Hamdan S, Jusoh I, Rahman MR, Ahmed AS (2011) The effect of alkali pretreatment on mechanical and morphological properties of tropical wood polymer composites. Mater Des 33:419–424. https://doi.org/10.1016/j.matdes.2011.04.044

  26. Kaya M (2018) Evaluation of a novel woody waste obtained from tea tree sawdust as an adsorbent for dye removal. Wood Sci Technol 52:245–260. https://doi.org/10.1007/s00226-017-0945-2

  27. Kim H, Okubo K, Fujii T, Takemura K (2013) Influence of fiber extraction and surface modification on mechanical properties of green composites with bamboo fiber. J Adhes Sci Technol 27:1348–1358. https://doi.org/10.1080/01694243.2012.697363

  28. Krishnamurthi B, Bharadwaj-Somaskandan S, Sergeeva T, Shutov F (2003) Effect of wood flour fillers on density and mechanical properties of polyurethane foams. Cell Polym 22(6):371–382

  29. Kushwaha P, Kumar R (2009) Studies on water absorption of bamboo-polyester composites: effect of silane treatment of mercerized bamboo. Polym Plast Technol Eng 49:45–52. https://doi.org/10.1080/03602550903283026

  30. Kushwaha P, Kumar R (2010) Studies on performance of acrylonitrile pretreated bamboo reinforced thermosetting resin composites. J Reinf Plast Compos 29:1347–1352. https://doi.org/10.1177/0731684409103701

  31. Kushwaha P, Kumar R (2011) Influence of chemical treatments on the mechanical and water absorption properties of bamboo fiber composites. J Reinf Plast Compos 30:73–85. https://doi.org/10.1177/0731684410383064

  32. Li S, Hu B, Ding Y, Liang H, Li C, Yu Z, Wu Z, Chen W, Yu S (2018) Wood-derived ultrathin carbon nanofiber aerogels. Angew Chem. https://doi.org/10.1002/ange.201802753

  33. Lin W, Huang Y, Li J, Liu Z, Yang W (2018) Preparation of highly hydrophobic and anti-fouling wood using poly (methylhydrogen) siloxane. Cellulose 25:7341–7353

  34. Liu W, Xie T, Qiu R, Fan M (2015) N-methylol acrylamide grafting bamboo fibers and their composites. Compos Sci Technol 117:100–106. https://doi.org/10.1016/j.compscitech.2015.06.005

  35. Liu L, Qian M, Pa S, Huang G, Yu Y, Fu S (2016a) Fabrication of green lignin-based fame retardants for enhancing the thermal and fire retardancy properties of polypropylene/wood composites. ACS Sustain Chem Eng 4:2422–2431. https://doi.org/10.1021/acssuschemeng.6b00112

  36. Liu W, Xie T, Qiu R, Fan M (2016b) Bamboo fibers grafted with a soybean-oil-based monomer for its unsaturated polyester composites. Cellulose 23:2501–2513. https://doi.org/10.1007/s10570-016-0969-z

  37. Mabrouk AB, Kaddami H, Boufi SE, Fouad Dufresne A (2012) Cellulosic nanoparticles from Alfa fibers (Stipa tenacissima): extraction procedures and reinforcement potential in polymer nanocomposites. Cellulose 19:843–853. https://doi.org/10.1007/s10570-012-9662-z

  38. Miao C, Hamad W (2013) Cellulose reinforced polymer composites and nanocomposites: a critical review. Cellulose 20:2221–2262. https://doi.org/10.1007/s10570-013-0007-3

  39. Monteiro SN, Calado V, Rodriguez RJ, Margem FM (2012) Thermogravimetric behavior of natural fibers reinforced polymer composites—an overview. Mater Sci Eng A 557:17–28. https://doi.org/10.1016/j.msea.2012.05.109

  40. Norma M, María R, Mirta A, Olagoke OI, Kolapo A (2016) Natural fiber thermoplastic composites. Plast Eng 1:727–752. https://doi.org/10.1201/b19190-23

  41. Olakanmi E, Strydom M (2016) Critical materials and processing challenges affecting the interface and functional performance of wood polymer composites (WPCs). MATER CHEM PHYS 171:290–302. https://doi.org/10.1016/j.matchemphys.2016.01.020

  42. Pal K, Mukherjee M, Frackowiak S (2014) Improvement of the physico-mechanical properties and stability of waste polypropylene in the presence of wood flour and (maleic anhydride)-grafted polypropylene. J Vinyl Addit Technol 20:24–30. https://doi.org/10.1002/vnl.21325

  43. Pendleton D, Hoffard T, Adcock T, Woodward B, Wolcott MP (2002) Durability of an extruded HDPE/wood composite. For Prod J 52:21–27. https://doi.org/10.1023/a:1020158128506

  44. Peng Y, Sandeep SN, Chen H, Yan N, Cao J (2018) Effects of lignin content on mechanical and thermal properties of polypropylene composites reinforced with micro particles of spray dried cellulose nanofibrils. ACS Sustain Chem Eng 6:11078–11086. https://doi.org/10.1021/acssuschemeng.8b02544

