Effect of High-Energy Ball-Milling Duration on the Physicochemical Properties of Chemically Treated MD2 Pineapple Peel Cellulose
Keywords:
Ball-milling, cellulose, chemical treatment, MD2, pineapple peel, waste valorisationAbstract
MD2 pineapple peel represents an abundant agro-waste rich in cellulose but remains underutilised in high-value applications. This study investigates the influence of ball-milling duration on the physicochemical properties of cellulose extracted from MD2 pineapple peel. The peel was chemically purified via alkaline delignification, bleaching, drying and high-energy ball milling for 0, 60, 90, and 120 min. The extraction yield of 10.6% (dry basis) was obtained using fresh peel with an initial moisture content of 83.4 ± 1.1%. FTIR confirmed removal of lignin and hemicellulose, while XRD showed diffraction patterns consistent with cellulose I, with crystallinity peaking at 60 min before declining with prolonged milling. SEM revealed initial fibre fragmentation and size reduction at 60 min, followed by increased particle agglomeration with prolonged milling. TGA indicated that milled-extracted cellulose exhibited high thermal stability, comparable to that of commercial microcrystalline cellulose. Among the milling durations investigated, 60 min produced the highest measured crystallinity index (66.67%) and the smallest apparent Feret diameter (193.3 ± 46.6 μm) among the extracted cellulose samples, while thermal stability remained comparable among the milled samples (Tmax = 354–355°C). These results highlight the influence of milling duration in refining processing conditions for the effective valorisation of pineapple peel into functional cellulose.
Downloads
Metrics
References
Abolore, R.S., Jaiswal, S. & Jaiswal, A.K. 2024. Green and sustainable pretreatment methods for cellulose extraction from lignocellulosic biomass and its applications: A review. Carbohydrate Polymer Technologies and Applications, 7: 100396. DOI: https://doi.org/10.1016/j.carpta.2023.100396
Ahmima, S., Naar, N., Jędrzejczak, P., Klapiszewska, I., Klapiszewski, L. & Jesionowski, T. 2024. Isolation and characterization of novel cellulose micro/nanofibers from Lygeum spartum through a chemo-mechanical process. Polymers, 16(21): 3001. DOI: https://doi.org/10.3390/polym16213001
Anwar, A., Zhao, T., Ghaffar, S., Nie, K., Xia, W., Wang, L., Cao, Z., Yang, X., Zhou, C. & Zhang, Y. 2024. A novel microwave-assisted $gamma$-valerolactone and glycolic acid pretreatment for green and sustainable production of hemp fibres. Industrial Crops and Products, 222: 119625. DOI: https://doi.org/10.1016/j.indcrop.2024.119625
AOAC International. 2000. Official Methods of Analysis of AOAC International. 17th Ed. AOAC International, Gaithersburg.
Ardila A., A.N., Arriola-Villaseñor, E., González, E.E.V., Guerrero, H.E.G., Hernández-Maldonado, J.A., Gutiérrez-Pineda, E. & Villa, C.C. 2024. Enhanced cellulose extraction from banana pseudostem waste: A comparative analysis using chemical methods assisted by conventional and focused ultrasound. Polymers, 16(19): 2785. DOI: https://doi.org/10.3390/polym16192785
Dai, H., Ou, S., Liu, Z. & Huang, H. 2017. Pineapple peel carboxymethyl cellulose/polyvinyl alcohol/mesoporous silica SBA-15 hydrogel composites for papain immobilization. Carbohydrate Polymers, 169: 504-514. DOI: https://doi.org/10.1016/j.carbpol.2017.04.057
Dai, H., Ou, S., Huang, Y. & Huang, H. 2018. Utilization of pineapple peel for production of nanocellulose and film application. Cellulose, 25(3): 1743-1756. DOI: https://doi.org/10.1007/s10570-018-1671-0
de Souza Fonseca, A., Panthapulakkal, S., Konar, S.K., Sain, M., Bufalino, L., Raabe, J., de Andrade Miranda, I.P., Martins, M.A. & Tonoli, G.H.D. 2019. Improving cellulose nanofibrillation of non-wood fiber using alkaline and bleaching pre-treatments. Industrial Crops and Products, 131: 203-212. DOI: https://doi.org/10.1016/j.indcrop.2019.01.046
Duc, C.K.T., Tuan, N.T., Linh, T.C., Luong, H.V.T. & Pham, D.T. 2026. Sustainable recovery of cellulose from lotus seedpods: Integrating process optimization and environmental-preliminary economic analysis. Bioresource Technology, 441: 133603. DOI: https://doi.org/10.1016/j.biortech.2025.133603
Fan, J., Zhang, S., Li, F., Yang, Y. & Du, M. 2020. Recent advances in cellulose-based membranes for their sensing applications. Cellulose, 27(16): 9157-9179. DOI: https://doi.org/10.1007/s10570-020-03445-7
FAOSTAT. 2026. Food and Agriculture Organization of the United Nations Statistics Division. Available at: https://www.fao.org/faostat/en/#home (Accessed: January 2026).
