Cassava Starch-Based Biocomposites Reinforced with Zinc Oxide and Spent Coffee Ground Cellulose: A Comparative Study and TOPSIS Evaluation

  • Nyoman Puspa Asri Food Technology Program, Faculty of Tourism, Ciputra University Surabaya, Surabaya, Indonesia
  • Hans Rachman Food Technology Program, Faculty of Tourism, Ciputra University Surabaya, Surabaya, Indonesia
  • Jaclyn Regina Anggara Food Technology Program, Faculty of Tourism, Ciputra University Surabaya, Surabaya, Indonesia
  • Raymond Hamidy Food Technology Program, Faculty of Tourism, Ciputra University Surabaya, Surabaya, Indonesia
  • Jessica Renata Yoewono Food Technology Program, Faculty of Tourism, Ciputra University Surabaya, Surabaya, Indonesia
  • Yohannes Somawiharja Food Technology Program, Faculty of Tourism, Ciputra University Surabaya, Surabaya, Indonesia
Keywords: Bioplastic, Cellulose, Spent Coffee Ground, TOPSIS, ZnO

Abstract

The accumulation of synthetic plastic waste and depletion of fossil resources have driven the search for sustainable alternatives, such as biodegradable bioplastics. This study explores the use of cellulose derived from spent coffee grounds (SCG) and zinc oxide (ZnO) as reinforcing fillers in cassava starch-based bioplastics fabricated via solution-casting methods.  Various formulations were developed using SCG cellulose (1%, 1.5%, and 2% with 10%, 15%, and 20% glycerol) or ZnO (1%, 1.5%, and 2% with 10% and 15% glycerol) The resulting films were evaluated for their mechanical, barrier, and optical properties, followed by structural analysis using Fourier Transform Infrared Spectroscopy (FTIR), X-ray Diffraction (XRD), and Scanning Electron Microscopy (SEM). Results showed that SCG-based cellulose significantly improved tensile strength (up to 1.87 MPa) but reduced transparency (to 46.38%), while ZnO-enhanced films exhibited higher light transmittance (up to 70.28%). FTIR confirmed hydrogen bonding interactions between the filler and the starch matrix, and XRD revealed differences in crystallinity, with cellulose showing semi-amorphous characteristics and ZnO contributing to higher peak intensity. SEM analysis supported these findings, indicating a more compact and continuous matrix in ZnO films. A multi-criteria decision-making analysis using the TOPSIS method identified the optimal cellulose-based formulation as 2% SCG cellulose with 20% glycerol, which achieved a tensile strength of 1.87 MPa, transparency of 46.40, and a water vapor permeability (WVP) of 2.318 × 10-6 g/m·day·Pa. These findings demonstrate the potential of SCG and ZnO as functional additives in biodegradable packaging materials and support the circular economy by valorizing organic waste.

References

Abdel Hamid, E.M., Mohamed, A.E., Mohamed, A.A., Galal, A.A., Mekhemr, A.A., Saleh, E.S., Hassan, M.I., Ahmed, M.H., Elgendy, S.K., 2025. "Optimization of corn starch/glycerol, acetic acid, and cellulose fibers ratio on biodegradable plastic synthesis by Box–Behnken design (BBD)." Clean Technol. Environ. Policy, 27, 4433-4455. https://doi.org/10.1007/s10098-025-03135-7

Abdullah, A.H., Putri, O.D., Fikriyyah, A., Nissa, R., Hidayat, S., Septiyanto, R., Karina, M., Satoto, R., 2020. "Harnessing the excellent mechanical, barrier and antimicrobial properties of zinc oxide (ZnO) to improve the performance of starch-based bioplastic." Polym. Technol. Mater., 59, 1259–1267. https://doi.org/10.1080/25740881.2020.1738466

Abe, M.M., Martins, J.R., Sanvezzo, P.B., Macedo, J. V, Branciforti, M.C., Halley, P., Botaro, V.R., Brienzo, M., 2021. "Advantages and disadvantages of bioplastics production from starch and lignocellulosic components." Polymers, 13(15), 2484. https://doi.org/10.3390/polym13152484

