Abstract
The applicability of cellulose nanofibrils (CNFs) has received attention due to their attractive properties. This study proposes the functionalization of açai CNFs with copaiba oil and vegetal tannins to produce films with potential for packaging. Bio-based films were evaluated by vapor permeability, colorimetry, and mechanical strength. CNFs were produced by mechanical fibrillation, from suspensions of bleached açai fibers and commercial eucalipytus pulp. Moreover, copaiba oil and vegetal tannin were added to the CNFs to produce films/nanopapers by casting from both suspensions with concentrations of 1% (based on CNF dry mass). The bulk densities of the eucalyptus CNF films were higher (1.126–1.171 g cm−3) compared to the açai CNF ones. Films from eucalyptus and açai pulps containing copaiba oil and tannins presented higher Tonset and Tmax, respectively (312 and 370 °C). Films with açaí CNFs functionalized with copaiba oil and tannin showed the lowest permeability value (370 g day−1 m−2). Films produced with eucalyptus pulp, and eucalyptus pulp functionalized with copaiba oil highlighted by superior mechanical strength, achieving 133.8 and 121.4 MPa, respectively. The evaluation of colorimetry showed a greater tendency to yellowing for açai films, especially those functionalized with vegetal tannins. Besides the low cost, functionalized vegetal-based nanomaterials could have attractive properties, with potential for application as some kind of packaging, for transporting basic products, such as breads, flours, or products with low moisture content, enabling efficient utilization of forest wastes.
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The datasets supporting the conclusions of this article are included in the article. Besides, the datasets used and/or analyzed during the current study are available from the corresponding author on reasonable request.
References
ABNT (2003) Brazilian Association of Technical Standards NBR 11941: Madeira – determination of basic density. Rio de Janeiro. 6p
Abraham E, Deepa B, Pothan LA, Jacob M, Thomas S, Cvelbar U, Anandjiwala R (2011) Extraction of nanocellulose fibrils from lignocellulosic fibres: a novel approach. Carbohydr Polym 86:1468–1475. https://doi.org/10.1016/j.carbpol.2011.06.034
Agrawal R, Saxena NS, Sharma KB, Thomas S, Sreekala MS (2000) Activation energy and crystallization kinetics of untreated and treat oil palm fibre reinforced phenol formaldehyde composites. Mater Sci Eng 277:77–82. https://doi.org/10.1016/S0921-5093(99)00556-0
Amaral AC, Bocca AL, Ribeiro AM, Nunes J, Peixoto DLG, Simioni AR, Primo FL, Lacava ZGM, Bentes R, Titze-de-Almeida R, Tedesco AC, Morais PC, Felipe MSS (2009) Amphotericin B in poly (lactic-co-glycolic acid) (PLGA) and dimercaptosuccinic acid (DMSA) nanoparticles against paracoccidioidomycosis. J Antimicrob Chemother 63:526–533. https://doi.org/10.1093/jac/dkn539
ASTM (2000) American Society for Testing and Materials - ASTM E 96-00. Standard test methods for water vapor transmission of materials, Philadelphia
ASTM (2018) American Society for Testing and Materials - ASTM D882. Standard test methods for tensile properties of thin plastic sheeting, West Conshohocken
Bian H, Gao Y, Yang Y, Fang G, Dai H (2018) Improving cellulose nanofibrillation of waste wheat straw using the combined methods of prewashing, p-toluenesulfonic acid hydrolysis, disk grinding, and endoglucanase post-treatment. Bioresour Technol 256:321–327