Ghazi, N.A.M., Khairuddin, F. & Noor, W.N.W.M. 2023. The factors that influence operation risk on pineapple production: A case study in Muar, Johor. IOP Conference Series: Earth and Environmental Science, 1182(1): 012027. DOI: https://doi.org/10.1088/1755-1315/1182/1/012027
Hernández-Varela, J.D., Chanona-Pérez, J.J., Calderón Benavides, H.A., Cervantes Sodi, F. & Vicente-Flores, M. 2021. Effect of ball milling on cellulose nanoparticles structure obtained from garlic and agave waste. Carbohydrate Polymers, 255: 117347. DOI: https://doi.org/10.1016/j.carbpol.2020.117347
Holilah, H., Prasetyoko, D., Ediati, R., Bahruji, H., Jalil, A.A., Asranudin, A. & Anggraini, S.D. 2021. Hydrothermal assisted isolation of microcrystalline cellulose from pepper (Piper nigrum L.) processing waste for making sustainable bio-composite. Journal of Cleaner Production, 305: 127229. DOI: https://doi.org/10.1016/j.jclepro.2021.127229
Jatav, J. & Bhattacharya, B. 2024. Pineapple-peel waste to pineapple-peel based active food packaging film: Paving the way for a sustainable environment. Biomass Conversion and Biorefinery, 14(9): 10475-10485. DOI: https://doi.org/10.1007/s13399-022-03104-w
Karimi Alavijeh, M. & Zarei, A. 2025. Introducing an efficient protocol for micropropagation high quality 'MD2' pineapple; novel insights into iron form effects on in vitro plantlet quality. Biocatalysis and Agricultural Biotechnology, 68: 103720. DOI: https://doi.org/10.1016/j.bcab.2025.103720
Khaghani-Dehaghani, M., Ebrahimi-Kahrizsangi, R., Setoudeh, N. & Nasiri-Tabrizi, B. 2011. Al2O3–TiB2 nanocomposite powder from Al–TiO2–H3BO3 mixture. International Journal of Refractory Metals and Hard Materials, 29(2): 244-249. DOI: https://doi.org/10.1016/j.ijrmhm.2010.11.001
Khalid, M.Y., Arif, Z.U., Noroozi, R., Hossain, M., Ramakrishna, S. & Umer, R. 2023. 3D/4D printing of cellulose nanocrystals-based biomaterials: Additives for sustainable applications. International Journal of Biological Macromolecules, 251: 126287. DOI: https://doi.org/10.1016/j.ijbiomac.2023.126287
Khiari, B., Ghouma, L., Ferjani, A.I., Azzaz, A.A., Jellali, S., Limousy, L. & Jeguirim, M. 2020. Kenaf stems: Thermal characterization and conversion for biofuel and biochar production. Fuel, 262: 116654. DOI: https://doi.org/10.1016/j.fuel.2019.116654
Kristanto, J., Azis, M.M. & Purwono, S. 2021. Multi-distribution activation energy model on slow pyrolysis of cellulose and lignin in TGA/DSC. Heliyon, 7(7): e07669. DOI: https://doi.org/10.1016/j.heliyon.2021.e07669
Kumaresan, P., Purayil, J.N. & Preethi, K. 2025. Valorization of pineapple (Ananas comosus) peel waste for levan production: Assessment of biological activities. International Journal of Biological Macromolecules, 296: 139482. DOI: https://doi.org/10.1016/j.ijbiomac.2025.139482
