Abstract
Due to energy crisis and environmental pollution, biopolymer-based packaging materials have been extensively investigated. Cellulose nanofibrils (CNFs), due to their good oxygen barrier performance and excellent mechanical as well as film-forming properties, have emerged as interesting packaging materials. However, the problem of the resulting films is the highly hygroscopic character of the cellulose fibers themselves, which would further lead to a decrease of the films’ mechanical and barrier properties. Herein, a facile preparation of hydrophobic CNF films was carried out by the attachment of 10-undecylenoyl chloride onto CNFs followed by vacuum filtration. The modified CNFs became thicker and rougher compared with the pristine CNFs and were easy to disperse in ethanol. The resulting CNF film showed a higher surface roughness and a tensile strength of (47 ± 4) MPa. Additionally, the modified CNF film was hydrophobic, leading to an obvious barrier improvement with the WVP value decreasing by 62.4% in comparison to the pristine CNF film. Since this hydrophobic CNF film is easy to prepare with a good vapor barrier property, it should be promising for packaging applications. Furthermore, the generated CNF film demonstrated good reactivity with thiol groups, which can be applied for further functionalization to enrich their application fields.
Graphical abstract
This is a preview of subscription content, log in via an institution to check access.
Similar content being viewed by others
References
Abdul Khalil HPS, Davoudpour Y, Islam MN, Mustapha A, Sudesh K, Dunqani R, Jawaid M (2014) Production and modification of nanofibrillated cellulose using various mechanical processes: a review. Carbohydr Polym 99:649–665. https://doi.org/10.1016/j.carbpol.2013.08.069
Abraham E, Deepa B, Pothan LA, Jacob M, Thomas S, Cvelbar U, Anandjiwala R (2011) Extraction of nanocellulose fibrils from lignocellulosic fibers: a novel approach. Carbohydr Polym 86:1468–1475. https://doi.org/10.1016/j.carbpol.2011.06.034
Andresen M, Johansson LS, Tanem BS, Stenius P (2006) Properties and characterization of hydrophobized microfibrillated cellulose. Cellulose 13:665–677. https://doi.org/10.1007/s10570-006-9072-1
Aulin C, Gällstedt M, Lindström T (2010) Oxygen and oil barrier properties of microfibrillated cellulose films and coatings. Cellulose 17:559–574. https://doi.org/10.1007/s10570-009-9393-y
Azeredo HMC, Rosa MF, Mattoso LHC (2017) Nanocellulose in bio-based food packaging applications. Ind Crops Prod 97:664–671. https://doi.org/10.1016/j.indcrop.2016.03.013
Bedane AH, Eić M, Farmahini-Farahani M, Xiao H (2015) Water vapor transport properties of regenerated cellulose and nanofibrillated cellulose films. J Membr Sci 493:46–57. https://doi.org/10.1016/j.memsci.2015.06.009
Benitez AJ, Torres-Rendon JG, Poutanen M, Walther A (2013) Humidity and multiscale structure govern mechanical properties and deformation modes in films of native cellulose nanofibrils. Biomacromolecules 14:4497–4506. https://doi.org/10.1021/bm401451m
Chinga-Carrasco G, Kuznetsova N, Garaeva M, Leirset I, Galiullina G, Kostochko A, Syverud K (2012) Bleached and unbleached MFC nanobarriers: properties and hydrophobisation with hexamethyldisilazane. J Nanopart Res 14:1280. https://doi.org/10.1007/s11051-012-1280-z
Cunha AG, Zhou Q, Larsson PT, Berglund LA (2014) Topochemical acetylation of cellulose nanopaper structures for biocomposites: mechanisms for reduced water vapour sorption. Cellulose 21:2773–2787. https://doi.org/10.1007/s10570-014-0334-z
Ferrer A, Quintana E, Filpponen I, Solala I, Vidal T, Rodríguez A, Laine J, Rojas OJ (2012) Effect of residual lignin and heteropolysaccharides in nanofibrillar cellulose and nanopaper from wood fibers. Cellulose 19:2179–2193. https://doi.org/10.1007/s10570-012-9788-z
Ferrer A, Pal L, Hubbe M (2017) Nanocellulose in packaging: advances in barrier layer technologies. Ind Crops Prod 95:574–582. https://doi.org/10.1016/j.indcrop.2016.11.012
Guo J, Fang W, Welle A, Feng W, Filpponen I, Rojas OJ, Levkin PA (2016) Superhydrophobic and slippery lubricant-infused flexible transparent nanocellulose films by photoinduced thiol-ene functionalization. ACS Appl Mater Interfaces 8:34115–34122. https://doi.org/10.1021/acsami.6b11741
