Synthesis of Cellulose/Chitosan/Alginate-Magnetite Composite Hydrogel as Adsorbent and A Heterogeneous Catalyst for The Fenton Reaction in The Removal Congo Red
DOI:
https://doi.org/10.25077/jrk.v17i2.924Keywords:
congo red, hydrogel composite, isotherm adsorption, Fenton ReactionAbstract
Congo Red (CR) is a synthetic dye widely used in the textile, paper, and plastic industries. Chemically, this dye contains azo (–N=N) and aromatic groups, which are toxic and persistent in the environment, making it resistant to biological degradation. Therefore, this study aims to synthesize a cellulose-based hydrogel composite derived from sawdust (Ce)-chitosan (Ch)-alginate (A) modified with magnetite (M) (Ce-Ch-A-M), which is synthesized through cross-linking and used to remove CR, with SA and KA composites serving as comparisons. The obtained composites were characterized using Attenuated Total Reflectance-Infra-Red (ATR-IR) to identify functional groups, Scanning Electron Microscopy-Energy Dispersive X-Ray (SEM-EDX) Mapping to analyze surface morphology and elemental distribution, X-Ray Diffraction (XRD) to analyze crystallinity, and Surface Area Analyzer (SAA) to analyze specific surface area and pore size. The results indicate that the Ce-Ch-A-M hydrogel composite exhibits better performance in removing CR. The adsorption process for Ce-A and Ch-A composites followed the Langmuir isotherm model with R² values of 0.9563 and 0.9826, respectively, while Ce-Ch-A-M adhered to the Freundlich isotherm model, indicating multilayer adsorption on a heterogeneous surface with an R² value of 0.9170. In the Fenton catalytic test, Fe as a catalyst demonstrated good performance in catalyzing H2O2 to remove up to 38% of CR. Overall, this study demonstrates that the Ce-Ch-A-M composite possesses good capability in removing anionic dyes, suggesting its potential for application in the treatment of other dyes.
References
1. Adeleke, A. O., Omar, R. C., Katibi, K. K., Dele-Afolabi, T. T., Ahmad, A., Quazim, J. O., Amusa, A. A., et al., Process optimization of superior biosorption capacity of biogenic oyster shells nanoparticles for Congo red and Bromothymol blue dyes removal from aqueous solution: Response surface methodology, equilibrium isotherm, kinetic, and reusability studies. Alexandria Eng. J., 92: 11–23 (2024).
2. Sudarshan, S., Harikrishnan, S., RathiBhuvaneswari, G., Alamelu, V., Aanand, S., Rajasekar, A. & Govarthanan, M., Impact of textile dyes on human health and bioremediation of textile industry effluent using microorganisms: current status and future prospects. J. Appl. Microbiol., 134(2): (2023).
3. Oladoye, P. O., Bamigboye, M. O., Ogunbiyi, O. D. & Akano, M. T., Toxicity and decontamination strategies of Congo red dye. Groundw. Sustain. Dev., 19: (2022).
4. Rasilingwani, T. E., Gumbo, J. R., Masindi, V. & Foteinis, S., Removal of Congo red dye from industrial effluents using metal oxide-clay nanocomposites: Insight into adsorption and precipitation mechanisms. Water Resour. Ind., 31: (2024).
5. Du, Y., Wang, Z., Fu, Y., Wang, R., An, J., Gao, Y., Gao, X., et al., A novel titanium dioxide/chitosan composite aerogel for efficient removal of Congo red: Experimental and DFT studies. Int. J. Biol. Macromol., 332: (2025).
6. Muhammad, H., Tuzen, M., Siddiqui, A. & Umar, A. R., Effective adsorption of Congo red azo dye from different water and wastewater by using porous Fe3O4-bentonite@chitosan nanocomposite: A multivariate optimization. Int. J. Biol. Macromol., 310: (2025).
7. Kausar, A., Ijaz, S., Rafaqat, M., Dahshan, A., Latif, A. A., Bibi, S., Al-Kadhi, N. S., et al., Chitosan-cellulose composite for the adsorptive removal of anionic dyes: Experimental and theoretically approach. J. Mol. Liq., 391: (2023).