Li, J., Wang, Z., Wang, P., Tian, J., Liu, T., Guo, J., Zhu, W., Khan, M.R., Xiao, H. & Song, J. 2024. On rheological properties of disc-shaped cellulose nanocrystals. Carbohydrate Polymers, 330: 121764. DOI: https://doi.org/10.1016/j.carbpol.2023.121764
Lv, T., Luo, Y., Chen, Y., Dai, D., Feng, X., Chen, H., Yu, Y., Ma, L., Zhang, Y. & Dai, H. 2022. Tuning the properties of pineapple peel cellulose nanofibrils by TEMPO-mediated oxidation and ball milling. Cellulose, 29(18): 9609-9625. DOI: https://doi.org/10.1007/s10570-022-04851-9
Macarez, A.-C., Maalej, H., Drobek, M., Pochat-Bohatier, C., Maalej, A., Chamkha, M. & Li, S. 2025. From olive stones waste to valuable resource: Exploring various techniques for cellulose extraction. Journal of Environmental Chemical Engineering, 13(5): 118204. DOI: https://doi.org/10.1016/j.jece.2025.118204
Madureira, A.R., Atatoprak, T., Cabuk, D., Sousa, F., Pullar, R.C. & Pintado, M. 2018. Extraction and characterisation of cellulose nanocrystals from pineapple peel. International Journal of Food Studies, 7(1): 24-33. DOI: https://doi.org/10.7455/ijfs/7.1.2018.a3
Mala, T., Piayura, S. & Itthivadhanapong, P. 2024. Characterization of dried pineapple (Ananas comosus L) peel powder and its application as a novel functional food ingredient in cracker product. Future Foods, 9: 100322. DOI: https://doi.org/10.1016/j.fufo.2024.100322
Mamudu, U., Kabyshev, A., Bekmyrza, K., Kuterbekov, K.A., Baratova, A., Omeiza, L.A. & Lim, R.C. 2025. Extraction, preparation and characterization of nanocrystalline cellulose from lignocellulosic Simpor leaf residue. Molecules, 30(7): 1622. DOI: https://doi.org/10.3390/molecules30071622
Mattonai, M., Pawcenis, D., del Seppia, S., Łojewska, J. & Ribechini, E. 2018. Effect of ball-milling on crystallinity index, degree of polymerization and thermal stability of cellulose. Bioresource Technology, 270: 270-277. DOI: https://doi.org/10.1016/j.biortech.2018.09.029
Naghdbishi, E. & Chackoshian Khorasani, A. 2025. A zero-waste approach to spent coffee grounds valorization: Cellulose production in series recycle flow reactors with its effluent upcycling into adsorbents for textile wastewater treatment. International Journal of Biological Macromolecules, 328(Part 1): 147444. DOI: https://doi.org/10.1016/j.ijbiomac.2025.147444
Oesef, K., Cranston, E.D. & Abdin, Y. 2024. Current advances in processing and modification of cellulose nanofibrils for high-performance composite applications. Materials & Design, 247: 113417. DOI: https://doi.org/10.1016/j.matdes.2024.113417
Ong, M.K., Cheng, C.R., Ong, C.A., Maqbool, M. & Zahid, N. 2025. Effects of polyhalite and doses application after anthesis on yield, quality and postharvest storage shelf life of MD2 pineapples (Ananas comosus). Journal of Food Quality, 2025(1): 1293311. DOI: https://doi.org/10.1155/jfq/1293311
