Abstract
The difficulty of dispersing cellulose nanocrystals (CNCs) in poly(lactic acid) (PLA) was still a primary obstacle to enhance the properties of PLA nanocomposites. In this work, two different methods were used to modify CNCs that were then added dropwise and mixed with the PLA solution to conveniently obtain the composites. Transmission electron microscopy and Fourier transform infrared spectroscopy were used to characterize CNCs before and after modification. Ultraviolet–visible spectroscopy, tensile tests, differential scanning calorimetry, and thermogravimetric analysis were used to characterize the PLA nanocomposites. The results revealed that the CNCs that were modified with surfactant had better dispersion and thermal stability in the PLA nanocomposites. The Young’s modulus and strength of PLA/SCNC nanocomposites were significantly reinforced (up to 66.0% and 29.8%, respectively). Meanwhile, the transmittance remained above 60% in the visible range. The solution precipitation approach was effective and simple, which could be used with other polymers.
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Abitbol T, Kloser E, Gray DG (2013) Estimation of the surface sulfur content of cellulose nanocrystals prepared by sulfuric acid hydrolysis. Cellulose 20(2):785–794
Alvarado N, Romero J, Torres A, Lopez De Dicastillo C, Rojas A, Jose Galotto M (2018) Supercritical impregnation of thymol in poly(lactic acid) filled with electrospun poly(vinyl alcohol)-cellulose nanocrystals nanofibers: development an active food packaging material. J Food Eng 217:1–10
Ansari F, Salajkova M, Zhou Q, Berglund LA (2015) Strong surface treatment effects on reinforcement efficiency in biocomposites based on cellulose nanocrystals in poly(vinyl acetate) matrix. Biomacromolecules 16(12):3916–3924
Arrieta MP, Fortunati E, Dominici F, Rayon E, Lopez J, Kenny JM (2014) Multifunctional PLA-PHB/cellulose nanocrystal films: processing, structural and thermal properties. Carbohydr Polym 107:16–24
Aulin C, Karabulut E, Amy T, Wagberg L, Lindstrom T (2013) Transparent nanocellulosic multilayer thin films on polylactic acid with tunable gas barrier properties. ACS Appl Mater Interfaces 5(15):7352–7359
Azeredo HMC, Rosa MF, Mattoso LHC (2017) Nanocellulose in bio-based food packaging applications. Ind Crop Prod 97:664–671
Bezerra Lima EM, Lima AM, Silva Minguita AP, Rojas Dos Santos NR, Soares Pereira IC, Matta Neves TT (2019) Poly(lactic acid) biocomposites with mango waste and organo-montmorillonite for packaging. J Appl Polym Sci 136:4751221
Boujemaoui A, Mongkhontreerat S, Malmstrom E, Carlmark A (2015) Preparation and characterization of functionalized cellulose nanocrystals. Carbohydr Polym 115:457–464
Brinatti C, Huang J, Berry RM, Tam KC, Loh W (2016) Structural and energetic studies on the interaction of cationic surfactants and cellulose nanocrystals. Langmuir 32(3):689–698
Chi K, Catchmark JM (2017) Enhanced dispersion and interface compatibilization of crystalline nanocellulose in polylactide by surfactant adsorption. Cellulose 24(11):4845–4860
Dhar P, Kumar A, Katiyar V (2016a) Magnetic cellulose nanocrystal based anisotropic polylactic acid nanocomposite films: influence on electrical, magnetic, thermal, and mechanical properties. ACS Appl Mater Interfaces 8(28):18393–18409
Dhar P, Tarafder D, Kumar A, Katiyar V (2016b) Thermally recyclable polylactic acid/cellulose nanocrystal films through reactive extrusion process. Polymer 87:268–282
Dhar P, Gaur SS, Soundararajan N, Gupta A, Bhasney SM, Milli M (2017) Reactive extrusion of polylactic acid/cellulose nanocrystal films for food packaging applications: influence of filler type on thermomechanical, rheological, and barrier properties. Ind Eng Chem Res 56(16):4718–4735
