Abstract
Structural, thermal and mechanical properties of the compostable composites comprising a biodegradable aliphatic–aromatic copolyester (namely, the poly(butylene adipate-co-terephthalate; PBAT), and microcrystalline cellulose (MCC) derived from agricultural waste, the wheat stalk, were investigated. Purely physical interaction between the components was found to be responsible to get the MCC phase quite uniformly embedded in the PBAT matrix, the latter being the dominating component of the composites surface. There were two distinct thermally activated degradation regimes characterized by separate activation processes corresponding to the decomposition of the MCC and the PBAT phases, respectively. The physically bound and rather weak but large PBAT–MCC interfacial areas provoked more rapid thermal degradation of the composites compared to the pure components. While the PBAT acted as a highly ductile material upon tensile loading, the composites maintained high ductility only up to 20% by weight of the MCC. The drastic reduction in the ductility for higher filler loading was attributed to the possible void formation at the interfacial region followed by crack initiation and propagation leading eventually to the premature specimen fracture. The composite materials thus fabricated were hence found to suit for low-load bearing applications.
Similar content being viewed by others
References
Srinivas K, Naidu AL, Bahubalendruni MVAR (2017) A review on chemical and mechanical properties of natural fiber reinforced polymer composites. Int J Performability Eng 13:189–200. https://doi.org/10.23940/ijpe.17.02.p8.189200
Prasad AVR, Rao KM (2011) Mechanical properties of natural fibre reinforces polyester composites: Jowar, sisal and bamboo. Mater Des 32:4658–4663. https://doi.org/10.1016/j.matdes.2011.03.015
Mandal A, Chakrabarty D (2014) 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 20:462–473. https://doi.org/10.1016/j.jiec.2013.05.003
Wang KH, Wu TM, Shih YF, Huang CM (2008) Water bamboo husk reinforced poly(lactic acid) green composites. Polym Eng Sci 48:1833–1839. https://doi.org/10.1002/pen.21151
Kowalczyk M, Piorkowska E, Kulpinski P, Pracella M (2011) Mechanical and thermal properties of PLA composites with cellulose nanofibers and standard size fibers. Compos Part A Appl Sci Manuf 42:1509–1514. https://doi.org/10.1016/j.compositesa.2011.07.003
Vinayaka DL, Guna VK, Madhavi D, Arpitha M, Reddy N (2017) Ricinus communis plant residues as a source for natural cellulose fibers potentially exploitable in polymer. Ind Crops Prod 100:126–131. https://doi.org/10.1016/j.indcrop.2017.02.019
Liu DY, Yuan XW, Bhattacharyya D, Easteal AJ (2010) Characterisation of solution cast cellulose nanofibre-reinforced poly(lactic acid). eXPRESS Polym Lett 4:26–31. https://doi.org/10.3144/expresspolymlett.2010.5
Giri J, Lach R, Grellmann W, Susan ABH, Saiter JM, Henning S, Katiyar V, Adhikari R (2019) Compostable composites of wheat stalk microcrystalline cellulose and poly(butylene adipate-co-terephthalate): surface properties and degradation behaviour. J Appl Polym Sci 136:48149. https://doi.org/10.1002/app.48149
Wu CS (2012) Characterization of cellulose acetate-reinforced aliphatic-aromatic copolyester composites. Carbohydr Polym 87:1249–1256. https://doi.org/10.1016/j.carbpol.2011.09.009
Pires M, Murariu M, Cardoso AM, Bonnaud L, Dubois P (2020) Thermal degradation of poly(lactic acid)–zeolite composites produced by melt-blending. Polym Bull 77:2111–2137. https://doi.org/10.1007/s00289-019-02846-4
de Oliveira AG, Morenos JF, de Sousa AFS, Escisio VA, Guimaraes MJdOC, da Silva ALN (2019) Composites based on high-density polyethylene, polylactide and calcium carbonate: Effect of calcium carbonate nanoparticles as co-compatibilizers. Polym Bull. https://doi.org/10.1007/s00289-019-02887-9