Bonan RF, Bonan PR, Batista AU, Sampaio FC, Albuquerque AJ, Moraes MC, Mattoso LH, Glenn GM, Medeiros ES, Oliveira JE (2015) In vitro antimicrobial activity of solution blow spun poly (lactic acid)/polyvinylpyrrolidone nanofibers loaded with Copaiba (Copaifera sp.) oil. Mater Sci Eng C Mater Biol Appl 48:372–377. https://doi.org/10.1016/j.msec.2014.12.021
Brandelero RPH, Almeida FM, Alfaro A (2015) Microestrutura e propriedades de filmes de amido-álcool polivinílico-alginato adicionados de óleos essenciais de copaíba e capim limão. Química Nova 38:910–916. https://doi.org/10.5935/0100-4042.20150098
Browning BL (1963) The chemistry of wood. Interscience, Warrenvile, p 689
Bufalino L, de Sena Neto AR, Tonoli GHD, de Souza Fonseca A, Costa TG, Marconcini JM, Colodette JL, Labory CRG, Mendes LM (2015) How the chemical nature of Brazilian hardwoods affects nanofibrillation of cellulose fibers and film optical quality. Cellulose 22:3657–3672. https://doi.org/10.1007/s10570-015-0771-3
Butchosa N, Zhou Q (2014) Water redispersible cellulose nanofibrils adsorbed with carboxymethyl cellulose. Cellulose 21:4349–4358. https://doi.org/10.1007/s10570-014-0452-7
Cano A, Contreras C, Chiralt A, González-Martínez C (2021) Using tannins as active compounds to develop antioxidant and antimicrobial chitosan and cellulose based films. Carbohydr Polymer Technol Appl 2:100156. https://doi.org/10.1016/j.carpta.2021.100156
Chen W, Abe K, Uetani K, Yu H, Liu Y, Yano H (2014) Individual cotton cellulose nanofibrils: pretreatment and fibrillation technique. Cellulose 21:1517–1528. https://doi.org/10.1007/s10570-014-0172-z
Coutts RSP, Warden PG (1992) Sisal pulp reinforced cement mortar. Cem Concr Compos 14:17–21. https://doi.org/10.1016/0958-9465(92)90035-T
Debone HS, Lopes PS, Severino P, Yoshida CMP, Souto EB, da Silva CF (2019) Chitosan/Copaiba oleoresin films for would dressing application. Int J Pharm 555:146–152. https://doi.org/10.1016/j.ijpharm.2018.11.054
Dias M, Mendonça M, Damásio R, Zidanes U, Mori F, Ferreira S, Tonoli G (2019) Influence of hemicellulose content of eucalyptus and pinus fibers on the grinding process for obtaining cellulose micro/nanofibrils. Holzforschung 73:1035–1046. https://doi.org/10.1515/hf-2018-0230
do Lago RC, de Oliveira ALM, Dias MC, de Carvalho EEN, Tonoli GHD, Vilas Boas EVB (2020) Obtaining cellulosic nanofibrils from oat straw for biocomposite reinforcement: mechanical and barrier properties. Ind Crop Prod 148:112264. https://doi.org/10.1016/j.indcrop.2020.112264
Fonseca CS, Scatolino MV, Silva LE, Martins MA, Guimarães M Jr, Tonoli GHD (2021) Valorization of jute biomass: performance of fiber–cement composites extruded with hybrid reinforcement (fibers and nanofibrils). Waste Biomass Valor. https://doi.org/10.1007/s12649-021-01394-1
Fukuzumi H, Tanaka R, Saito T et al (2014) Dispersion stability and aggregation behavior of TEMPO-oxidized cellulose nanofibrils in water as a function of salt addition. Cellulose 21:1553–1559. https://doi.org/10.1007/s10570-014-0180-z
Furtado PS, Melo JRS, Meireles PW, Honorio TS, Miguel NCO et al (2021) Benign prostatic hyperplasia therapy through liquisolid technology composed of polymer-layered nanocomposites based on silicate that contain babassu oil and copaiba oil-resin. J Drug Deliv Sci Technol. https://doi.org/10.1016/j.jddst.2021.102586
Ghanbarzadeh B, Almasi H (2011) Physical properties of edible emulsified films based on carboxymethyl cellulose and oleic acid. Int J Biol Macromol 48:44–49. https://doi.org/10.1016/j.ijbiomac.2010.09.014
