Journal of Multidisciplinary Applied Natural Science
Periódico de Acesso Aberto
Scopus CiteScore 2024
4.8
Calculated on 05 May, 2025
SJR 2024
0.31
Powered by scimagojr.com
Periódico de Acesso Aberto
4.8
Calculated on 05 May, 2025
0.31
Powered by scimagojr.com
https://doi.org/10.47352/jmans.2774-3047.332
Hans Kristianto
Christ Joseph Carlo Wibowo Apoenx
Stephanie Hanafi
Susiana Prasetyo
Asaf K Sugih
Wibawa Hendra Saputera
Johnner P Sitompul
In recent years, Fe3O4 nanoparticles have been widely developed as adsorbents for various applications. However, their hydrophobic surface limits their application in polar systems, necessitating surface modifications to enhance adsorption. In this study, gallic acid was employed to modify Fe3O4 nanoparticles, as its carboxyl and phenolic hydroxyl groups can provide sites for protein adsorption. The research aims to determine the optimal pH, adsorption capacity, isotherm models, and thermodynamic parameters for bovine serum albumin (BSA) adsorption, as a model protein, onto gallic acid-modified and unmodified Fe3O4 nanoparticles using batch experiments. The experiments varied pH (3.6–5.6), initial BSA concentrations (0.50–1.75 mg/L), and temperatures (30–50 °C). FTIR analysis confirmed successful modification through the presence of C=O stretching bonds, while BSA adsorption was indicated by the appearance of amide groups and transmission electron microscopy (TEM) observations. Maximum adsorption was achieved at pH 4.8, in the vicinity of BSA isoelectric point. The Langmuir isotherm model best described the adsorption process for all adsorbents. Thermodynamic analysis showed that BSA adsorption was spontaneous and endothermic with increased randomness, as evidenced by negative Gibbs free energy, along with positive enthalpy and entropy values. Surface modification with gallic acid enhanced BSA adsorption capacity to 68.49 mg/g compared to 34.84 mg/g for unmodified Fe3O4 at 50 °C.
[1] L. Shen, B. Li, and Y. Qiao. (2018). "Fe3O4 Nanoparticles in Targeted Drug/Gene Delivery Systems". Materials. 11 (2): 324. 10.3390/ma11020324.
DOI: https://doi.org/10.3390/ma11020324[2] M. D. Nguyen, H. V. Tran, S. Xu, and T. R. Lee. (2021). "Fe3O4 Nanoparticles: Structures, Synthesis, Magnetic Properties, Surface Functionalization, and Emerging Applications". Applied Sciences. 11 (23): 11301. 10.3390/app112311301.
DOI: https://doi.org/10.3390/app112311301[3] E. U. Ikhuoria, I. E. Uwidia, R. O. Okojie, I. H. Ifijen, I. D. Chikaodili, and A. Fatiqin. (2024). "Advancing Green Nanotechnology: Harnessing the Bio-Reducing Properties of Musa paradisiaca Peel Extract for Sustainable Synthesis of Iron Oxide Nanoparticles". Journal of Multidisciplinary Applied Natural Science. 4 (1): 108-119. 10.47352/jmans.2774-3047.194.
DOI: https://doi.org/10.47352/jmans.2774-3047.194[4] L. S. Ganapathe, M. A. Mohamed, R. M. Yunus, and D. D. Berhanuddin. (2020). "Magnetite (Fe3O4) Nanoparticles in Biomedical Applications: From Synthesis to Surface Functionalisation". Magnetochemistry. 6 (4): 68. 10.3390/magnetochemistry6040068.
DOI: https://doi.org/10.3390/magnetochemistry6040068[5] S. E. Kim, M. V. Tieu, S. Y. Hwang, and M. H. Lee. (2020). "Magnetic Particles: Their Applications from Sample Preparation to Biosensing Platforms". Micromachines. 11 (3): 302. 10.3390/mi11030302.
DOI: https://doi.org/10.3390/mi11030302[6] S. Yu, V. M. H. Ng, F. Wang, Z. Xiao, C. Li, L. B. Kong, W. Que, and K. Zhou. (2018). "Synthesis and Application of Iron-Based Nanomaterials as Anodes for Lithium-Ion Batteries and Supercapacitors". Journal of Materials Chemistry A. 6 (20): 9332-9367. 10.1039/C8TA01683F.