Hu Z, Berry RM, Pelton R, Cranston ED (2017) One-pot water-based hydrophobic surface modification of cellulose nanocrystals using plant polyphenols. ACS Sustain Chem Eng 5:5018–5026. https://doi.org/10.1021/acssuschemeng.7b00415
Johnson RK, Zink-Sharp A, Glasser WG (2011) Preparation and characterization of hydrophobic derivatives of TEMPO-oxidized nanocelluloses. Cellulose 18:1599–1609. https://doi.org/10.1007/s10570-011-9579-y
Jonoobi M, Harum J, Mathew AP, Hussein MZB, Oksman K (2010) Preparation of cellulose nanofibers with hydrophobic surface characteristics. Cellulose 17:299–307. https://doi.org/10.1007/s10570-009-9387-9
Klemm D, Philipp B, Heinze T, Heinze U, Wagenknecht W (1998) Comprehensive cellulose chemistry: functionalization of cellulose. Wiley-VCH, Weinheim
Laine J, Stenius P (1994) Surface characterization of unbleached kraft pulps by means of ESCA. Cellulose 1:145–160. https://doi.org/10.1007/BF00819664
Le D, Kongparakul S, Samart C, Phanthong P, Karnjanakom S, Abudula A, Guan G (2016) Preparation hydrophobic nanocellulose-silica film by a facile one-pot method. Carbohydr Polym 153:266–274. https://doi.org/10.1016/j.carbpol.2016.07.112
Li J, Li L, Du X, Feng W, Welle A, Trapp O, Grunze M, Hirtz M, Levkin PA (2014) Reactive superhydrophobic surface and its photoinduced disulfide-ene and thiol-ene (bio)functionalization. Nano Lett 15:675–681. https://doi.org/10.1021/nl5041836
Lu P, Tian X, Liu Y, Wang Z (2016) Effects of Cellulosic based sheet pore structure and soybean oil-based polymer layer on cellulosic packaging performance as a barrier for water and water vapor. BioRes. 11:8483–8495. https://doi.org/10.15376/biores.11.4.8483-8495
Nair SS, Yan N (2015) Effect of high residual lignin on the thermal stability of nanofibrils and its enhanced mechanical performance in aqueous environments. Cellulose 22:3137–3150. https://doi.org/10.1007/s10570-015-0737-5
Nair SS, Kuo PY, Chen H, Yan N (2017) Investigating the effect of lignin on the mechanical, thermal, and barrier properties of cellulose nanofibril reinforced epoxy composite. Ind Crops Prod 100:208–217. https://doi.org/10.1016/j.indcrop.2017.02.032
Nechyporchuk O, Belgacem MN, Bras J (2016) Production of cellulose nanofibrils: a review of recent advances. Ind Crops Prod 93:2–25. https://doi.org/10.1016/j.indcrop.2016.02.016
Nie S, Zhang K, Lin X, Zhang C, Yan D, Liang H, Wang S (2018) Enzymatic pretreatment for the improvement of dispersion and film properties of cellulose nanofibrils. Carbohydr Polym 181:1136–1142. https://doi.org/10.1016/j.carbpol.2017.11.020
Österberg M, Vartiainen J, Lucenius J, Hippi U, Seppälä J, Serimaa R, Laine J (2013) A fast method to produce strong NFC films as a platform for barrier and functional materials. ACS Appl Mater Interfaces 5:4640–4647. https://doi.org/10.1021/am401046x
Peng Y, Gardner DJ, Han Y, Kiziltas A, Cai Z, Tshabalala MA (2013) Influence of drying method on the material properties of nanocellulose I: thermostability and crystallinity. Cellulose 20:2379–2392. https://doi.org/10.1007/s10570-013-0019-z
Poletto M, Zarrera AJ, Forte MMC, Santana RMC (2012) Thermal decomposition of wood: influence of wood components and cellulose crystallite size. Bioresour Technol 109:148–153. https://doi.org/10.1016/j.biortech.2011.11.122
Prakobna K, Terenzi C, Zhou Q, Furó I, Berglund LA (2015) Core-shell cellulose nanofibers for biocomposite-nanostructural effects in hydrated state. Carbohydr Polym 125:92–102. https://doi.org/10.1016/j.carbpol.2015.02.059
Qing Y, Cai Z, Wu Y, Yao C, Wu Q, Li X (2015) Facile preparation of optically transparent and hydrophobic cellulose nanofibril composite films. Ind Crops Prod 77:13–20. https://doi.org/10.1016/j.indcrop.2015.08.016
Rajinipriya M, Nagalakshmaiah M, Robert M, Elkoun S (2018) Importance of agricultural and industrial waste in the field of nanocellulose and recent industrial developments of wood based nanocellulose: a review. ACS Sustain Chem Eng 6:2807–2828. https://doi.org/10.1021/acssuschemeng.7b03437
Rojo E, Peresin MS, Sampson WW, Hoeger IC, Vartiainen J, Laine J, Rojas OJ (2015) Comprehensive elucidation of the effect of residual lignin on the physical, barrier, mechanical and surface properties of nanocellulose films. Green Chem 17:1853–1866. https://doi.org/10.1039/C4GC02398F
Sehaqui H, Zimmermann T, Tingaut P (2014) Hydrophobic cellulose nanopaper through a mild esterification procedure. Cellulose 21:367–382. https://doi.org/10.1007/s10570-013-0110-5