Siyamak S, Ibrahim NA, Abdolmohammadi S, Yunus WMZBW, Rahman MZA (2012) Enhancement of mechanical and thermal properties of oil palm empty bunch fiber poly(butylenes adipate-co-terephthalate) biocomposites by matrix esterification using succinic anhydride. Molecules 17:1969–1991. https://doi.org/10.3390/molecules17021969
Ibrahim NA (2010) Effect of fiber treatment on the mechanical properties of kenaf fiber–ecoflex composites. J Reinf Plast Compos 29:2192–2198. https://doi.org/10.1177/0731684409347592
Nagata M, Inaki K (2011) Biodegradable and photocurable multiblock copolymers with shape-memory properties from poly(ɛ-caprolactone) diol, poly(ethylene glycol), and 5-cinnamoyloxysophthalic acid. J Appl Polym Sci 120:3556–3564. https://doi.org/10.1002/app.33531
Adhikari R, Bhandari NL, Causin V, Le HH, Radusch HJ, Michler GH, Saiter JM (2012) Study of morphology, mechanical properties, and thermal behavior of green aliphatic–aromatic copolyester/bamboo flour composites. Polym Eng Sci 52:2297–2303. https://doi.org/10.1002/pen.23335
Cho MJ, Park BD (2011) Tensile and thermal properties of nanocellulose-reinforced poly(vinyl alcohol) Nanocomposites. J Ind Eng Chem 17:36–40. https://doi.org/10.1016/j.jiec.2010.10.006
Zhou L, He H, Jiang C, Ma L, Yu P (2017) Cellulose nanocrystals from cotton stalk for reinforcement of poly(vinyl alcohol) composites. Cellulose Chem Technol 51:109–119
Sonia A, Dasan KP (2013) Cellulose microfibers (CMF)/poly(ethylene-co-vinyl acetate) (EVA) composites for the food packaging application: a study based on barrier and biodegradation behavior. J Food Eng 118:78–89. https://doi.org/10.1016/j.jfoodeng.2013.03.020
Pokhrel S, Lach R, Le HH, Wutzler A, Grellmann W, Radusch HJ, Dhakal RP, Esposito A, Henning S, Yadav PN, Saiter JM, Heinrich G, Adhikari R (2016) Fabrication and characterization of completely biodegradable copolyester–chitosan blends: I. Spectroscopic and thermal characterization. Macromol Symp 366:23–34. https://doi.org/10.1002/masy.201650043
Adsul M, Soni SK, Bhargava SK, Bansal V (2012) Facile approach for the dispersion of regenerated cellulose in aqueous system in the form of nanoparticles. Biomacromolecules 13:2890–2895. https://doi.org/10.1021/bm3009022
Cherian BM, Lopes Leao A, Ferreira de Souza S, Manzine Costa L, Molina de Olyveira G, Kottaisamy M, Nagarajan ER, Thomas S (2011) Cellulose nanocomposites with nanofibres isolated from pineapple leaf fibers for medical applications. Carbohydr Polym 86:1790–1798. https://doi.org/10.1016/j.carbpol.2011.07.009
Hamedi MM, Hajian A, Fall AB, Hakansson K, Salajikova M, Lundell F, Wagberg L, Berglund LA (2014) Highly conducting, strong nanocomposites based on nanocellulose-assisted aqueous dispersions of single-wall carbon nanotubes. ACS Nano 8:2467–2476. https://doi.org/10.1021/nn4060368
Sanjay MR, Arpitha GR, Naik LL, Gopalakrisha K, Yogesha B (2016) Applications of natural fibers and its composites: an overview. Nat Resour 7:108–114. https://doi.org/10.4236/nr.2016.73011
Das M, Chakraborty D (2009) The effect of alkalization and fiber loading on the mechanical properties of bamboo fiber composites, Part 1: Polyester resin matrix. J Appl Polym Sci 112:489–495. https://doi.org/10.1002/app.29342
Teamsinsungvon A, Ruksakulpiwat Y, Jarukumjorn K (2010) Properties of biodegradable poly(lactic acid)/poly(butylene adipate-co-terephthalate)/calcium carbonate composites. Adv Mater Res 123–125:193–196. https://doi.org/10.4028/www.scientific.net/AMR.123-125.193
Pereda M, Amica G, Racz I, Marcovinch NE (2011) Structure and properties of nanocomposite films based on the sodium caseinate and nanocellulose fibers. J Food Eng 103:76–83. https://doi.org/10.1016/j.jfoodeng.2010.10.001