Agustin, S., Cahyanto, M.N., Wahyuni, E.T., Supriyadi, 2024. "Effect of glycerol plasticizer on the structure and characteristics of bacterial cellulose-based biocomposite films." IOP Conf. Ser. Earth Environ. Sci., 1377. https://doi.org/10.1088/1755-1315/1377/1/012046

Akshaykranth, A., Ajayan, J., Anitha, N., 2025. "Development of biodegradable PLA/Nanoclay/ZnO polymer films for future Industrial packaging applications." Results Surf. Interfaces, 19, 100518. https://doi.org/https://doi.org/10.1016/j.rsurfi.2025.100518

Ali, S., Mehra, V., Eltaggaz, A., Deiab, I., Pervaiz, S., 2024. "Optimization and prediction of additively manufactured PLA-PHA biodegradable polymer blend using TOPSIS and GA-ANN." Manuf. Lett., 41, 795–802. https://doi.org/https://doi.org/10.1016/j.mfglet.2024.09.099

Ali, S.S., Elsamahy, T., Abdelkarim, E.A., Abdelfattah, A., Ramadan, H., Mostafa, S., Metwally, S.M., Sun, J., 2023. 12 - Engineered yeast for the production of bioplastics, in: Daverey, A., Dutta, K., Joshi, S., Gea, T.B.T.-A. in Y.B. for B. and S. (Eds.), Elsevier, pp. 277–296. https://doi.org/https://doi.org/10.1016/B978-0-323-95449-5.00017-5

Anugrahwidya, R., Armynah, B., Tahir, D., 2022. "Composites bioplastic film for various concentration of zinc oxide (ZnO) nanocrystals towards physical properties for high biodegradability in soil and seawater." J. Polym. Environ., 30, 2589–2601. https://doi.org/10.1007/s10924-021-02363-4

Arifin, H.R., Djali, M., Nurhadi, B., Azlin-Hasim, S., Masruchin, N., Vania, P.A., Hilmi, A., 2022. "Corn starch-based bionanocomposite film reinforced with ZnO nanoparticles and different types of plasticizers." Front. Sustain. Food Syst., 6, 886219. https://doi.org/10.3389/fsufs.2022.886219

Armynah, B., Anugrahwidya, R., Tahir, D., 2022. "Composite cassava starch/chitosan/Pineapple Leaf Fiber (PALF)/Zinc Oxide (ZnO): Bioplastics with high mechanical properties and faster degradation in soil and seawater." Int. J. Biol. Macromol., 213, 814–823. https://doi.org/https://doi.org/10.1016/j.ijbiomac.2022.06.038

Asri, N., Yuniati, Y., Hindarso, H., Suprapto, S., Yogaswara, R., 2020. "Biodiesel production from Kesambi (Schleichera oleosa) oil using multi-walled carbon nanotubes supported zinc oxide as a solid acid catalyst." IOP Conf. Ser. Earth Environ. Sci., 456, 12003. https://doi.org/10.1088/1755-1315/456/1/012003

Atiwesh, G., Mikhael, A., Parrish, C.C., Banoub, J., Le, T.-A.T., 2021. "Environmental impact of bioplastic use: A review." Heliyon, 7(9), e07918. https://doi.org/https://doi.org/10.1016/j.heliyon.2021.e07918

Azlim, N.A., Mohammadi Nafchi, A., Oladzadabbasabadi, N., Ariffin, F., Ghalambor, P., Jafarzadeh, S., Al-Hassan, A.A., 2022. "Fabrication and characterization of a pH-sensitive intelligent film incorporating dragon fruit skin extract." Food Sci. Nutr., 10, 597–608. https://doi.org/10.1002/fsn3.2680

Ballesteros-Mártinez, L., Pérez-Cervera, C., Andrade-Pizarro, R., 2020. "Effect of glycerol and sorbitol concentrations on mechanical, optical, and barrier properties of sweet potato starch film." Nutr. Food Sci. J., 20, 1–9. https://doi.org/https://doi.org/10.1016/j.nfs.2020.06.002

Baltscheit, J., Schmidt, N., Schröder, F., Meyer, J., 2020. "Investigations on the aging behavior of transparent bioplastics for optical applications." InfoMat, 2, 424–433. https://doi.org/https://doi.org/10.1002/inf2.12065