DOI: https://doi.org/10.1039/C8TA01683F[7] H. Kristianto, S. Prasetyo, and A. K. Sugih. (2022). "Green-Synthesized Iron Nanoparticles Using Leucaena leucocephala Crude Extract as a Fenton-Like Catalyst". 2493 : 050001. 10.1063/5.0109914
DOI: https://doi.org/10.1063/5.0109914[8] E. D. Suhardi, F. V. Hermawan, H. Kristianto, S. Prasetyo, and A. K. Sugih. (2024). "Enhancing Water–Wastewater Treatment Efficiency: A Synergistic Approach Using Polyaluminum Chloride, Sodium Alginate, and Magnetite for Congo Red Removal". Chemical Papers. 78 : 3971-3981. 10.1007/s11696-024-03367-9.
DOI: https://doi.org/10.1007/s11696-024-03367-9[9] H. Kristianto, W. H. Saputera, and J. P. Sitompul. (2025). "Novel Developments in Magnetic Coagulation: Enhancing Water and Wastewater Treatment Efficiency". International Journal of Environmental Science and Technology. 10.1007/s13762-025-06668-y.
DOI: https://doi.org/10.1007/s13762-025-06668-y[10] A. K. Sugih, M. A. Deiza, S. F. Nurmawan, S. Prasetyo, D. Tan, and H. Kristianto. (2025). "Combination of FeCl3 and Fe3O4 as a Magnetic Coagulant for Congo Red Removal". Indonesian Journal of Urban and Environmental Technology. 8 (1): 99-115. 10.25105/urbanenvirotech.v8i1.22575.
DOI: https://doi.org/10.25105/urbanenvirotech.v8i1.22575[11] H. Kristianto, W. H. Saputera, and J. P. Sitompul. (2025). "Small-Scale Protocol for Magnetic Coagulation Testing". MethodsX. 15 103550. 10.1016/j.mex.2025.103550.
DOI: https://doi.org/10.1016/j.mex.2025.103550[12] Y. Shen, B. Jiang, and Y. Xing. (2021). "Recent Advances in the Application of Magnetic Fe3O4 Nanomaterials for the Removal of Emerging Contaminants". Environmental Science and Pollution Research. 28 : 7599-7620. 10.1007/s11356-020-11877-8.
DOI: https://doi.org/10.1007/s11356-020-11877-8[13] B. Zhang, H. Zhang, X. Li, X. Lei, C. Li, D. Yin, X. Fan, and Q. Zhang. (2013). "Synthesis of BSA/Fe3O4 Magnetic Composite Microspheres for Adsorption of Antibiotics". Materials Science and Engineering C. 33 (7): 4401-4408. 10.1016/j.msec.2013.06.038.
DOI: https://doi.org/10.1016/j.msec.2013.06.038[14] C. He, M. Xie, F. Hong, X. Chai, H. Mi, X. Zhou, L. Fan, Q. Zhang, T. Ngai, and J. Liu. (2016). "A Highly Sensitive Glucose Biosensor Based on Gold Nanoparticles/Bovine Serum Albumin/Fe3O4 Biocomposite Nanoparticles". Electrochimica Acta. 222 : 1709-1715. 10.1016/j.electacta.2016.11.162.
DOI: https://doi.org/10.1016/j.electacta.2016.11.162[15] L. Qian, J. Sun, C. Hou, J. Yang, Y. Li, D. Lei, M. Yang, and S. Zhang. (2017). "Immobilization of Bovine Serum Albumin on Ionic Liquid-Functionalized Magnetic Fe3O4 Nanoparticles for Use in a Surface Imprinting Strategy". Talanta. 168 : 174-182. 10.1016/j.talanta.2017.03.044.
DOI: https://doi.org/10.1016/j.talanta.2017.03.044[16] K. Atacan and M. Ozacar. (2015). "Characterization and Immobilization of Trypsin on Tannic Acid-Modified Fe3O4 Nanoparticles". Colloids and Surfaces B: Biointerfaces. 128 : 227-236. 10.1016/j.colsurfb.2015.01.038.