Shimizu M, Saito T, Fukuzumi H, Isogai A (2014) Hydrophobic, ductile, and transparent nanocellulose films with quaternary alkylammonium carboxylates on nanofibril surfaces. Biomacromol 15:4320–4325. https://doi.org/10.1021/bm501329v
Shimizu M, Saito T, Isogai A (2016) Water-resistant and high oxygen-barrier nanocellulose films with interfibrillar cross-linkages formed through multivalent metal ions. J Membr Sci 500:1–7. https://doi.org/10.1016/j.memsci.2015.11.002
Solala I, Bordes R, Larsson A (2018) Water vapor mass transport across nanofibrillated cellulose films: effect of surface hydrophobization. Cellulose 25:347–356. https://doi.org/10.1007/s10570-017-1608-z
Song J, Rojas OJ (2013) Approaching super-hydrophobicity from cellulosic materials: a review. Nord Pulp Pap Res J 28:216–238
Song Z, Xiao H, Zhao Y (2014) Hydrophobic-modified nano-cellulose fiber/PLA biodegradable composites for lowering water vapor transmission rate (WVTR) of paper. Carbohydr Polym 111:442–448. https://doi.org/10.1016/j.carbpol.2014.04.049
Spence KL, Venditti RA, Rojas OJ, Habibi Y, Pawlak JJ (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. https://doi.org/10.1007/s10570-010-9424-8
Stenstad P, Andresen M, Tanem BS, Stenius P (2008) Chemical surface modifications of microfibrillated cellulose. Cellulose 15:35–45. https://doi.org/10.1007/s10570-007-9143-y
Teisala H, Tuominen M, Kuusipalo J (2014) Superhydrophobic coatings on cellulose-based materials: fabrication, properties, and applications. Adv Mater Interfaces 1:1300026. https://doi.org/10.1002/admi.201300026
Tingaut P, Zimmermann T, Lopez-Suevos F (2010) Synthesis and characterization of bionanocomposites with tunable properties from poly(lactic acid) and acetylated microfibrillated cellulose. Biomacromol 11:454–464. https://doi.org/10.1021/bm901186u
Tomé LC, Pinto RJB, Trovatti E, Freire CSR, Silvestre AJD, Neto CP, Gandini A (2011) Transparent bionanocomposties with improved properties prepared from acetylated bacterial cellulose and poly(lactic acid) through a simple approach. Green Chem 13:419–427. https://doi.org/10.1039/C0GC00545B
Vaca-Garcia C, Borredon ME, Gaseta A (2001) Determination of the degree of substitution (DS) of mixed cellulose esters by elemental analysis. Cellulose 8:225–231. https://doi.org/10.1023/A:1013133921626
Wang Y, Heinze T, Zhang K (2016) Stimuli-responsive nanoparticles from ionic cellulose derivatives. Nanoscale 8:648–657. https://doi.org/10.1039/c5nr05862g
Wang J, Gardner DJ, Stark NM, Bousfield DW, Tajvidi M, Cai Z (2018a) Moisture and oxygen barrier properties of cellulose nanomaterial-based films. ACS Sustain Chem Eng 6:49–70. https://doi.org/10.1021/acssuschemeng.7b03523
Wang S, Sha J, Wang W, Qin C, Li W, Qin C (2018b) Superhydrophobic surfaces generated by one-pot spray-coating of chitosan-based nanoparticles. Carbohydr Polym 195:39–44. https://doi.org/10.1016/j.carbpol.2018.04.068
Yang H, Yan R, Chen H, Zheng C, Lee DH, Liang DT (2006) In-depth investigation of biomass pyrolysis based on three major components: hemicelluloses, cellulose and lignin. Energy Fuels 20:388–393. https://doi.org/10.1021/ef0580117
Zhang K, Zhang Y, Yan D, Zhang C, Nie S (2018) Enzyme-assisted mechanical production of cellulose nanofibrils: thermal stability. Cellulose. https://doi.org/10.1007/s10570-018-1928-7
Acknowledgments
This work was supported by the Natural Science Foundation of Guangxi (2018GXNSFBA138027), Scientific Research Foundation of Guangxi University (XGZ170232), the State Key Laboratory of Pulp and Paper Engineering (201806), the Foundation of Key Laboratory of Pulp and Paper Science and Technology of Ministry of Education/Shandong Province of China (KF201716) and the Middle-young Age Ability Enhancement Program of Guangxi (2018KY0023).
Author information
Authors and Affiliations
Corresponding author
Ethics declarations
Conflict of interest
The authors declare that they have no conflict of interest.
Additional information
Publisher's Note
Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
Rights and permissions
About this article
Cite this article
Li, W., Wang, S., Wang, W. et al. Facile preparation of reactive hydrophobic cellulose nanofibril film for reducing water vapor permeability (WVP) in packaging applications. Cellulose 26, 3271–3284 (2019). https://doi.org/10.1007/s10570-019-02270-x
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1007/s10570-019-02270-x