Trovatti E, Fernandes SCM, Rubatat L, da Silva PD, Freire CSR, Silverstre AJD, Neto CP (2012) Pullulan–nanofibrillated cellulose composites films with improved thermal and mechanical properties. Compos Sci Technol 72:1556–1561. https://doi.org/10.1016/j.compscitech.2012.06.003
Yu T, Li Y (2014) Influence of poly(butylenes adipate-co-terephthalate) on the properties of the biodegradable composites base on ramie/poly(lactic acid). Compos Part A Appl Sci Manuf 58:24–29. https://doi.org/10.1016/j.compositesa.2013.11.013
Pandey JP, Takagi H, Nakagaito AN, Saini DR, Ahn SH (2012) An overview on the cellulose based conducting composites. Compos Part B Eng 43:2822–2826. https://doi.org/10.1016/j.compositesb.2012.04.045
ElNahrawy AM, Haroun AA, Hamadneh I, Al-Dujailid AH, Kamel S (2017) Conducting cellulose/TiO2 composites by in situ polymerization of pyrrole. Carbohydr Polym 168:182–190. https://doi.org/10.1016/j.carbpol.2017.03.066
Mulinari DR, Voorwald HJC, Cioffi MO, da Silva MLCP (2017) Cellulose fiber-reinforced high-density polyethylene composites—mechanical and thermal properties. J Compos Mater 51:1807–1815. https://doi.org/10.1177/0021998316665241
Dayo AQ, Gao BC, Wang J, Liu WB, Derradji M, Shah AH, Babar AA (2017) Natural hemp fiber reinforced polybenzoxazine composites: curing behavior, mechanical and thermal properties. Compos Sci Technol 144:114–124. https://doi.org/10.1016/j.compscitech.2017.03.024
Ng LF, Malingam SD, Selamat MZ, Mustafa Z, Bapokutty O (2020) A comparison study on the mechanical properties of composites based on kenaf and pineapple leaf fibres. Polym Bull 77:1449–1463. https://doi.org/10.1007/s00289-019-02812-0
Siyamak S, Ibrahim NA, Abdolmohammadi S, Yunus WMZW, Rahman MZAB (2012) Effect of fiber esterification on fundamental properties of oil palm empty fruit bunch fiber/poly(butylenes adipate-co-terephthalate) biocomposites. Int J Mol Sci 13:1327–1346. https://doi.org/10.3390/ijms13021327
Pang JH, Liu X, Wu M, Wu YY, Zhang XM, Sun RC (2014) Fabrication and characterization of regenerated cellulose films using different liquids. J Spectrosc 214057:8. https://doi.org/10.1155/2014/214057
Giri J, Adhikari R (2012) A brief review on extraction of nanocellulose and its application. Bibechana 9:81–87. https://doi.org/10.3126/bibechana.v9i0.7179
Mueller S, Weder C, Foster EJ (2014) Isolation of cellulose nanocrytals from pseudostems of banana plants. RSC Adv 4:907–915. https://doi.org/10.1039/C3RA46390G
Ponce-Reyes CE, Chanona-Perez JJ, Garibay-Febles V, Palacios-Gonzalez E, Karamath J, Terres-Rojas E, Calderon-Dominguez G (2014) Preparation of cellulose nanoparticles from agave waste and its morphological and structural characterization. Rev Mex Ing Quim 13:897–906
Cesar NR, Pereira-da-Silva MA, Botaro VR, de Menezes AJ (2015) Cellulose nanocrystals from natural fiber of the macrophyte Typha domingensis: extraction and characterization. Cellulose 22:449–460. https://doi.org/10.1007/s10570-014-0533-7
Chan CH, Chia CH, Zakaria S, Ahmad I, Dufresne A (2013) Production and characterisation of cellulose and nano-crystalline cellulose from kenaf core wood. BioResources 8:785–794. https://doi.org/10.15376/biores.8.1.785-794
Vinayaka DL, Guna V, Madhavi D, Arpitha M, Reddy N (2017) Ricinus communis residues as a source for natural cellulose fibers potentially exploitable in polymer composites. Ind Crops Prod 100:126–131. https://doi.org/10.1016/j.indcrop.2017.02.019
Cadena Chamorro ME, Velez RJM, Santa JF, Otalvaro GV (2017) Natural fibers from plantain pseudostem (Musa paradisiaca) for use in fiber-reinforced composites. J Nat Fibers 14:678–690. https://doi.org/10.1080/15440478.2016.1266295
Satyamurthy P, Vigneshwaran N (2013) A novel process for synthesis of spherical nanocellulose by controlled hydrolysis of microcrystalline cellulose using anaerobic microbial consortium. Enzyme Microb Technol 52:20–25. https://doi.org/10.1016/j.enzmictec.2012.09.002