DOI: https://doi.org/10.1016/j.colsurfb.2015.01.038[17] K. Atacan, B. Cakiroglu, and M. Ozacar. (2017). "Efficient Protein Digestion Using Immobilized Trypsin onto Tannin-Modified Fe3O4 Magnetic Nanoparticles". Colloids and Surfaces B: Biointerfaces. 156 : 9-18. 10.1016/j.colsurfb.2017.04.055.
DOI: https://doi.org/10.1016/j.colsurfb.2017.04.055[18] E. Hermawan, L. U. Carmen, H. Kristianto, S. Prasetyo, A. K. Sugih, and A. A. Arbita. (2022). "Synthesis of Magnetic Natural Coagulants and Their Application for Treating Congo Red Synthetic Wastewater". Water, Air, and Soil Pollution. 233 : 443. 10.1007/s11270-022-05923-z.
DOI: https://doi.org/10.1007/s11270-022-05923-z[19] H. Nosrati, M. Adibtabar, A. Sharafi, H. Danafar, and M. H. Kheiri. (2018). "PAMAM-Modified Citric Acid-Coated Magnetic Nanoparticles as pH-Sensitive Biocompatible Carriers Against Human Breast Cancer Cells". Drug Development and Industrial Pharmacy. 44 (8): 1377-1384. 10.1080/03639045.2018.1451881.
DOI: https://doi.org/10.1080/03639045.2018.1451881[20] H. Nosrati, N. Sefidi, A. Sharafi, H. Danafar, and H. K. Manjili. (2018). "Bovine Serum Albumin-Coated Iron Oxide Magnetic Nanoparticles as Biocompatible Carriers for Curcumin Anticancer Drug". Bioorganic Chemistry. 76 : 501-509. 10.1016/j.bioorg.2017.12.033.
DOI: https://doi.org/10.1016/j.bioorg.2017.12.033[21] M. Shen, Y. Yu, G. Fan, G. Chen, Y. M. Jin, W. Tang, and W. Jia. (2014). "Synthesis and Characterization of Monodispersed Chitosan-Coated Fe3O4 Nanoparticles via a Facile One-Step Solvothermal Process for Adsorption of Bovine Serum Albumin". Nanoscale Research Letters. 9 : 296. 10.1186/1556-276X-9-296.
DOI: https://doi.org/10.1186/1556-276X-9-296[22] Z. U. Rahman, Y. Dong, C. Ren, Z. Zhang, and X. Chen. (2012). "Protein Adsorption on Citrate-Modified Magnetic Nanoparticles". Journal of Nanoscience and Nanotechnology. 12 : 2598-2606. 10.1166/jnn.2012.5751.
DOI: https://doi.org/10.1166/jnn.2012.5751[23] H. Kristianto, E. Reynaldi, S. Prasetyo, and A. K. Sugih. (2020). "Adsorbed Leucaena Protein on Citrate-Modified Fe3O4 Nanoparticles: Synthesis, Characterization, and Application as a Magnetic Coagulant". Sustainable Environment Research. 30 : 32. 10.1186/s42834-020-00074-4.
DOI: https://doi.org/10.1186/s42834-020-00074-4[24] R. Neha, A. Jaiswal, J. Bellare, and N. K. Sahu. (2017). "Synthesis of Surface-Grafted Mesoporous Magnetic Nanoparticles for Cancer Therapy". Journal of Nanoscience and Nanotechnology. 17 : 5181-5188. 10.1166/jnn.2017.13853.
DOI: https://doi.org/10.1166/jnn.2017.13853[25] Q. Xiao, C. Liu, H. Ni, Y. Zhu, Z. Jiang, and A. Xiao. (2019). "β-Agarase Immobilized on Tannic Acid-Modified Fe3O4 Nanoparticles for Efficient Preparation of Bioactive Neoagaro-Oligosaccharides". Food Chemistry. 272 : 586-595. 10.1016/j.foodchem.2018.08.017.
DOI: https://doi.org/10.1016/j.foodchem.2018.08.017[26] B. Badhani, N. Sharma, and R. Kakkar. (2015). "Gallic Acid: A Versatile Antioxidant with Promising Therapeutic and Industrial Applications". RSC Advances. 5 : 27540-27557. 10.1039/C5RA01911G.
DOI: https://doi.org/10.1039/C5RA01911G[27] N. A. A. Al-Zahrani, R. M. El-Shishtawy, and A. M. Asiri. (2020). "Recent Developments of Gallic Acid Derivatives and Their Hybrids in Medicinal Chemistry: A Review". European Journal of Medicinal Chemistry. 204 : 112609. 10.1016/j.ejmech.2020.112609.