Fortunati E, Peltzer M, Armentano I, Torre L, Jimenez A, Kenny JM (2012) Effects of modified cellulose nanocrystals on the barrier and migration properties of PLA nano-biocomposites. Carbohydr Polym 90(2):948–956
Fortunati E, Luzi F, Puglia D, Petrucci R, Kenny JM, Torre L (2015) Processing of PLA nanocomposites with cellulose nanocrystals extracted from Posidonia oceanica waste: innovative reuse of coastal plant. Ind Crop Prod 67:439–447
Gan PG, Sam ST, Bin Abdullah MF, Omar MF (2019) Thermal properties of nanocellulose-reinforced composites: a review. J Appl Polym Sci 137:48544
Gupta A, Simmons W, Schueneman GT, Hylton D, Mintz EA (2017) Rheological and thermo-mechanical properties of poly(lactic acid)/lignin-coated cellulose nanocrystal composites. ACS Sustain Chem Eng 5(2):1711–1720
Hamad K, Kaseem M, Ayyoob M, Joo J, Deri F (2018) Polylactic acid blends: the future of green, light and tough. Prog Polym Sci 85:83–127
Hong JS, Srivastava D, Lee I (2018) Fabrication of poly(lactic acid) nano- and microparticles using a nanomixer via nanoprecipitation or emulsion diffusion. J Appl Polym Sci 135:4619918
Hu C, Li Z, Wang Y, Gao J, Dai K, Zheng G (2017) Comparative assessment of the strain-sensing behaviors of polylactic acid nanocomposites: reduced graphene oxide or carbon nanotubes. J Mater Chem C 5(9):2318–2328
Huang L, Ye Z, Berry R (2016) Modification of cellulose nanocrystals with quaternary ammonium-containing hyperbranched polyethylene ionomers by ionic assembly. ACS Sustain Chem Eng 4(9):4937–4950
Kaboorani A, Riedl B (2015) Surface modification of cellulose nanocrystals (CNC) by a cationic surfactant. Ind Crop Prod 65:45–55
Kargarzadeh H, Huang J, Lin N, Ahmad I, Mariano M, Dufresne A (2018) Recent developments in nanocellulose-based biodegradable polymers, thermoplastic polymers, and porous nanocomposites. Prog Polym Sci 87:197–227
Khalil HPSA, Banerjee A, Saurabh CK, Tye YY, Suriani AB, Mohamed A (2018) Biodegradable films for fruits and vegetables packaging application: preparation and properties. Food Eng Rev 10(3):139–153
Kian LK, Saba N, Jawaid M, Sultan MTH (2019) A review on processing techniques of bast fibers nanocellulose and its polylactic acid (PLA) nanocomposites. Int J Biol Macromol 121:1314–1328
Lepeltier E, Bourgaux C, Couvreur P (2014) Nanoprecipitation and the “Ouzo effect”: application to drug delivery devices. Adv Drug Deliv Rev 71:86–97
Lizundia E, Fortunati E, Dominici F, Luis Vilas J, Manuel Leon L, Armentano I (2016) PLLA-grafted cellulose nanocrystals: role of the CNC content and grafting on the PLA bionanocomposite film properties. Carbohydr Polym 142:105–113
Luzi F, Fortunati E, Jimenez A, Puglia D, Pezzolla D, Gigliotti G (2016) Production and characterization of PLA_PBS biodegradable blends reinforced with cellulose nanocrystals extracted from hemp fibres. Ind Crop Prod 93(SI):276–289
Mariano M, Pilate F, de Oliveira FB, Khelifa F, Dubois P, Raquez J, Dufresne A (2017) Preparation of cellulose nanocrystal-reinforced poly(lactic acid) nanocomposites through noncovalent modification with PLLA-based surfactants. ACS OMEGA 2(6):2678–2688
Monika Dhar P, Katiyar V (2017) Thermal degradation kinetics of polylactic acid/acid fabricated cellulose nanocrystal based bionanocomposites. Int J Biol Macromol 104(A):827–836
Mujica-Garcia A, Hooshmand S, Skrifvars M, Kenny JM, Oksman K, Peponi L (2016) Poly(lactic acid) melt-spun fibers reinforced with functionalized cellulose nanocrystals. RSC Adv 6(11):9221–9231