Benitez, J.J., Florido-Moreno, P., Porras-Vázquez, J.M., Tedeschi, G., Athanassiou, A., Heredia-Guerrero, J.A., Guzman-Puyol, S., 2024. "Transparent, plasticized cellulose-glycerol bioplastics for food packaging applications." Int. J. Biol. Macromol., 273, 132956. https://doi.org/https://doi.org/10.1016/j.ijbiomac.2024.132956

Cabernard, L., Pfister, S., Oberschelp, C., Hellweg, S., 2022. Growing environmental footprint of plastics driven by coal combustion. Nat. Sustain., 5, 139–148. https://doi.org/10.1038/s41893-021-00807-2

Dadashi, P., Torbatinejad, K., Babaei, A., 2025. "Hybridization as a promising approach to engineering the desired performance of bio-nanocomposites: GO-ZnO hybrid reinforced PCL." Sci. Rep., 15, 17259. https://doi.org/10.1038/s41598-025-02087-8

Debeaufort, F., Martin-Polo, M., Voilley, A., 1993. "Polarity homogeneity and structure affect water vapor permeability of model edible films." J. Food Sci., 58, 426–429. https://doi.org/https://doi.org/10.1111/j.1365-2621.1993.tb04290.x

Devika, R., Saha, R., 2024. "Characterization and optimization studies of cellulose-based bioplastics extracted from Musa paradisiaca L." Glob. Nest J., 26 (2), 1-10. https://doi.org/10.30955/gnj.005613

Dibha, A., MASRURI, M., Srihardyastutie, A., 2023. "Degradable bioplastic developed from pine-wood nanocellulose as a filler combined with orange peel extract." Indones. J. Chem., 23(1), 127–139. https://doi.org/10.22146/ijc.75520

Folino, A., Pangallo, D., Calabrò, P.S., 2023. "Assessing bioplastics biodegradability by standard and research methods: Current trends and open issues." J. Environ. Chem. Eng., 11, 109424. https://doi.org/https://doi.org/10.1016/j.jece.2023.109424

Fransiska, D., Abdullah, A.H.D., Nurhayati, Irianto, H.E., Nissa, R.C., Sedayu, B.B., Syamani, F.A., Raharjo, S., Suwarti, Agusman, 2024. "Impact of agar–glycerol ratios on the physicochemical properties of biodegradable seaweed films: A compositional study." Int. J. Biol. Macromol., 280, 135855. https://doi.org/https://doi.org/10.1016/j.ijbiomac.2024.135855

Gea, S., Meldawati Pasaribu, K., Sarumaha, A., Rahayu, S.R.I., 2022. "Cassava starch/bacterial cellulose-based bioplastics with Zanthoxylum acanthopodium." Biodiversitas J. Biol. Divers., 23 (5), 2601-2608. https://doi.org/10.13057/biodiv/d230542

Gonçalves, S.M., dos Santos, D.C., Motta, J.F.G., Santos, R.R. dos, Chávez, D.W.H., Melo, N.R. de, 2019. Structure and functional properties of cellulose acetate films incorporated with glycerol. Carbohydr. Polym., 209, 190–197. https://doi.org/https://doi.org/10.1016/j.carbpol.2019.01.031

Guivier, M., Chevigny, C., Domenek, S., Casalinho, J., Perré, P., Almeida, G., 2024. "Water vapor transport properties of bio-based multilayer materials determined by original and complementary methods." Sci. Rep., 14, 50. https://doi.org/10.1038/s41598-023-50298-8

Guzman-Puyol, S., Benítez, J.J., Heredia-Guerrero, J.A., 2022. "Transparency of polymeric food packaging materials." Food Res. Int., 161, 111792. https://doi.org/https://doi.org/10.1016/j.foodres.2022.111792

Hamidy, R., Rachman, H., Anggara, J., Sulistyo, J., Asri, N., 2025. "Extraction and Characterization of cellulose from arabica spent coffee grounds." J. IPTEK, 29, 95–104. https://doi.org/10.31284/j.iptek.2025.v29i1.7815

Hasna, T., Lestari, C., Putri, W., Fathuroya, V., 2022. "The effect of ZnO (zinc oxide) and glycerol concentrations on the mechanical properties of bioplastics made from Canna tuber (Canna edulis) starch." Adv. Food Sci. Sustain. Agric. Agroindustrial Eng., 5, 21–28. https://doi.org/10.21776/ub.afssaae.2022.005.01.2

Hernandez, C., Rosa, D., 2016. Extraction of cellulose nanowhiskers: natural fibers source, methodology and application. Polymer Science: Research Advances, Practical Applications And Educational Aspects. Formatex Research Center, Brazil. pp. 232–242.