DOI: https://doi.org/10.1016/j.ejmech.2020.112609[28] S. T. Shah, W. A. Yehya, O. Saad, K. Simarani, Z. Chowdhury, A. A. Alhadi, and L. A. Al-Ani. (2017). "Surface Functionalization of Iron Oxide Nanoparticles with Gallic Acid as Potential Antioxidant and Antimicrobial Agents". Nanomaterials. 7 (10): 306. 10.3390/nano7100306.
DOI: https://doi.org/10.3390/nano7100306[29] K. Atacan, B. Cakiroglu, and M. Ozacar. (2016). "Improvement of Stability and Activity of Immobilized Trypsin on Modified Fe3O4 Magnetic Nanoparticles for Hydrolysis of Bovine Serum Albumin and Application in Bovine Milk". Food Chemistry. 212 : 460-468. 10.1016/j.foodchem.2016.06.011.
DOI: https://doi.org/10.1016/j.foodchem.2016.06.011[30] D. Dorniani, M. Z. Hussein, A. U. Kura, S. Fakurazi, A. H. Shaari, and Z. Ahmad. (2012). "Preparation of Fe3O4 Magnetic Nanoparticles Coated with Gallic Acid for Drug Delivery". International Journal of Nanomedicine. 7 : 5745-5756. 10.2147/IJN.S35746.
DOI: https://doi.org/10.2147/IJN.S35746[31] X. Mu, C. Yan, Q. Tian, J. Lin, and S. Yang. (2017). "BSA-Assisted Synthesis of Ultrasmall Gallic Acid–Fe(III) Coordination Polymer Nanoparticles for Cancer Theranostics". International Journal of Nanomedicine. 12 : 7207-7223. 10.2147/IJN.S146064.
DOI: https://doi.org/10.2147/IJN.S146064[32] H. Kristianto, J. Alexander, S. Prasetyo, and A. K. Sugih. (2022). "Tannic Acid-Modified Iron Oxide Nanoparticles and Their Application in Protein Adsorption: Isotherm, Kinetic, and Thermodynamic Studies". Molekul. 17 (1): 49-59. 10.20884/1.jm.2022.17.1.5571.
DOI: https://doi.org/10.20884/1.jm.2022.17.1.5571[33] M. M. Bradford. (1976). "A Rapid and Sensitive Method for the Quantitation of Microgram Quantities of Protein Utilizing the Principle of Protein–Dye Binding". Analytical Biochemistry. 72 : 248-254. 10.1016/0003-2697(76)90527-3.
DOI: https://doi.org/10.1006/abio.1976.9999[34] E. C. Lima, A. Hosseini-Bandegharaei, J. C. Moreno-Piraján, and I. Anastopoulos. (2019). "A Critical Review of the Estimation of Thermodynamic Parameters on Adsorption Equilibria: Wrong Use of Equilibrium Constants in the Van’t Hoff Equation". Journal of Molecular Liquids. 273 : 425-434. 10.1016/j.molliq.2018.10.048.
DOI: https://doi.org/10.1016/j.molliq.2018.10.048[35] H. N. Tran, E. C. Lima, R. S. Juang, J. C. Bollinger, and H. P. Chao. (2021). "Thermodynamic Parameters of Liquid-Phase Adsorption Processes Calculated from Different Equilibrium Constants: A Comparison Study". Journal of Environmental Chemical Engineering. 9 (6): 106674. 10.1016/j.jece.2021.106674.
DOI: https://doi.org/10.1016/j.jece.2021.106674[36] N. R. Jannah and D. Onggo. (2019). "Synthesis of Fe3O4 Nanoparticles for Colour Removal of Printing Ink Solutions". IOP Conference Series: Journal of Physics: Conference Series. 1245 : 012040. 10.1088/1742-6596/1245/1/012040.
DOI: https://doi.org/10.1088/1742-6596/1245/1/012040[37] A. R. Khaskheli, S. Naz, F. Ozul, A. Aljabour, S. A. Mahesar, I. H. Patir, and M. Ersoz. (2016). "Urchin-Like Cobalt Nanostructures for Catalytic Degradation of Nitroanilines". Advanced Materials Letters. 7 (9): 748-753. 10.5185/amlett.2016.6264.