Murariu M, Doumbia A, Bonnaud L, Dechief A, Paint Y, Ferreira M (2011) High-performance polylactide/ZnO nanocomposites designed for films and fibers with special end-use properties. Biomacromolecules 12(5):1762–1771
Nagalakshmaiah M, El Kissi N, Dufresne A (2016) Ionic compatibilization of cellulose nanocrystals with quaternary ammonium salt and their melt extrusion with polypropylene. ACS Appl Mater Interfaces 8(13):8755–8764
Nair SS, Chen H, Peng Y, Huang Y, Yan N (2018) Polylactic acid biocomposites reinforced with nanocellulose fibrils with high lignin content for improved mechanical, thermal, and barrier properties. ACS Sustain Chem Eng 6(8):10058–10068
Natterodt JC, Shirole A, Sapkota J, Zoppe JO, Weder C (2018) Polymer nanocomposites with cellulose nanocrystals made by co-precipitation. J Appl Polym Sci 135:4564824SI
Patel DK, Dutta SD, Lim K (2019) Nanocellulose-based polymer hybrids and their emerging applications in biomedical engineering and water purification. RSC Adv 9(33):19143–19162
Peelman N, Ragaert P, De Meulenaer B, Adons D, Peeters R, Cardon L (2013) Application of bioplastics for food packaging. Trends Food Sci Technol 32(2):128–141
Pei A, Zhou Q, Berglund LA (2010) Functionalized cellulose nanocrystals as biobased nucleation agents in poly(l-lactide) (PLLA)—crystallization and mechanical property effects. Compos Sci Technol 70(5):815–821
Petersson L, Kvien I, Oksman K (2007) Structure and thermal properties of poly(lactic acid)/cellulose whiskers nanocomposite materials. Compos Sci Technol 67(11–12):2535–2544
Rabanel J, Faivre J, Tehrani SF, Lalloz A, Hildgen P, Banquy X (2015) Effect of the polymer architecture on the structural and biophysical properties of PEG-PLA nanoparticles. ACS Appl Mater Interfaces 7(19):10374–10385
Ranjbar D, Raeiszadeh M, Lewis L, MacLachlan MJ, Hatzikiriakos SG (2020) Adsorptive removal of Congo red by surfactant modified cellulose nanocrystals: a kinetic, equilibrium, and mechanistic investigation. Cellulose 27(6):3211–3232
Rasal RM, Janorkar AV, Hirt DE (2010) Poly(lactic acid) modifications. Prog Polym Sci 35(3):338–356
Rhim J, Park H, Ha C (2013) Bio-nanocomposites for food packaging applications. Prog Polym Sci 38(10–11):1629–1652
Robles E, Urruzola I, Labidi J, Serrano L (2015) Surface-modified nano-cellulose as reinforcement in poly(lactic acid) to conform new composites. Ind Crop Prod 71:44–53
Roman M, Winter WT (2004) Effect of sulfate groups from sulfuric acid hydrolysis on the thermal degradation behavior of bacterial cellulose. Biomacromolecules 5(5):1671–1677
Salajkova M, Berglund LA, Zhou Q (2012) Hydrophobic cellulose nanocrystals modified with quaternary ammonium salts. J Mater Chem 22(37):19798–19805
Scaffaro R, Maio A, Lopresti F (2019) Effect of graphene and fabrication technique on the release kinetics of carvacrol from polylactic acid. Compos Sci Technol 169:60–69
Shojaeiarani J, Bajwa DS, Stark NM (2018) Spin-coating: a new approach for improving dispersion of cellulose nanocrystals and mechanical properties of poly(lactic acid) composites. Carbohydr Polym 190:139–147
Siakeng R, Jawaid M, Ariffin H, Sapuan SM, Asim M, Saba N (2019) Natural fiber reinforced polylactic acid composites: a review. Polym Compos 40(2):446–463
Spinella S, Lo Re G, Liu B, Dorgan J, Habibi Y, Leclere P (2015) Polylactide/cellulose nanocrystal nanocomposites: efficient routes for nanofiber modification and effects of nanofiber chemistry on PLA reinforcement. Polymer 65:9–17
Sung SH, Chang Y, Han J (2017) Development of polylactic acid nanocomposite films reinforced with cellulose nanocrystals derived from coffee silverskin. Carbohydr Polym 169:495–503
Turner JF, Riga A, O’Connor A, Zhang J, Collis J (2004) Characterization of drawn and undrawn poly-l-lactide films by differential scanning calorimetry. J Therm Anal Calorim 75(1):257–268