Janas, S., Kowalska, M., 2023. "Accuracy of drying selected products using a moisture analyzer method based on infrared radiation." Metrol. Meas. Syst., 30 (2), 305–321. https://doi.org/10.24425/mms.2023.144873

Jannah, M., Ahmad, A., Hayatun, A., Taba, P., Chadijah, S., 2019. "Effect of filler and plastisizer on the mechanical properties of bioplastic cellulose from rice husk." J. Phys. Conf. Ser., 1341, 32019. https://doi.org/10.1088/1742-6596/1341/3/032019

Karaca, A.E., Özel, C., Özarslan, A.C., Yücel, S., 2022. "The simultaneous extraction of cellulose fiber and crystal biogenic silica from the same rice husk and evaluation in cellulose-based composite bioplastic films." Polym. Compos., 43, 6838–6853. https://doi.org/https://doi.org/10.1002/pc.26729

Karmee, S.K., 2018. "A spent coffee grounds based biorefinery for the production of biofuels, biopolymers, antioxidants and biocomposites." Waste Manag., 72, 240–254. https://doi.org/https://doi.org/10.1016/j.wasman.2017.10.042

Khouaja, A., Koubaa, A., Ben Daly, H., 2025. "Mechanical and morphological properties of cellulose biocomposites." Chemosphere, 379, 144415. https://doi.org/https://doi.org/10.1016/j.chemosphere.2025.144415

Klink, M.J., Laloo, N., Leudjo Taka, A., Pakade, V.E., Monapathi, M.E., Modise, J.S., 2022. "Synthesis, characterization and antimicrobial activity of zinc oxide nanoparticles against selected waterborne bacterial and yeast pathogens." Molecules, 27(11), 3532. https://doi.org/10.3390/molecules27113532

Krishnamurthy, A., Amritkumar, P., 2019. "Synthesis and characterization of eco-friendly bioplastic from low-cost plant resources." SN Appl. Sci., 1, 1432. https://doi.org/10.1007/s42452-019-1460-x

Lee, S.W., Said, N.S., Sarbon, N.M., 2021. "The effects of zinc oxide nanoparticles on the physical, mechanical and antimicrobial properties of chicken skin gelatin/tapioca starch composite films in food packaging." J. Food Sci. Technol., 58, 4294–4302. https://doi.org/10.1007/s13197-020-04904-6

Liu, Y.-R., Tang, X., Zeng, Q., Lai, J.-P., 2024. "Impacts of ultraviolet absorption by zinc oxide nanoparticle modifiers on asphalt aging." Sci. Rep., 14, 19918. https://doi.org/10.1038/s41598-024-70875-9

Long, J., Zhang, W., Zhao, M., Ruan, C.-Q., 2023. "The reduce of water vapor permeability of polysaccharide-based films in food packaging: A comprehensive review." Carbohydr. Polym., 321, 121267. https://doi.org/https://doi.org/10.1016/j.carbpol.2023.121267

Lounis, F.M., Benhacine, F., Hadj-Hamou, A.S., 2024. "Improving water barrier properties of starch based bioplastics by lignocellulosic biomass addition: Synthesis, characterization and antibacterial properties." Int. J. Biol. Macromol., 283, 137823. https://doi.org/https://doi.org/10.1016/j.ijbiomac.2024.137823

Mohammad Azmin, S.N.H., Aliah, N., Mat Nor, M.S., 2020. Development and "Characterization of food packaging bioplastic film from cocoa pod husk cellulose incorporated with sugarcane bagasse fibre." J. Bioresour. Bioprod., 5, 259–266. https://doi.org/10.1016/j.jobab.2020.10.003