DOI: https://doi.org/10.5185/amlett.2016.6264[38] K. H. Sizeland, K. A. Hofman, I. C. Hallett, D. E. Martin, J. Potgieter, N. M. Kirby, A. Hawley, S. T. Mudie, T. M. Ryan, R. G. Haverkamp, and M. H. Cumming. (2018). "Nanostructure of Electrospun Collagen: Do Electrospun Collagen Fibers Form Native Structures?". Materialia. 3 : 90-96. 10.1016/j.mtla.2018.10.001.
DOI: https://doi.org/10.1016/j.mtla.2018.10.001[39] D. Pop, R. Buzatu, E. A. Moacă, C. G. Watz, S. C. Pînzaru, L. B. Tudoran, F. Nekvapil, Ș. Avram, C. A. Dehelean, M. O. Crețu, M. Nicolov, C. Szuhanek, and A. Jivănescu. (2021). "Development and Characterization of Fe3O4@Carbon Nanoparticles and Their Biological Screening Related to Oral Administration". Materials. 14 (13): 3556. 10.3390/ma14133556.
DOI: https://doi.org/10.3390/ma14133556[40] M. S. C. Barreto, E. J. Elzinga, and L. R. F. Alleoni. (2020). "Molecular Insights into Protein Adsorption on Hematite Surfaces Disclosed by In Situ ATR-FTIR/2D-COS Study". Scientific Reports. 10 : 13441. 10.1038/s41598-020-70201-z.
DOI: https://doi.org/10.1038/s41598-020-70201-z[41] V. S. Raghuwanshi, B. Yu, C. Browne, and G. Garnier. (2020). "Reversible pH-Responsive Bovine Serum Albumin Hydrogel Sponge Nanolayer". Frontiers in Bioengineering and Biotechnology. 8 : 573. 10.3389/fbioe.2020.00573.
DOI: https://doi.org/10.3389/fbioe.2020.00573[42] G. R. Mahdavinia and H. Etemadi. (2019). "Surface Modification of Iron Oxide Nanoparticles with κ-Carrageenan/Carboxymethyl Chitosan for Effective Adsorption of Bovine Serum Albumin". Arabian Journal of Chemistry. 12 (8): 3692-3703. 10.1016/j.arabjc.2015.12.002.
DOI: https://doi.org/10.1016/j.arabjc.2015.12.002[43] C. H. Kim, Z. F. Zhang, L. S. Wang, and T. Sun. (2020). "Preparation of MnO2-Impregnated Carbon-Coated Fe3O4 Nanocomposites and Their Application for Bovine Serum Albumin Adsorption". Rare Metals. 39 (3): 1151-1158. 10.1007/s12598-016-0779-3.
DOI: https://doi.org/10.1007/s12598-016-0779-3[44] M. M. Majd, V. Kordzadeh-Kermani, V. Ghalandari, A. Askari, and M. Sillanpaa. (2022). "Adsorption Isotherm Models: A Comprehensive and Systematic Review (2010–2020)". Science of the Total Environment. 812 : 151334. 10.1016/j.scitotenv.2021.151334.
DOI: https://doi.org/10.1016/j.scitotenv.2021.151334[45] M. Zhang, L. Fan, Y. Liu, and J. Li. (2023). "Migration of Gallic Acid from the Aqueous Phase to the Oil–Water Interface Using Pea Protein to Improve the Physicochemical Stability of Water-in-Oil Emulsions". Food Hydrocolloids. 135 : 108179. 10.1016/j.foodhyd.2022.108179.
DOI: https://doi.org/10.1016/j.foodhyd.2022.108179[46] T. Kopac and K. Bozgeyik. (2010). "Effect of Surface Area Enhancement on the Adsorption of Bovine Serum Albumin onto Titanium Dioxide". Colloids and Surfaces B: Biointerfaces. 76 (1): 265-271. 10.1016/j.colsurfb.2009.11.002.
DOI: https://doi.org/10.1016/j.colsurfb.2009.11.002[47] S. K. Swain and D. Sarkar. (2013). "Study of Bovine Serum Albumin Protein Adsorption and Release on Hydroxyapatite Nanoparticles". Applied Surface Science. 286 99-103. 10.1016/j.apsusc.2013.09.027.