8. Li, M., Qu, H., Li, Q., Lu, S., Wu, Y., Tang, Z., Liu, X., et al., A carboxymethyl cellulose/chitosan-based hydrogel harvests robust adhesive, on-demand detachment and self-healing performances for deep burn healing. Chem. Eng. J., 498: (2024).
9. Long, J., Gao, Y., Sheng, K., Yao, J., Yu, Q., Deng, Z., Zhang, X., et al., Bio-derived cellulose adsorbent from licorice residues for high-efficiency and recyclable removal of phenothiazines. Int. J. Biol. Macromol., 154146 (2026). doi:10.1016/j.ijbiomac.2026.154146
10. Aslam, A. A., Hassan, S. U., Saeed, M. H., Kokab, O., Ali, Z., Nazir, M. S., Siddiqi, W., et al., Cellulose-based adsorbent materials for water remediation: Harnessing their potential in heavy metals and dyes removal. J. Clean. Prod., 421: (2023).
11. Singh, S., Kumar, S., Hsan, N., Devnani, G. L., Rahman, M. M. & Koh, J., A sustainable chitosan-modified carboxymethyl cellulose hybrid adsorbent: Dual application in carbon dioxide capture and acid dye removal. J. Ind. Eng. Chem., 162: 528–541 (2026).
12. Wen, Z., Gao, D., Niu, H., Lin, J., Li, Z., Zeng, J., Ke, F., et al., Three-dimensional porous adsorbent based on chitosan-alginate-cellulose sponge for selective and efficient removal of anionic dyes. J. Environ. Chem. Eng., 11(5): (2023).
13. Sabzevari, S., Farrokhzad, H. & Poorkhalil, A., Synthesis and characterization of a hydrogel film based on chitosan/carboxymethyl cellulose for food packaging applications. Carbohydr. Polym. Technol. Appl., 11: (2025).
14. Kurczewska, J. & Cegłowski, M., Tetracycline adsorbents based on alginate and chitosan - A promising approach to mitigate antibiotic resistance. J. Water Process Eng., 77: (2025).
15. Chen, J., Wang, X., Huang, X., Tong, Z., Zhou, J., Shen, Y. & Hao, C., Construction of cellulose-based hydrogel compounded with modified kaolin and its removal performance for heavy metal ions and dyes in water. Int. J. Biol. Macromol., 306: (2025).
16. Phouthavong, V., Yan, R., Nijpanich, S., Hagio, T., Ichino, R., Kong, L. & Li, L., Magnetic Adsorbents for Wastewater Treatment: Advancements in Their Synthesis Methods. Materials (Basel)., 15(3): (2022).
17. Slama, N. E. H., Masmoudi, G., Fizer, M., Mariychuk, R. & Dhaouadi, H., Comprehensive study of Fenton reaction efficiency on textile wastewater treatment from dye solution to real effluent with emphasis on Fukui function analysis. J. Mol. Liq., 402: (2024).
18. Zhou, Y., Jin, K., Pei, L., Zhang, X., Zhang, H., Yang, Q., Liang, S., et al., The study of reactive dyes degradation in a current cycle reversal system combining cathodic electro-Fenton and anodic oxidation. J. Environ. Chem. Eng., 13(3): (2025).
19. Abdul Rahman, A. S., Fizal, A. N. S., Khalil, N. A., Ahmad Yahaya, A. N., Hossain, M. S. & Zulkifli, M., Fabrication and Characterization of Magnetic Cellulose–Chitosan–Alginate Composite Hydrogel Bead Bio-Sorbent. Polymers (Basel)., 15(11): (2023).
20. Sofyan, M. I., Mawarni, R. S., Sirumapea, L., Pramono, E., Marlina, A. & Ndruru, S. T. C. L., Simple Isolation and Characterization of Cellulose of Wastepaper. AIP Conf. Proc., 2902(1): (2023).
21. Cui, C., Qiao, W., Li, D. & Wang, L. jun., Dual cross-linked magnetic gelatin/carboxymethyl cellulose cryogels for enhanced Congo red adsorption: Experimental studies and machine learning modelling. J. Colloid Interface Sci., 678: 619–635 (2025).