Nasution, H., Elisa, J., Dalimunthe, N., Asdita, M., Zoelva, A., Sartika, M., 2023. "The role of stirring speed on the properties improvement of bioplastic composite sagu starch modified with cellulose microcrystal and betel leaf extract." RASAYAN J. Chem., 16, 1912–1919. https://doi.org/10.31788/RJC.2023.1638261

Nayanathara Thathsarani Pilapitiya, P.G.C., Ratnayake, A.S., 2024. "The world of plastic waste: A review." Clean. Mater., 11, 100220. https://doi.org/https://doi.org/10.1016/j.clema.2024.100220

Ngo, T.M.P., Dang, T.M.Q., Tran, T.X., Rachtanapun, P., 2018. "Effects of zinc oxide nanoparticles on the properties of pectin/alginate edible films." Int. J. Polym. Sci., 2018, 5645797. https://doi.org/https://doi.org/10.1155/2018/5645797

Nigam, S., Das, A.K., Patidar, M.K., 2021. "Synthesis, characterization and biodegradation of bioplastic films produced from Parthenium hysterophorus by incorporating a plasticizer (PEG600)." Environ. Challenges, 5, 100280. https://doi.org/https://doi.org/10.1016/j.envc.2021.100280

Nurhayati, I., Kurniawati, C.T., Kholif, M. Al, 2025. "Sustainable bioplastics from sweet corn cob waste: Influence of zinc oxide and glycerol on mechanical properties and biodegradability." Indones. J. Environ. Manag. Sustain., 9, 1–11. https://doi.org/10.26554/ijems.2025.9.1.1-11

Oluwasina, Olugbenga, Aderibigbe, A., Ikupoluyi, S., Oluwasina, Olayinka, Ewetumo, T., 2024. "Physico-electrical properties of starch-based bioplastic enhanced with acid-treated cellulose and graphene oxide fillers." Sustain. Chem. Environ., 6, 100093. https://doi.org/https://doi.org/10.1016/j.scenv.2024.100093

Popescu, M.-C., Dogaru, B.-I., Popescu, C.-M., 2020. "Effect of cellulose nanocrystals nanofiller on the structure and sorption properties of carboxymethyl cellulose–glycerol–cellulose nanocrystals nanocomposite systems." Materials, 13(13), 2900. https://doi.org/10.3390/ma13132900

Putranti, L., Nugraheni, P., 2023. "Effect of carboxymethyl cellulose addition on the characteristic of chitosan-based bioplastic." IOP Conf. Ser. Earth Environ. Sci., 1289, 12038. https://doi.org/10.1088/1755-1315/1289/1/012038

Rahmatullah, R., Putri, R., Rendana, M., Waluyo, U., Andrianto, T., 2022. Effect of plasticizer and concentration on characteristics of bioplastic based on cellulose acetate from kapok (Ceiba pentandra)." Fiber. Sci. Technol. Indones., 7, 73–83. https://doi.org/10.26554/sti.2022.7.1.73-83

Ranote, S., Kowalczuk, M., Guzenko, N., Duale, K., Chaber, P., Musioł, M., Jankowski, A., Marcinkowski, A., Kurcok, P., Chauhan, G.S., Chauhan, S., Kumar, K., 2024. "Towards scalable and degradable bioplastic films from Moringa oleifera gum/poly(vinyl alcohol) as packaging material." Int. J. Biol. Macromol., 269, 132219. https://doi.org/https://doi.org/10.1016/j.ijbiomac.2024.132219

Safitri, A., Sinaga, P.S.D., Nasution, H., Harahap, H., Masyithah, Z., Iriany, Hasibuan, R., 2022. "The role of various plastisizers and fillers additions in improving tensile strength of starch-based bioplastics: A mini review." IOP Conf. Ser. Earth Environ. Sci., 1115, 12076. https://doi.org/10.1088/1755-1315/1115/1/012076

Sanyang, M.L., Sapuan, S.M., Jawaid, M., Ishak, M.R., Sahari, J., 2016. "Effect of plasticizer type and concentration on physical properties of biodegradable films based on sugar palm (Arenga pinnata) starch for food packaging." J. Food Sci. Technol., 53, 326–336. https://doi.org/10.1007/s13197-015-2009-7