DOI: https://doi.org/10.1016/j.apsusc.2013.09.027[48] M. Alkan, O. Demirbas, M. Dogan, and O. Arslan. (2006). "Surface Properties of Bovine Serum Albumin-Adsorbed Oxides: Adsorption, Kinetics, and Electrokinetic Properties". Microporous and Mesoporous Materials. 96 (1-3): 331-340. 10.1016/j.micromeso.2006.07.007.
DOI: https://doi.org/10.1016/j.micromeso.2006.07.007[49] M. A. Al-Ghouti and D. A. Daana. (2020). "Guidelines for the Use and Interpretation of Adsorption Isotherm Models: A Review". Journal of Hazardous Materials. 393 : 122383. 10.1016/j.jhazmat.2020.122383.
DOI: https://doi.org/10.1016/j.jhazmat.2020.122383[50] A. M. Aljeboree, A. N. Alshirifi, and A. F. Alkaim. (2017). "Kinetics and Equilibrium Study for the Adsorption of Textile Dyes on Coconut Shell Activated Carbon". Arabian Journal of Chemistry. 10 : S3381-S3393. 10.1016/j.arabjc.2014.01.020.
DOI: https://doi.org/10.1016/j.arabjc.2014.01.020[51] M. P. Schmidt and C. E. Martinez. (2016). "Kinetic and Conformational Insights of Protein Adsorption onto Montmorillonite Revealed Using In Situ ATR-FTIR/2D-COS". Langmuir. 32 (31): 7719-7729. 10.1021/acs.langmuir.6b00786.
DOI: https://doi.org/10.1021/acs.langmuir.6b00786[52] S. Dominguez-Medina, S. McDonough, P. Swanglap, C. F. Landes, and S. Link. (2012). "In Situ Measurement of Bovine Serum Albumin Interaction with Gold Nanospheres". Langmuir. 28 (24): 9131-9139. 10.1021/la3005213.
DOI: https://doi.org/10.1021/la3005213[53] Z. Wang, T. Yue, Y. Yuan, R. Cai, C. Niu, and C. Guo. (2013). "Kinetics of Adsorption of Bovine Serum Albumin on Magnetic Carboxymethyl Chitosan Nanoparticles". International Journal of Biological Macromolecules. 58 : 57-65. 10.1016/j.ijbiomac.2013.03.037.
DOI: https://doi.org/10.1016/j.ijbiomac.2013.03.037[54] J. Lyklema. (1995). "Fundamentals of Interface and Colloid Science". Academic Press. 10.1016/S1874-5679(06)80004-8.
DOI: https://doi.org/10.1016/S1874-5679(06)80004-8[55] Y. Yu, Y. Y. Zhuang, Z. H. Wang, and M. Q. Qiu. (2004). "Adsorption of Water-Soluble Dyes onto Modified Resin". Chemosphere. 54 (3): 425-430. 10.1016/S0045-6535(03)00654-4.
DOI: https://doi.org/10.1016/S0045-6535(03)00654-4[56] L. Abarca-Cabrera, P. Fraga-Garcia, and S. Berensmeier. (2021). "Bio–Nano Interactions: Binding Proteins, Polysaccharides, Lipids, and Nucleic Acids onto Magnetic Nanoparticles". Biomaterials Research. 25 : 12. 10.1186/s40824-021-00212-y.
DOI: https://doi.org/10.1186/s40824-021-00212-y[57] M. Rahmayanti, S. J. Santosa, and Sutarno. (2016). "Comparative Study on the Adsorption of [AuCl4]- onto Salicylic Acid- and Gallic Acid-Modified Magnetite Particles". Indonesian Journal of Chemistry. 16 (3): 329-337. 10.22146/ijc.21150.
DOI: https://doi.org/10.22146/ijc.21150[58] N. M. Fedortsov, E. V. Budkevich, I. A. Evdokimov, S. A. Ryabtseva, and R. O. Budkevich. (2022). "Bovine Serum Albumin with Gallic Acid: Molecular Modeling and Physicochemical Profiling". Foods and Raw Materials. 10 (1): 163-170. 10.21603/2308-4057-2022-1-163-170.
DOI: https://doi.org/10.21603/2308-4057-2022-1-163-170