22. Ibrahim, N. I., Sultan, M. T. H., Łukaszewicz, A., Shah, A. U. M., Shahar, F. S., Józwik, J., Najeeb, M. I., et al., Characterization and isolation method of Gigantochloa scortechinii (Buluh Semantan) cellulose nanocrystals. Int. J. Biol. Macromol., 272: (2024).
23. Antunes, B. da F., Santana, L. R., Oliveira, R. M., Valério Filho, A., Carreno, N. L. V., Wolke, S. I., da Silva, R., et al., Cellulose, cellulose nanofibers, and cellulose acetate from Butia fruits (Butia odorata): Chemical, morphological, structural, and thermal properties. Int. J. Biol. Macromol., 281: (2024).
24. Ding, L., Han, X., Chen, L. & Jiang, S., Preparation and properties of hydrophobic and transparent wood. J. Bioresour. Bioprod., 7(4): 295–305 (2022).
25. Raza, M., Mustafa, J., Al-Marzouqi, A. H. & Abu-Jdayil, B., Isolation and characterization of cellulose from date palm waste using rejected brine solution. Int. J. Thermofluids, 21: (2024).
26. Sunesh, N. P., Suyambulingam, I., Divakaran, D., Senthamaraikannan, P., Priya, S. & Han, S. S., Isolation and characterization of cellulose particles from groundnut (Arachis hypogaea) shell waste for sustainable reinforcement applications. Int. J. Biol. Macromol., 327: (2025).
27. Pradyasti, A., Lee, M. J., Kim, H. J. & Kim, M. H., Carboxymethyl cellulose/alginate/chitosan-based polyelectrolyte complex hydrogel with irregularly shaped multi-metallic nanowires for efficient continuous-flow Cr(VI) remediation. Int. J. Biol. Macromol., 309: (2025).
28. Hardiningtyas, S. D., Glenn, C. & Setyaningsih, I., Alginate–cellulose nanofiber hydrogel for stable microalgae immobilization for phycoremediation of aquaculture wastewater. J. Water Process Eng., 79: (2025).
29. Hingrajiya, R. D. & Patel, M. P., Fe3O4 modified chitosan based co-polymeric magnetic composite hydrogel: Synthesis, characterization and evaluation for the removal of methylene blue from aqueous solutions. Int. J. Biol. Macromol., 244: (2023).
30. Xu, G., Zhang, H., Xu, F., Sun, L., Lin, X., Ma, L., Peng, H., et al., Poly-dopamine coated-cellulose/chitosan hybrid carbon aerogel composite phase change materials with efficient photothermal conversion and storage. J. Energy Storage, 101: (2024).
31. El-Gendi, H., Albrahim, J. S., Alenezi, H., El-Fakharany, E. M., El-Maradny, Y. A. & Saleh, A. K., Bioactive bacterial cellulose/chitosan/sodium alginate composite film functionalized with Moringa oleifera seed extract: Antimicrobial, anticancer, and molecular docking studies. Int. J. Biol. Macromol., 307: (2025).
32. Kloster, M., Mosiewicki, M. A. & Marcovich, N. E., Chitosan/sodium alginate aerogels showing effective adsorption of anionic Congo Red and cationic Methylene Blue dyes for sustainable water treatment. Int. J. Biol. Macromol., 329: (2025).
33. Shah, M. A. R., Khan, R. A., Khan, H. U., Rehman, O. U., Kayani, S.-I., Zeb, L., Khan, K. A., et al., Carboxymethyl cellulose/sodium alginate composite films encapsulated with turmeric essential oil-in-water nanoemulsion and gallic acid for grapes preservation. Food Chem., 504: 147954 (2026).
34. Grzybek, P., Pryciuk, J., Wardejn, S., Gołombek, K., Gaida, R., Pechociakova, M., Wacławek, S., et al., Polyol-modified biopolymer membranes of sodium alginate and chitosan for CO2/N2 and CO2/O2 separation: Linking structure and gas transport performance. Chem. Eng. J. Adv., 24: (2025).