Sapei, L., Padmawijaya, K., Sijayanti, O., "Wardhana, P., 2017. Study of the influence of ZnO addition on the properties of chitosan-banana starch bioplastics." IOP Conf. Ser. Mater. Sci. Eng., 223, 12044. https://doi.org/10.1088/1757-899X/223/1/012044

Singh, T., Pal, N., Sharma, P., Passari, A., 2023. "Spent coffee ground: transformation from environmental burden into valuable bioactive metabolites. Rev. Environ." Sci. Bio/Technology, 22, 887–898. https://doi.org/10.1007/s11157-023-09669-w

Steven, S., Fauza, A.N., Mardiyati, Y., Santosa, S.P., Shoimah, S.M., 2022. Facile preparation of cellulose bioplastic from Cladophora sp. algae via hydrogel method. Polymers, 14(21), 4699 . https://doi.org/10.3390/polym14214699

Tagudin, N.M.F.B.A., Ibrahim, N.B., 2025. "Synthesis of polylactic acid from apple, pineapple, and potato residues." ASEAN J. Chem. Eng., 25(1), 75-86.. https://doi.org/10.22146/ajche.16580

Tamimi, N., Mohammadi Nafchi, A., Hashemi-Moghaddam, H., Baghaie, H., 2021. "The effects of nano-zinc oxide morphology on functional and antibacterial properties of tapioca starch bionanocomposite." Food Sci. Nutr., 9, 4497–4508. https://doi.org/10.1002/fsn3.2426

Tarique, J., Sapuan, S.M., Khalina, A., 2021. "Effect of glycerol plasticizer loading on the physical, mechanical, thermal, and barrier properties of arrowroot (Maranta arundinacea) starch biopolymers." Sci. Rep., 11, 13900.

https://doi.org/10.1038/s41598-021-93094-y

Viana Freitas, V., Borges, L., Vidigal, M., Santos, M., Stringheta, P., 2024. "Coffee: A comprehensive overview of origin, market, and the quality process." Trends Food Sci. Technol., 146, 104411. https://doi.org/10.1016/j.tifs.2024.104411

Vyas, A., Ng, S., Fu, T., Anum, I., 2025. ZnO-Embedded carboxymethyl cellulose bioplastic film synthesized from sugarcane bagasse for packaging applications." Polymers, 17(5), 579. https://doi.org/10.3390/polym17050579

Werapun, U., Werapun, W., Phatthiya, A., 2024. "Characterization of composite bioplastic from Cassava starch with titanium dioxide and zinc oxide." Dig. J. Nanomater. Biostructures, 19, 275–282. https://doi.org/10.15251/DJNB.2024.191.275

Xie, D., Zhang, R., Zhang, C., Yang, S., Xu, Z., Song, Y., 2023. "A novel, robust mechanical strength, and naturally degradable double crosslinking starch-based bioplastics for practical applications." Int. J. Biol. Macromol., 253, 126959. https://doi.org/https://doi.org/10.1016/j.ijbiomac.2023.126959

Yahia, R., Owda, M.E., Abou-Zeid, R.E., Abdelhai, F., El-Gamil, H.Y., Abdo, A.M., Ali, A.A., 2024. "Biodegradable, UV absorber and thermal stable bioplastic films from waxy corn starch/polyvinyl alcohol blends." Biomass Convers. Biorefinery, 14, 27989–28006. https://doi.org/10.1007/s13399-022-03683-8

Zhou, S.-J., Xiong, S.-J., Wang, H.-M., Yu, S., Yuan, T.-Q., 2025. "Direct utilization of cassava flour in biodegradable films: The compatibilizing effect of cassava protein on poly (butylene adipate-co-terephthalate) and cassava starch." Int. J. Biol. Macromol., 319, 145532. https://doi.org/https://doi.org/10.1016/j.ijbiomac.2025.145532

Published
2026-04-30
How to Cite
Puspa Asri, N., Rachman, H., Anggara , J. R., Hamidy, R., Yoewono, J. R., & Somawiharja, Y. (2026). Cassava Starch-Based Biocomposites Reinforced with Zinc Oxide and Spent Coffee Ground Cellulose: A Comparative Study and TOPSIS Evaluation. SEAN ournal of hemical ngineering, 26(1), 145-165. https://doi.org/10.22146/ajche.23638
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