  45. Pickering K (2008) Properties and performance of natural-fibre composites. Woodhead Publishing, Cambridge

  46. Ramires E, Megiatto J, Gardrat C, Castellan A, Frollini E (2010) Biobased composites from glyoxal-phenol matrices reinforced with microcrystalline cellulose. Polímeros 20:126. https://doi.org/10.1590/S0104-14282010005000016

  47. Robin JJ, Breton Y (2001) Reinforcement of recycled polyethylene with wood fibers heat. J Reinf Plast Compos 20:1253–1262. https://doi.org/10.1177/073168401772679183

  48. Sahoo S, Mohanty S, Nayak S (2015) Toughened bio-based epoxy blend network modified with transesterified epoxidized soybean oil: synthesis and characterization. RSC Adv 5:13674–13691. https://doi.org/10.1039/C4RA11965G

  49. Sahin M, Schlögl S, Kalinka G, Wang J, Kaynak B, Mühlbacher I, Ziegler W, Kern W, Grützmacher H (2018) Tailoring the interfaces in glass fiber-reinforced photopolymer composites. Polymer 141:221–231. https://doi.org/10.1016/s0921-5093(00)01357-5

  50. Segerholm B, Ibach R, Westin M (2012) Moisture sorption, biological durability, and mechanical performance of WPC containing modified wood and polylactates. BioResources 7:4575–4585

  51. Sgriccia N, Hawley M, Misra M (2008) Characterization of natural fiber surfaces and natural fiber composites. Compos A Appl Sci Manuf 39:1632–1637. https://doi.org/10.1016/j.compositesa.2008.07.007

  52. Soykeabkae N, Arimoto N, Nishino T, Peijs T (2008) All-cellulose composites by surface selective dissolution of aligned lignocellulosic fibres. Compos Sci Technol 68:2210. https://doi.org/10.1016/j.compscitech.2008.03.023

  53. Spinacé MAS, Janeiro LG, Bernardino FC, Grossi TA, DePaol MA (2011) Poliolefinas reforçadas com fibras vegetais curtas: sisal × curauá Polyolefins reinforced with short vegetal fibers: sisal vs. curauá. Curauá. Polímeros 2:168

  54. Tang MM, Bacon R (1964) Carbonization of cellulose fibers—I, low temperature pyrolysis. Carbon 2:211–220. https://doi.org/10.1016/0008-6223(64)90035-1

  55. Wang T, Nolte M, Shanks B (2014) Catalytic dehydration of C6 carbohydrates for the production of hydroxymethylfurfural (HMF) as a versatile platform chemical. Green Chem 16:548–572. https://doi.org/10.1039/C3GC41365A

  56. Wang K, Dong Y, Yan Y, Zhang S, Li J (2016) Improving dimensional stability and durability of wood polymer composites by grafting polystyrene onto wood cell walls. Polym Compos 39:119–125. https://doi.org/10.1002/pc.23912

  57. Weingarten R, Tompsett G, Conner W, Huber G, Catal J (2011) Design of solid acid catalysts for aqueous-phase dehydration of carbohydrates: the role of Lewis and Brønsted acid sites. J Catal 279:174–182. https://doi.org/10.1016/j.jcat.2011.01.013

  58. Yao X, Shen C, Xu S (2019) The effects of coupling/grafting modification of wood fiber on the dimensional stability, mechanical and thermal properties of high density polyethylene/wood fiber composites. Mater Res Express 6(11):115328. https://doi.org/10.1088/2053-1591/ab4a63

  59. Zhang H (2014) Effect of a novel coupling agent, alkyl ketene dimer, on the mechanical properties of wood–plastic composites. Mater Des 9:130–134. https://doi.org/10.1016/j.matdes.2014.02.048

  60. Zhang W, Lu YH, Khanal S, Xu S (2018a) Effects of compatibilizers on selected properties of HDPE composites highly filled with bamboo flour. Wood Fiber Sci 50:254–264

  61. Zhang W, Yao X, Khanal S, Xu S (2018b) A novel surface treatment for bamboo flour and its effect on the dimensional stability and mechanical properties of high density polyethylene/bamboo flour composites. Constr Build Mater 186:1220

Download references


The authors are grateful for the financial support from the National Natural Science Foundation of China (Grant No. 31700498), Major scientific and technological projects for university in Fujian Province (2016H61010036), Science and technology extension project of Fujian Forestry Department (2018TG132), Natural Science Foundation of Fujian Province (2016H6005). The authors are also grateful to Mr. Mingen Fei from Washington State University.

Author information

Correspondence to Wenbin Yang.

Additional information

Publisher's Note

Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.

Electronic supplementary material

Below is the link to the electronic supplementary material.

Supplementary material 1 (DOCX 154 kb)

Rights and permissions

Reprints and Permissions

About this article

Verify currency and authenticity via CrossMark

Cite this article

Lin, H., Li, R., Li, D. et al. Hydrophobic wood flour derived from a novel p-TsOH treatment for improving interfacial compatibility of wood/HDPE composites. Cellulose (2020). https://doi.org/10.1007/s10570-020-03046-4

Download citation


  • p-toluenesulfonic
  • Hydrophobic wood fiber
  • Interfacial compatibility
  • Surface modification
  • Biocomposites