Ghanbarzadeh B, Almasi H, Entezami AA (2010) Physical properties of edible modified starch/carboxymethyl cellulosefilms. Innov Food Sci 11:697–702. https://doi.org/10.1016/j.ifset.2010.06.001
Guimarães M Jr, Botaro VR, Novack KM, Teixeira FG, Tonoli GHD (2015) Starch/PVA-based nanocomposites reinforced with bamboo nanofibrils. Ind Crop Prod 70:72–83. https://doi.org/10.1016/j.indcrop.2015.03.014
Guimarães M Jr, Teixeira FG, Tonoli GHD (2018) Effect of the nano-fibrillation of bamboo pulp on the thermal, structural, mechanical and physical properties of nanocomposites based on starch/poly (vinyl alcohol) blend. Cellulose. 25:1–27. https://doi.org/10.1007/s10570-018-1691-9
Guimarães BMR, Scatolino MV, Martins MA et al (2021) Bio-based films/nanopapers from lignocellulosic wastes for production of added-value micro-/nanomaterials. Environ Sci Pollut Res. https://doi.org/10.1007/s11356-021-16203-4
Guo F, Wang R (2014) On the persistence and unique continuation properties for an integrable two-component Dullin–Gottwald–Holm system. Nonlinear Anal: Theory Methods Appl 96:38–46. https://doi.org/10.1016/j.na.2013.10.021
Kennedy F, Phillips GO, Williams EPA (1987) Wood and cellulosic: industrial utilization, biotechnology, structure and properties. Halsted, New York, p 1130
Leiviskä T, Rämö J (2008) Coagulation of wood extractives in chemical pulp bleaching filtrate by cationic polyelectrolytes. J Hazard Mater 153:525–531. https://doi.org/10.1016/j.jhazmat.2007.08.084
Leiviskä T, Rämö J, Nurmesniemic H, Pöykiö R, Kuokkanene T (2009) Size fractionation of wood extractives, lignin and trace elements in pulp and paper mill wastewater before and after biological treatment. Water Res 43:3199–3206. https://doi.org/10.1016/j.watres.2009.04.051
Linan LZ, Cidreira ACM, Rocha CQ, Menezes FF, Rocha GJM, Paiva AEM (2021) Utilization of acai berry residual biomass for extraction of lignocellulosic byproducts. J Bioresources Bioprod. https://doi.org/10.1016/j.jobab.2021.04.007
Mészáros E, Jakab E, Várhegyi G (2007) TG/MS, Py-GC/MS and THM-GC/MS study of the composition and thermal behavior of extractive components of Robinia pseudoacacia. J Anal Appl Pyrolysis 79:61–70. https://doi.org/10.1016/j.jaap.2006.12.007
Missio André L, Mattos BD, Ferreira DF, Magalhães WLE, Bertuol DA, Gatto DA, Petutschnigg A, Tondi G (2018) Nanocellulose-tannin films: from trees to sustainable active packaging. J Clean Prod 184:143–151. https://doi.org/10.1016/j.jclepro.2018.02.205
Mitchell JG, Kogure K (2006) Bacterial motility: links to the environment and a driving force for microbial physics. FEMS Microbiol Ecol 55:3–16. https://doi.org/10.1111/j.1574-6941.2005.00003.x
Morelli CL, Mahrous M, Belgacem MN, Branciforti MC, Bretas RES, Bras J (2015) Natural copaiba oil as antibacterial agent for bio-based active packaging. Ind Crop Prod 70:134–141. https://doi.org/10.1016/j.indcrop.2015.03.036
Okahisa Y, Furukawa Y, Ishimoto K, Narita C, Intharapichai K, Ohara H (2018) Comparison of cellulose nanofiber properties produced from different parts of the oil palm tree. Carbohydr Polym 198:313–319. https://doi.org/10.1016/j.carbpol.2018.06.089
Paschoalick TM, Garcia FT, Sobral PJA, Habitante AMQB (2003) Characterization of some functional properties of edible films based on muscle proteins of Nile tilapia. Food Hydrocoll 17:419–427. https://doi.org/10.1016/S0268-005X(03)00031-6
Pena DWP, Tonoli GHD, de Paula PT et al (2021) Exfoliating agents for skincare soaps obtained from the crabwood waste bagasse, a natural abrasive from Amazonia. Waste Biomass Valor 12:4441–4461. https://doi.org/10.1007/s12649-020-01336-3
