, Volume 25, Issue 8, pp 4623–4637 | Cite as

Enhanced performances of polyvinyl alcohol films by introducing tannic acid and pineapple peel-derived cellulose nanocrystals

  • Hongjie Dai
  • Yue Huang
  • Huihua HuangEmail author
Original Paper


The applications of polyvinyl alcohol (PVA) films are still hampered due to great affinity to water, poor mechanical strength and lack of biological properties. To overcome these shortcomings, this study presented a successful development of PVA films by the introductions of tannic acid (TA) and pineapple peel-derived cellulose nanocrystals (PPNc). The structure, morphology, light transmittance, water adsorption and solubility, and mechanical properties of the prepared films were studied and compared. The uniform dispersions of PPNc and TA in PVA matric were observed by the SEM and XRD results. The introductions of TA and PPNc effectively enhanced thermal stability and tensile strength, but slightly reduced the light transmittance of the films. The water adsorption ability and solubility of the films were corresponded to the contents of TA and PPNc. Especially, the introduction of TA endowed the films with a strong anti-ultraviolet ability and antibacterial activity against Staphylococcus aureus. Based on the overall results, the prepared films can be used as green and active packaging materials.

Graphical Abstract


Pineapple peel Cellulose nanocrystals Tannic acid Polyvinyl alcohol Film 



This work was supported by National Natural Science Foundation of China under Grant Nos. 31471673 and 31271978.