35. Phatchayawat, P. P., Khamkeaw, A., Yodmuang, S. & Phisalaphong, M., 3D bacterial cellulose-chitosan-alginate-gelatin hydrogel scaffold for cartilage tissue engineering. Biochem. Eng. J., 184: (2022).
36. Fu, J., Yap, J. X., Leo, C. P. & Chang, C. K., Carboxymethyl cellulose/sodium alginate beads incorporated with calcium carbonate nanoparticles and bentonite for phosphate recovery. Int. J. Biol. Macromol., 234: (2023).
37. Wang, M., Zang, Y., Hong, K., Zhao, X., Yu, C., Liu, D., An, Z., et al., Preparation of pH-sensitive carboxymethyl cellulose/chitosan/alginate hydrogel beads with reticulated shell structure to deliver Bacillus subtilis natto. Int. J. Biol. Macromol., 192: 684–691 (2021).
38. Huang, X., Lee, C. S., Zhang, K., Alhamzani, A. G. & Hsiao, B. S., Sodium Alginate–Aldehyde Cellulose Nanocrystal Composite Hydrogel for Doxycycline and Other Tetracycline Removal. Nanomaterials, 13(7): (2023).
39. Ahmed, A. M., Berrada, M., Mekonnen, M. L., Assen, A. H., Mengesha, E. T., Beniazza, R., Mekonnen, K. N., et al., Surface charge modulation in metal-crosslinked sodium alginate-chitosan composite adsorbent: Optimized anionic-to-cationic polysaccharide component ratio for Cd and Cr removal from water. Carbohydr. Polym. Technol. Appl., 11: (2025).
40. Germanos, G., Youssef, S., Farah, W., Lescop, B., Rioual, S. & Abboud, M., The impact of magnetite nanoparticles on the physicochemical and adsorption properties of magnetic alginate beads. J. Environ. Chem. Eng., 8(5): (2020).
41. Alotaibi, A. M. & Elsayed, N. H., Adsorption and eliminating of diquat herbicide using layer double hydroxide enclosed in double layer hydrogel beads of carboxymethyl cellulose and alginate: Synthesis, characterization, adsorption isotherm, kinetics, thermodynamics and optimization via bo. Int. J. Biol. Macromol., 303: (2025).
42. Cai, C., Gao, L. & Xiong, Y., Green recyclable chitosan/carboxymethyl cellulose/sodium alginate magnetic double-network composite hydrogels for adsorption of MB and Cu2+. J. Water Process Eng., 63: (2024).
43. Xu, J., Sun, Y. & Zhang, J., Solvothermal synthesis of Fe3O4 nanospheres for high-performance electrochemical non-enzymatic glucose sensor. Sci. Rep., 10(1): (2020).
44. Shafiei sabet, S., Komijani, S., Sharifian, G., Hosseini, F. & Mohajer, F., Chitosan glutamate nanoparticles loaded with Nisin for antibacterial and anticancer studies. Int. J. Biol. Macromol., 333: (2025).
45. Yi, W., Wang, F., Tan, Z., Wang, H., Wu, Y., Hao, X. & Xiong, F., All-biomass flexible sensor based on lignin carbon nanospheres/cellulose for human motion detection. Int. J. Biol. Macromol., 331: (2025).
46. Halbus, A. F., Athab, Z. H., Mohammed, S. B. & Baqir, S. J., Thermoresponsive and reusable chitosan/hydroxypropyl cellulose monolithic hydrogel with interconnected porosity engineered via freeze–thaw processing for selective dyes removal. Int. J. Biol. Macromol., 333: (2025).
47. Farras Fadillah, R., Badriani, R. E. & Fildzah, C. A., Efektivitas Media Filter Pasir Silika dan Arang Ampas Tebu untuk Menurunkan Warna Menggunakan Filtrasi Upflow. Rekayasa, 18(1): 9–19 (2025).
48. Amrillah, N. A. Z., Rahayu, A., Dhias Cahya Hakika., Vivi Sisca., Veranica., Firda Mahira Alfiata Chusna., Lia Anggresani., et al., Isothermic Adsorption Study of Nitrate Ion Adsorption in Bioethanol Waste Using Quaternary Ammonium Polymer. Sains Nat. J. Biol. Chem., 15(1): 01–09 (2025).