Pizzi A (2008) Tannins: major sources, properties and applications. In: Belgacem MN, Gandini A (eds) Monomers, polymers and composites from renewable resources. Elsevier, Amsterdam, p 553
Protásio TP, Scatolino MV, Araújo ACC, Oliveira AFCF, Figueiredo ICR, Assis MR, Trugilho PF (2019) Assessing proximate composition, extractive concentration, and lignin quality to determine appropriate parameters for selection of superior Eucalyptus firewood. BioEnergy Res 12:626–641. https://doi.org/10.1007/s12155-019-10004-x
Protásio TP, Scatolino MV, Lima MDR, Araújo ACC, Figueiredo ICR, Bufalino L, Hein PRG, Trugilho PF (2020) Insights in quantitative indexes for better grouping and classification of eucalyptus clones used in combustion and energy cogeneration processes in Brazil. Biomass Bioenergy 143:105835. https://doi.org/10.1016/j.biombioe.2020.105835
Quideau S, Deffieux D, Douat-Casassus C, Pouységu L (2011) Plant polyphenols: chemical properties, biological activities and synthesis. Angew Chem Int Ed 50:586–621. https://doi.org/10.1002/anie.201000044
Santana JS, do Rosário JM, Pola CC, Otoni CG, Soares NFF, Camilloto GP, Cruz RS (2017) Cassava starch-based nanocomposites reinforced with cellulose nanofibrils extracted from sisal. J Appl Polym Sci 134:44637. https://doi.org/10.1002/app.44637
Santos JG (2019) The thermodynamic method of vitrification of copaíba oil-resin (Copaifera Langsdorffii). Int J of Sci Res, 8. https://www.ijsr.net/archive/v8i2/ART20194751. Accessed on 14 May 2021
Scandinavian Pulp, Paper and Board Testing Committee (2000) Method SCAN-C 62:00, Water retention value of chemical pulps.
Scatolino MV, Bufalino L, Mendes LM, Guimarães Júnior M, Tonoli GHD (2017) Impact of nanofibrillation degree of eucalyptus and Amazonian hardwood sawdust on physical properties of cellulose nanofibril films. Wood Sci Technol 51:1095–1115. https://doi.org/10.1007/s00226-017-0927-4
Scatolino MV, Fonseca CS, da Silva GM et al (2018) How the surface wettability and modulus of elasticity of the Amazonian paricá nanofibrils films are affected by the chemical changes of the natural fibers. Eur J Wood Prod 76:1581–1594. https://doi.org/10.1007/s00107-018-1343-7
Schindelin J, Arganda-Carreras I, Frise E, Kaynig V, Longair M, Pietzsch T, Preibisch S, Rueden C, Saalfeld S, Schmid B, Tinevez JY, White DJ, Hartenstein V, Eliceiri K, Tomancak P, Cardona A (2012) Fiji: an open-source platform for biological-image analysis. Nature methods 9:676–682. https://doi.org/10.1038/nmeth.2019
Souza LO, Lessa OA, Dias MC, Tonoli GHD, Rezende DVB, Martins MA, Neves ICO, de Resende JV, Carvalho EEN, Vilas Boas EVB, de Oliveira JR, Franco M (2019) Study of morphological properties and rheological parameters of cellulose nanofibrils of cocoa shell (Theobroma cacao L.). Carbohydr Polym 214:152–158. https://doi.org/10.1016/j.carbpol.2019.03.037
Stark NM (2016) Opportunities for cellulose nanomaterials in packaging films: a review and future trends. J Renew Mater 4:313–326. https://doi.org/10.7569/JRM.2016.634115
Su J, Yuan X, Huang Z, Wang X, Lu X, Zhang L, Wang S (2012) Physicochemical properties of soy protein isolate/carboxymethyl cellulose blend films crosslinked by Maillard reactions: color, transparency and heat-sealing ability. Mater Sci Eng C 32:40–46. https://doi.org/10.1016/j.msec.2011.09.009
TAPPI (2002) Technical Association of the Pulp and Paper Industry T 222 om-02, Acid insoluble lignin in wood and pulp
TAPPI (2012a) Technical Association of the Pulp and Paper Industry T 211 om-12, Ash in wood, pulp, paper, and paperboard: combustion at 525°C.