  1. Bardet R, Reverdy C, Belgacem N, Leirset I, Syverud K, Bardet M, Bras J (2015) Substitution of nanoclay in high gas barrier films of cellulose nanofibrils with cellulose nanocrystals and thermal treatment. Cellulose 22:1227–1241. CrossRefGoogle Scholar
  2. Chaabouni O, Boufi S (2017) Cellulose nanofibrils/polyvinyl acetate nanocomposite adhesives with improved mechanical properties. Carbohydr Polym 156:64–70. CrossRefPubMedGoogle Scholar
  3. Chen YN, Peng L, Liu T, Wang Y, Shi S, Wang H (2016a) Poly(vinyl alcohol)–tannic acid hydrogels with excellent mechanical properties and shape memory behaviors. ACS Appl Mater Inter 8(40):27199–27206. CrossRefGoogle Scholar
  4. Chen YW, Lee HV, Juan JC, Phang S (2016b) Production of new cellulose nanomaterial from red algae marine biomass Gelidium elegans. Carbohydr Polym 151:1210–1219. CrossRefPubMedGoogle Scholar
  5. Choo K, Ching YC, Cheng HC, Julai S, Liou NS (2016) Preparation and characterization of polyvinyl alcohol-chitosan composite films reinforced with cellulose nanofiber. Acta Polym Sin 9:644. CrossRefGoogle Scholar
  6. Dai H, Huang H (2016) Modified pineapple peel cellulose hydrogels embedded with sepia ink for effective removal of methylene blue. Carbohydr Polym 148:1–10. CrossRefPubMedGoogle Scholar
  7. Dai H, Huang H (2017a) Enhanced swelling and responsive properties of pineapple peel carboxymethyl cellulose-g-poly(acrylic acid-co-acrylamide) superabsorbent hydrogel by the introduction of carclazyte. J Agric Food Chem 65(3):565–573. CrossRefPubMedGoogle Scholar
  8. Dai H, Huang H (2017b) Synthesis, characterization and properties of pineapple peel cellulose-g-acrylic acid hydrogel loaded with kaolin and sepia ink. Cellulose 24:69–84. CrossRefGoogle Scholar
  9. Dai H, Ou S, Liu Z, Huang H (2017) Pineapple peel carboxymethyl cellulose/polyvinyl alcohol/mesoporous silica SBA-15 hydrogel composites for papain immobilization. Carbohydr Polym 169:504–514. CrossRefPubMedGoogle Scholar
  10. Dai H, Huang Y, Huang H (2018a) Eco-friendly polyvinyl alcohol/carboxymethyl cellulose hydrogels reinforced with graphene oxide and bentonite for enhanced adsorption of methylene blue. Carbohydr Polym 185:1–11. CrossRefPubMedGoogle Scholar
  11. Dai H, Ou S, Huang Y, Liu Z, Huang H (2018b) Enhanced swelling and multiple-responsive properties of gelatin/sodium alginate hydrogels by the addition of carboxymethyl cellulose isolated from pineapple peel. Cellulose 25:293–606. CrossRefGoogle Scholar
  12. Dai H, Ou S, Huang Y, Huang H (2018c) Utilization of pineapple peel for production of nanocellulose and film application. Cellulose 25:1743–1756. CrossRefGoogle Scholar
  13. Fan L, Yang J, Yang H, Peng M, Hu J (2016) Preparation and characterization of chitosan/gelatin/PVA hydrogel for wound dressings. Carbohydr Polym 146:427–434. CrossRefPubMedGoogle Scholar
  14. Feng X, Meng X, Zhao J, Miao M, Shi L, Zhang S, Fang J (2015) Extraction and preparation of cellulose nanocrystals from dealginate kelp residue: structures and morphological characterization. Cellulose 22:1763–1772. CrossRefGoogle Scholar
  15. French AD (2014) Idealized powder diffraction patterns for cellulose polymorphs. Cellulose 21:885–896. CrossRefGoogle Scholar
  16. Haafiz MKM, Hassan A, Zakaria Z, Inuwa IM (2014) Isolation and characterization of cellulose nanowhiskers from oil palm biomass microcrystalline cellulose. Carbohydr Polym 103:119–125. CrossRefPubMedGoogle Scholar
  17. Hietala M, Sain S, Oksman K (2017) Highly redispersible sugar beet nanofibers as reinforcement in bionanocomposites. Cellulose 24:2177–2189. CrossRefGoogle Scholar
  18. Hong KH (2016) Polyvinyl alcohol/tannic acid hydrogel prepared by a freeze-thawing process for wound dressing applications. Polym Bull 74:2861–2872. CrossRefGoogle Scholar
  19. Ibrahim MM, El-Zawawy WK, Nassar MA (2010) Synthesis and characterization of polyvinyl alcohol/nanospherical cellulose particle films. Carbohydr Polym 79:694–699. CrossRefGoogle Scholar
  20. Islam MS, Rahaman MS, Yeum JH (2015) Electrospun novel super-absorbent based on polysaccharide–polyvinyl alcohol-montmorillonite clay nanocomposites. Carbohydr Polym 115:69–77. CrossRefPubMedGoogle Scholar
  21. Jiang F, Hsieh YL (2013) Chemically and mechanically isolated nanocellulose and their self-assembled structures. Carbohydr Polym 95:32–40. CrossRefPubMedGoogle Scholar
  22. Johar N, Ahmad I, Dufresne A (2012) Extraction, preparation and characterization of cellulose fibres and nanocrystals from rice husk. Ind Crop Prod 37:93–99. CrossRefGoogle Scholar
  23. Khan RA, Salmieri S, Dussault D, Uribe-Calderon J, Kamal MR, Safrany A, Lacroix M (2010) Production and properties of nanocellulose-reinforced methylcellulose-based biodegradable films. J Agric Food Chem 58:7878–7885. CrossRefPubMedGoogle Scholar
  24. Kim TJ, Silva JL, Jung YS (2011) Enhanced functional properties of tannic acid after thermal hydrolysis. Food Chem 126:116–120. CrossRefGoogle Scholar
  25. Lan G, Lu B, Wang T, Wang L, Chen J, Yu K, Liu J, Dai F, Wu D (2015) Chitosan/gelatin composite sponge is an absorbable surgical hemostatic agent. Colloid Surf B 136:1026–1034. CrossRefGoogle Scholar
  26. Li W, Wu Q, Zhao X, Huang Z, Cao J, Li J, Liu S (2014) Enhanced thermal and mechanical properties of PVA composites formed with filamentous nanocellulose fibrils. Carbohydr Polym 113:403–410. CrossRefPubMedGoogle Scholar
  27. Lim M, Shin H, Shin DM, Lee S, Lee J (2016) Poly(vinyl alcohol) nanocomposites containing reduced graphene oxide coated with tannic acid for humidity sensor. Polymer 84:89–98. CrossRefGoogle Scholar
  28. Liu D, Bian Q, Li Y, Wang Y, Xiang A, Tian H (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