Chiu HT, Huang SY, Chen YF, Kuo MT, Chiang TY, Chang CY, Wang YH (2013) Heat treatment effect on the mechanical properties and morphologies of poly (lactic acid)/poly (butylenes adipate-co-terephthalate) blends. Int J Polym Sci 951696:11. https://doi.org/10.1155/2013/951696
Bandera D, Sapkota J, Josset S, Weder C, Tingaut P, Gao X, Foster EJ, Zimmermann T (2014) Influence of mechanical treatment on the properties of cellulose nanofibers isolated from microcrystalline cellulose. React Funct Polym 85:134–141. https://doi.org/10.1016/j.reactfunctpolym.2014.09.009
Pan M, Zhou X, Chen M (2013) Cellulose nanowhiskers isolation and properties from acid hydrolysis combined with high pressure homogenization. BioResources 8:933–943
Dzul-Cervantes M, Herrera-Franco PJ, Tabi T, Valadez-Gonzalez A (2017) Using factorial design methodology to assess PLA-g-Ma and henequen microfibrillated cellulose content on the mechanical properties of poly(lactic acid) composites. Int J Polym Sci 4046862:14. https://doi.org/10.1155/2017/4046862
Sun JX, Sun XF, Zhao H, Sun RC (2004) Isolation and characterization of cellulose from sugarcane bagasse. J Polym Degrad Stab 84:331–339. https://doi.org/10.1016/j.polymdegradstab.2004.02.008
Jonoobi M, Aitomaki Y, Mathew A, Oksman K (2014) Thermoplastic polymer impregnation cellulose nanofibre networks: morphology, mechanical and optical properties. Compos Part A Appl Sci Manuf 58:30–35. https://doi.org/10.1016/j.compositesa.2013.11.010
Abraham E, Elbi PA, Deepa B, Jyotishkumar P, Pothen LA, Narine SS, Thomas S (2012) X-ray diffraction and biodegradation analysis of green composites of natural rubber/nanocellulose. Polym Degrad Stab 97:2378–2387. https://doi.org/10.1016/j.polymdegradstab.2012.07.028
Graupner N, Ziegmann G, Wilde F, Beckmannd F, Müssig J (2016) Procedural influences on compression and injection moulded cellulose fibre-reinforced polylactide (PLA) composites: influence of fibre loading, fibre length, fibre orientation and voids. Compos Part A Appl Sci Manuf 81:158–171. https://doi.org/10.1016/j.compositesa.2015.10.040
Cao X, Wang X, Ding B, Yu J, Sun G (2013) Novel spider web-like nanoporous networks based on jute cellulose nanowhiskers. Carbohydr Polym 92:2041–2047. https://doi.org/10.1016/j.carbpol.2012.11.085
Giri J (2019) Wheat stalk micro- and nanocellulose based degradable polymer composites: morphological, mechanical and degradation behavior, PhD Thesis, Tribhuvan University, Kathmandu
Pandit R (2015) Templating nanostructures in epoxy resin using styrenic block copolymers, PhD Thesis, Tribhuvan University, Kathmandu
Saiter JM, Dobircau L, Saiah R, Sreekumar PA, Galandon A, Gattin R, Leblanc N, Adhikari R (2010) Relaxation map of a 100 % green thermoplastic film. Glass transition and fragility. Phys B 405:900–905. https://doi.org/10.1016/j.physb.2009.10.011
Acknowledgements
JG sincerely acknowledges the Nepal Academy of Science and Technology (NAST) for providing PhD research grants. She further thanks German Research Foundation (DFG) and foundation “Akademie Mitteldeutsche Kunststoffinnovationen” (AMK) for offering financial supports for research stays in Germany.
Author information
Authors and Affiliations
Corresponding authors
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.
Rights and permissions
About this article
Cite this article
Giri, J., Lach, R., Le, H.H. et al. Structural, thermal and mechanical properties of composites of poly(butylene adipate-co-terephthalate) with wheat straw microcrystalline cellulose. Polym. Bull. 78, 4779–4795 (2021). https://doi.org/10.1007/s00289-020-03339-5
Received:
Revised:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1007/s00289-020-03339-5