49. Abukhadra, M. R., Saad, I., Othman, S. I., Katowah, D. F., Ajarem, J. S., Alqarni, S. A., Allam, A. A., et al., Characterization of Fe0@Chitosan/Cellulose structure as effective green adsorbent for methyl Parathion, malachite Green, and levofloxacin Removal: Experimental and theoretical studies. J. Mol. Liq., 368: 120730 (2022).
50. Zhu, H., Chen, S., Duan, H., He, J. & Luo, Y., Removal of anionic and cationic dyes using porous chitosan/carboxymethyl cellulose-PEG hydrogels: Optimization, adsorption kinetics, isotherm and thermodynamics studies. Int. J. Biol. Macromol., 231: (2023).
51. Jiang, W., Yang, J., Wang, Y., Gao, Y., Ren, W., Yu, Y. & Liu, Q., Efficient dye degradation via fenton-like catalysis using GO/MX-Fe2+ composites: Synthesis, performance, and mechanism. J. Water Process Eng., 77: (2025).
52. Tchuifon, D. R. T., Fotsop, C. G., Tchaptchet, T. H., Mekuete, L. B. K., Feudjio, F. D. S., Fongang, J. G., Nguena, K. L. T., et al., Magnetic porous (Cu-MOF@Fe3O4) materials-based metal organic framework as heterogeneous catalytic supports for optimized tartrazine yellow (E102) dye degradation by Fenton-like process. J. Mol. Struct., 1348: (2025).
53. Hamidon, T. S., Maznan, N. N., Idris, N. N., Trache, D. & Hussin, M. H., Kinetics and equilibrium studies of congo red adsorption using alginate hydrogel beads impregnated with coconut shell derived-cellulose nanocrystals. J. Ind. Eng. Chem., 149: 616–629 (2025).
54. Chen, X., Huang, Z., Luo, S. Y., Zong, M. H. & Lou, W. Y., Multi-functional magnetic hydrogels based on Millettia speciosa Champ residue cellulose and Chitosan: Highly efficient and reusable adsorbent for Congo red and Cu2+ removal. Chem. Eng. J., 423: (2021).
Downloads
Published
How to Cite
Issue
Section
Citation Check
License
This work is licensed under a Creative Commons Attribution 4.0 International License.
Please find the rights and licenses in Jurnal Riset Kimia (J. Ris. Kim). By submitting the article/manuscript of the article, the author(s) agree with this policy. No specific document sign-off is required.
1. License
The use the article will be governed by the Creative Commons Attribution license as currently displayed on Creative Commons Attribution 4.0 International License.Â
2. Author(s)' Warranties
The author warrants that the article is original, written by stated author(s), has not been published before, contains no unlawful statements, does not infringe the rights of others, is subject to copyright that is vested exclusively in the author and free of any third party rights, and that any necessary written permissions to quote from other sources have been obtained by the author(s).
3. User Rights
Under the Creative Commons license, the journal permits users to copy, distribute, and display the material for any purpose. Users will also need to attribute authors and J. Ris. Kim on distributing works in the journal and other media of publications.
4. Rights of Authors
Authors retain all their rights to the published works, such as (but not limited to) the following rights;
- Copyright and other proprietary rights relating to the article, such as patent rights,
- The right to use the substance of the article in own future works, including lectures and books,
- The right to reproduce the article for own purposes,
- The right to self-archive the article,
- The right to enter into separate, additional contractual arrangements for the non-exclusive distribution of the article's published version (e.g., post it to an institutional repository or publish it in a book), with an acknowledgment of its initial publication in this journal.
5. Co-Authorship
If the article was jointly prepared by more than one author, any authors submitting the manuscript warrants that he/she has been authorized by all co-authors to be agreed on this copyright and license notice (agreement) on their behalf, and agrees to inform his/her co-authors of the terms of this policy. J. Ris. Kim will not be held liable for anything that may arise due to the author(s) internal dispute. J. Ris. Kim will only communicate with the corresponding author.
![](https://i1.wp.com/www.internetgeography.net/wp-content/uploads/2017/11/word-doc-icon.png"){kind=icon}