Pereira, P.H.F., Ornaghi Jr, H.L., Arantes, V. & Cioffi, M.O.H. 2021. Effect of chemical treatment of pineapple crown fiber in the production, chemical composition, crystalline structure, thermal stability and thermal degradation kinetic properties of cellulosic materials. Carbohydrate Research, 499: 108227. DOI: https://doi.org/10.1016/j.carres.2020.108227
Putro, P.A., Sumardi, T., Sulaeman, A.S., Roza, L., Ramza, H. & Anugrah, D.S.B. 2023. Synthesizing cellulose and its derivatives from pineapple peel: A systematic literature review. Biointerface Research in Applied Chemistry, 13: 575. DOI: https://doi.org/10.33263/BRIAC136.575
Qasim, U., Ali, Z., Nazir, M.S., Ul Hassan, S., Rafiq, S., Jamil, F., Al-Muhtaseb, A.A.H., Ali, M., Khan Niazi, M.B., Ahmad, N.M., Ullah, S., Mukhtar, A. & Saqib, S. 2020. Isolation of cellulose from wheat straw using alkaline hydrogen peroxide and acidified sodium chlorite treatments: Comparison of yield and properties. Advances in Polymer Technology, 2020: 9765950. DOI: https://doi.org/10.1155/2020/9765950
Reddy, K.O., Maheswari, C.U., Dhlamini, M.S., Mothudi, B.M., Kommula, V.P., Zhang, J., Zhang, J. & Rajulu, A.V. 2018. Extraction and characterization of cellulose single fibers from native African Napier grass. Carbohydrate Polymers, 188: 85-91. DOI: https://doi.org/10.1016/j.carbpol.2018.01.110
Rezvani, P., Forouhar, A. & Saberian, H. 2025. Optimization of cellulose extraction from sugarcane bagasse and comparison of its quantity and quality with other cellulosic waste sources. Journal of Food Science and Technology (Iran), 22(166): 290-306.
Rico, X., Gullón, B., Alonso, J.L. & Yáñez, R. 2020. Recovery of high value-added compounds from pineapple, melon, watermelon and pumpkin processing by-products: An overview. Food Research International, 132: 109086. DOI: https://doi.org/10.1016/j.foodres.2020.109086
Sadeghi-Shapourabadi, M., Elkoun, S. & Robert, M. 2023. Microwave-assisted chemical purification and ultrasonication for extraction of nano-fibrillated cellulose from potato peel waste. Macromol, 3(4): 766-781. DOI: https://doi.org/10.3390/macromol3040044
Sarangi, P.K., Singh, T.A., Singh, N.J., Shadangi, K.P., Srivastava, R.K., Singh, A.K., Chandel, A.K., Pareek, N. & Vivekanand, V. 2022. Sustainable utilization of pineapple wastes for production of bioenergy, biochemicals and value-added products: A review. Bioresource Technology, 351: 127085. DOI: https://doi.org/10.1016/j.biortech.2022.127085
Sitorus, B., Syahbanu, I., Yoni, F., Antonius & Panjaitan, S.D. 2024. Isolated pineapple peel microcellulose as a matrix for polypyrrole-based capacitor. Cellulose Chemistry and Technology, 58(3-4): 223-231. DOI: https://doi.org/10.35812/CelluloseChemTechnol.2024.58.22
Soni, S., Noor, U. & Gupta, E. 2022. Ananas comosus peel waste, a novel substrate of therapeutic potential: Evidences and prospects. Indian Journal of Natural Products and Resources, 13(2): 129-143.