TAPPI (2012b) Technical Association of the Pulp and Paper Industry T 559 cm-12, Grease resistance test for paper and paperboard.
TAPPI (2017) Technical Association of the Pulp and Paper Industry T 204 cm-17, Solvent extractives of wood and pulp.
Trindade R, da Silva JK, Setzer WN (2018) Copaifera of the neotropics: a review of the phytochemistry and pharmacology. Int J Mol Sci 19:1511. https://doi.org/10.3390/ijms19051511
Veiga Junior VF, Pinto AC (2002) The Copaifera L. genus. Quim Nova 25:273–286. https://doi.org/10.1590/S0100-40422002000200016
Xie H, Zhang H, Liu X, Tian S, Liu Y, Fu S (2021) Ag immobilized lignin-based PU coating: a promising candidate to promote the mechanical properties, thermal stability, and antibacterial property of paper packaging. Int J Biol Macromol 189:690–697. https://doi.org/10.1016/j.ijbiomac.2021.08.184
Yue Y, Han J, Han G, Zhang Q, French AD, Wu Q (2015) Characterization of cellulose I/II hybrid fibers isolated from energycane bagasse during the delignification process: morphology, crystallinity and percentage estimation. Carbohydr Polym 133:438–447. https://doi.org/10.1016/j.carbpol.2015.07.058
Zhang C, Wu H, Kessler MR (2015) High bio-content polyurethane composites with urethane modified lignin as filler. Polymer 69:52–57. https://doi.org/10.1016/j.polymer.2015.05.046
Zhang C, Nair SS, Chen H, Yan N, Farnood R, Li F (2019) Thermally stable, enhanced water barrier, high strength starch bio-composite reinforced with lignin containing cellulose nanofibrils. Carbohydr Polym 230:115626. https://doi.org/10.1016/j.carbpol.2019.115626
Zhou Y, Zhou X, Li B, Xu Y, Essawy H, Wu Z, Du G (2019) Tannin-furanic resin foam reinforced with cellulose nanofibers (CNF). Ind Crop Prod 134:107–112
Acknowledgements
The authors thank the Coordenacão de Aperfeiçoamento de Pessoa de Nível Superior (CAPES, Brazil), Conselho Nacional de Desenvolvimento Científico e Tecnológico (CNPq, finance code 300985/2022-3) for their financial support. Thanks also to the Brazilian Lignocellulosic Composites and Nanocomposites Network (RELIGAR), to the Biomaterials Engineering Graduation Program (PPGBIOMAT-UFLA, Brazil), and to State University of Amapa (UEAP) and Foundation for Research Support of Amapa (FAPEAP) (finance code 0022.0279.1202.0016/2021 - Edital 003/2021 postdoc scholarship). Finally, thanks go to the Laboratory of Electron Microscopy and Analysis of the Ultrastructural Federal University of Lavras, (http://www.prp.ufla.br/labs/microscopiaeletronica/) for the technical support for experiments involving electron microscopy.
Funding
Foundation for Research Support of Minas Gerais (FAPEMIG). Conselho Nacional de Desenvolvimento Científico e Tecnológico (CNPq, finance code 300985/2022-3). State University of Amapa (UEAP) and Foundation for Research Support of Amapa (FAPEAP) (finance code 0022.0279.1202.0016/2021 - Edital 003/2021 postdoc scholarship).
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MVS contributed with the writing of the initial version, review, data collection, and data analysis. LB and MCD were major contributors in writing the manuscript, specifically writing the initial version, review, and editing of the manuscript. MSS and LMM contributed to the search for new raw materials resources and review. TMS, GHDT, and FTAJ contributed with supervision, conceptualization, funding acquisition, and project administration. All authors read and approved the final manuscript.
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Scatolino, M.V., Bufalino, L., Dias, M.C. et al. Copaiba oil and vegetal tannin as functionalizing agents for açai nanofibril films: valorization of forest wastes from Amazonia. Environ Sci Pollut Res 29, 66422–66437 (2022). https://doi.org/10.1007/s11356-022-20520-7
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DOI: https://doi.org/10.1007/s11356-022-20520-7