Vatansever E, Arslan D, Nofar M (2019) Polylactide cellulose-based nanocomposites. Int J Biol Macromol 137:912–938
Wang T, Drzal LT (2012) Cellulose-nanofiber-reinforced poly(lactic acid) composites prepared by a water-based approach. ACS Appl Mater Interfaces 4(10):5079–5085
Wang W, Liang T, Zhang B, Bai H, Ma P, Dong W (2018) Green functionalization of cellulose nanocrystals for application in reinforced poly(methyl methacrylate) nanocomposites. Carbohydr Polym 202:591–599
Wang Z, Yao Z, Zhou J, He M, Jiang Q, Li A, Li S, Liu M, Luo S, Zhang D (2019) Improvement of polylactic acid film properties through the addition of cellulose nanocrystals isolated from waste cotton cloth. Int J Biol Macromol 129:878–886
Wu H, Nagarajan S, Zhou L, Duan Y, Zhang J (2016) Synthesis and characterization of cellulose nanocrystal-graft-poly(d-lactide) and its nanocomposite with poly(l-lactide). Polymer 103:365–375
Wu H, Nagarajan S, Shu J, Zhang T, Zhou L, Duan Y, Zhang J (2018) Green and facile surface modification of cellulose nanocrystal as the route to produce poly(lactic acid) nanocomposites with improved properties. Carbohydr Polym 197:204–214
Xie Q, Wang S, Chen X, Zhou Y, Fang H, Li X, Cheng S, Ding Y (2018) Thermal stability and crystallization behavior of cellulose nanocrystals and their poly(l-lactide) nanocomposites: effects of surface ionic group and poly(d-lactide) grafting. Cellulose 25(12):6847–6862
Xu C, Chen J, Wu D, Chen Y, Lv Q, Wang M (2016) Polylactide/acetylated nanocrystalline cellulose composites prepared by a continuous route: a phase interface-property relation study. Carbohydr Polym 146:58–66
Xu T, Yang H, Yang D, Yu Z (2017) Polylactic acid nanofiber Scaffold decorated with chitosan islandlike topography for bone tissue engineering. ACS Appl Mater Interfaces 9(25):21094–21104
Yin Y, Zhao L, Jiang X, Wang H, Gao W (2017) Poly(lactic acid)-based biocomposites reinforced with modified cellulose nanocrystals. Cellulose 24(11):4773–4784
Yin Y, Ma J, Tian X, Jiang X, Wang H, Gao W (2018) Cellulose nanocrystals functionalized with amino-silane and epoxy-poly(ethylene glycol) for reinforcement and flexibilization of poly(lactic acid): material preparation and compatibility mechanism. Cellullose 25(11):6447–6463
Yu H, Wang C, Abdalkarim SYH (2017a) Cellulose nanocrystals/polyethylene glycol as bifunctional reinforcing/compatibilizing agents in poly(lactic acid) nanofibers for controlling long-term in vitro drug release. Cellulose 24(10):4461–4477
Yu H, Zhang H, Song M, Zhou Y, Yao J, Ni Q (2017b) From cellulose nanospheres, nanorods to nanofibers: various aspect ratio induced nucleation/reinforcing effects on polylactic acid for robust-barrier food packaging. ACS Appl Mater Interfaces 9(50):43920–43938
Zhang Y, Jiang Y, Han L, Wang B, Xu H, Zhong Y (2018) Biodegradable regenerated cellulose-dispersed composites with improved properties via a pickering emulsion process. Carbohydr Polym 179:86–92
Acknowledgments
This work was supported by the National Natural Science Foundation of China (No. 31670569) and the Fundamental Research Funds for the Central Universities (No. 2572019CG05). The work was supported by a Postdoctoral Science Foundation Funded Project (LBH-Q17003).
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Li, C., Sun, C., Wang, C. et al. Cellulose nanocrystal reinforced poly(lactic acid) nanocomposites prepared by a solution precipitation approach. Cellulose 27, 7489–7502 (2020). https://doi.org/10.1007/s10570-020-03294-4
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DOI: https://doi.org/10.1007/s10570-020-03294-4