Sun, C., Hu, Y., Zhu, Z., He, Z., Mei, L., Wang, C., Xie, Q., Chen, X. & Du, X. 2024. Starch nanoparticles with predictable size prepared by alternate treatments of ball milling and ultrasonication. International Journal of Biological Macromolecules, 272: 132862. DOI: https://doi.org/10.1016/j.ijbiomac.2024.132862
Syguła, E., Piasecka, K., Łyczko, J. & Białowiec, A. 2025. The potential of decision tree application in threshold analysis of hazardous volatile organic compound release from biochar: Implications for environmental risk assessment. Science of the Total Environment, 998: 180252. DOI: https://doi.org/10.1016/j.scitotenv.2025.180252
Tarchoun, A.F., Trache, D. & Klapötke, T.M. 2019. Microcrystalline cellulose from Posidonia oceanica brown algae: Extraction and characterization. International Journal of Biological Macromolecules, 138: 837-845. DOI: https://doi.org/10.1016/j.ijbiomac.2019.07.176
Tejedor, M.B., Pazesh, S., Nordgren, N., Schuleit, M., Rutland, M.W., Alderborn, G. & Millqvist-Fureby, A. 2018. Milling induced amorphisation and recrystallization of $alpha$-lactose monohydrate. International Journal of Pharmaceutics, 537(1-2): 140-147. DOI: https://doi.org/10.1016/j.ijpharm.2017.12.021
Telidi, U.S.M. & Salim, N.S.M. 2023. Effect of ball milling time on structural properties and colour analysis of calamansi (Citrus microcarpa) peel powder. Transactions on Science and Technology, 10(3): 164-169.
Valášek, P., Müller, M., Šleger, V., Kolář, V., Hromasová, M., D'Amato, R. & Ruggiero, A. 2021. Influence of alkali treatment on the microstructure and mechanical properties of coir and abaca fibers. Materials, 14(10): 2636. DOI: https://doi.org/10.3390/ma14102636
Vishnoi, Y., Trivedi, A.K., Gupta, M.K., Singh, H., Rangappa, S.M. & Siengchin, S. 2024. Extraction of nano-crystalline cellulose for development of aerogel: Structural, morphological and antibacterial analysis. Heliyon, 10(1): e23846. DOI: https://doi.org/10.1016/j.heliyon.2023.e23846
Wang, Y., Yu, Y., Hu, S., Yu, J., Huang, Y. & Dai, H. 2025. Preparation of agrowaste-based nanocellulose by NaOH-assisted ball milling technique: Influence of component intervention. Gels, 11(8): 631. DOI: https://doi.org/10.3390/gels11080631
Yang, C., Yuan, X., Wang, X., Wu, K., Liu, Y., Liu, C., Lu, H. & Liang, B. 2020. Ball milling promoted direct liquefaction of lignocellulosic biomass in supercritical ethanol. Frontiers of Chemical Science and Engineering, 14(4): 605-613. DOI: https://doi.org/10.1007/s11705-019-1841-0
Zhang, S., Feng, X., Huang, Y., Wang, Y., Chen, H., Yu, Y., Ma, L., Zhang, Y. & Dai, H. 2022. Facile isolation of cellulose nanofibrils from agro-processing residues and its improved stabilization effect on gelatin emulsion. International Journal of Biological Macromolecules, 216: 272-281. DOI: https://doi.org/10.1016/j.ijbiomac.2022.07.005
Zhao, J., Jin, X., Yan, M., Huang, C., Yong, Q. & Ling, Z. 2024. Supramolecular regulation and controllable coproduction of bamboo nanocellulose and mono/oligosaccharides via dual-enzymatic treatment assisted by ball milling. ACS Sustainable Chemistry & Engineering, 12(41): 15216-15227. DOI: https://doi.org/10.1021/acssuschemeng.4c06144
Zheng, Y., Fu, Z., Li, D. & Wu, M. 2018. Effects of ball milling processes on the microstructure and rheological properties of microcrystalline cellulose as a sustainable polymer additive. Materials, 11(7): 1057. DOI: https://doi.org/10.3390/ma11071057
Published
How to Cite
Issue
Section
Any reproduction of figures, tables and illustrations must obtain written permission from the Chief Editor (wicki@ukm.edu.my). No part of the journal may be reproduced without the editor’s permission