  29. Lizundia E, Urruchi A, Vilas JL, León LM (2016) Increased functional properties and thermal stability of flexible cellulose nanocrystal/ZnO films. Carbohydr Polym 136:250–258. CrossRefPubMedGoogle Scholar
  30. Mallakpour S, Nezamzadeh EA (2017) Preparation and characterization of chitosan-poly(vinyl alcohol) nanocomposite films embedded with functionalized multi-walled carbon nanotube. Carbohydr Polym 166:377–386. CrossRefPubMedGoogle Scholar
  31. Mandal A, Chakrabarty D (2013) Studies on the mechanical, thermal, morphological and barrier properties of nanocomposites based on poly(vinyl alcohol) and nanocellulose from sugarcane bagasse. J Ind Eng Chem. CrossRefGoogle Scholar
  32. Mi H, Jing X, Peng J, Salick MR, Peng X, Turng L (2014) Poly(ε-caprolactone) (PCL)/cellulose nano-crystal (CNC) nanocomposites and foams. Cellulose 21:2727–2741. CrossRefGoogle Scholar
  33. Mok CF, Ching YC, Muhamad F, Osman NAA, Singh R (2017) Poly(vinyl alcohol)-α-chitin composites reinforced by oil palm empty fruit bunch fibers-derived nanocellulose. Int J Polym Anal Charact 22(4):1–11. CrossRefGoogle Scholar
  34. 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. Carbohydr Polym 135:1–9. CrossRefPubMedGoogle Scholar
  35. Nepomuceno NC, Santos ASF, Oliveira JE, Glenn GM, Medeiros ES (2017) Extraction and characterization of cellulose nanowhiskers from Mandacaru (Cereus jamacaru DC.) spines. Cellulose 24:119–129. CrossRefGoogle Scholar
  36. Pereira VA, de Arruda INQ, Stefani R (2015) Active chitosan/PVA films with anthocyanins from Brassica oleraceae (Red Cabbage) as time-temperature indicators for application in intelligent food packaging. Food Hydrocolloid 43:180–188. CrossRefGoogle Scholar
  37. Rashid M, Gafur MA, Sharafat MK, Minami H, Maj M, Ahmad H (2017) Biocompatible microcrystalline cellulose particles from cotton wool and magnetization via a simple in situ co-precipitation method. Carbohydr Polym 170:72–79. CrossRefPubMedGoogle Scholar
  38. Rubentheren V, Ward TA, Chee CY, Nair P (2015a) Physical and chemical reinforcement of chitosan film using nanocrystalline cellulose and tannic acid. Cellulose 22:2529–2541. CrossRefGoogle Scholar
  39. Rubentheren V, Ward TA, Chee CY, Tang CK (2015b) Processing and analysis of chitosan nanocomposites reinforced with chitin whiskers and tannic acid as a crosslinker. Carbohydr Polym 115:379–387. CrossRefPubMedGoogle Scholar
  40. Rubentheren V, Ward TA, Chee CY, Nair P, Salami E, Fearday C (2016) Effects of heat treatment on chitosan nanocomposite film reinforced with nanocrystalline cellulose and tannic acid. Carbohy Polym 140:202–208. CrossRefPubMedGoogle Scholar
  41. Sahiner N, Sagbas S, Sahiner M, Silan C, Aktas N, Turk M (2016) Biocompatible and biodegradable poly (tannic acid) hydrogel with antimicrobial and antioxidant properties. Int J Biol Macromol 82:150–159. CrossRefPubMedGoogle Scholar
  42. Santos RMD, Flauzino Neto WP, Silvério HA, Martins DF, Dantas NO, Pasquini D (2013) Cellulose nanocrystals from pineapple leaf, a new approach for the reuse of this agro-waste. Ind Crop Prod 50:707–714. CrossRefGoogle Scholar
  43. Shanthini GM, Sakthivel N, Menon R, Nabhiraj PY, Gómez-Tejedor JA, Meseguer-due As JM, Gómez Ribelles JL, Krishna JBM, Kalkura SN (2016) Surface stiffening and enhanced photoluminescence of ion implanted cellulose–polyvinyl alcohol–silica composite. Carbohydr Polym 153:619–630. CrossRefPubMedGoogle Scholar
  44. Sionkowska A, Kaczmarek B, Lewandowska K (2014) Modification of collagen and chitosan mixtures by the addition of tannic acid. J Mol Liq 199:318–323. CrossRefGoogle Scholar
  45. Song T, Tanpichai S, Oksman K, Universitet LT, Materialvetenskap Matematik IFRT (2016) Cross-linked polyvinyl alcohol (PVA) foams reinforced with cellulose nanocrystals (CNCs). Cellulose 23:1925–1938. CrossRefGoogle Scholar
  46. Tang J, Sisler J, Grishkewich N, Tam KC (2017) Functionalization of cellulose nanocrystals for advanced applications. J Colloid Interf Sci 494:397–409. CrossRefGoogle Scholar
  47. Timofejeva A, D’Este M, Loca D (2017) Calcium phosphate/polyvinyl alcohol composite hydrogels: a review on the freeze-thawing synthesis approach and applications in regenerative medicine. Eur Polym J 95:547–565. CrossRefGoogle Scholar
  48. Wan J, Guo J, Miao Z, Guo X (2016) Reverse micellar extraction of bromelain from pineapple peel-Effect of surfactant structure. Food Chem 197:450–456. CrossRefPubMedGoogle Scholar
  49. Wang B, Li D (2015) Strong and optically transparent biocomposites reinforced with cellulose nanofibers isolated from peanut shell. Compos Part A Appl Sci 79:1–7. CrossRefGoogle Scholar
  50. Xu F, Weng B, Gilkerson R, Materon LA, Lozano K (2015) Development of tannic acid/chitosan/pullulan composite nanofibers from aqueous solution for potential applications as wound dressing. Carbohydr Polym 115:16–24. CrossRefPubMedGoogle Scholar
  51. Yu Z, Cai Z, Chen Q, Liu M, Ye L, Ren J, Liao W, Liu S (2016) Engineering β-sheet peptide assemblies for biomedical applications. Biomater Sci 4:365–374. CrossRefPubMedGoogle Scholar
  52. Yue Y, Zhou C, French AD, Xia G, Han G, Wang Q, Wu Q (2012) Comparative properties of cellulose nano-crystals from native and mercerized cotton fibers. Cellulose 19:1173–1187. CrossRefGoogle Scholar
  53. Zhang X, Do MD, Casey P, Sulistio A, Qiao GG, Lundin L, Lillford P, Kosaraju S (2010) Chemical modification of gelatin by a natural phenolic cross-linker, tannic acid. J Agric Food Chem 58:6809–6815. CrossRefPubMedGoogle Scholar

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© Springer Science+Business Media B.V., part of Springer Nature 2018

Authors and Affiliations

  1. 1.School of Food Science and EngineeringSouth China University of TechnologyGuangzhou CityChina

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