Developing a New Model for Optimizing Response in Design of Experiments Considering Consumable Factors: Removal of Pollutant from Wastewater with Fe3O4/graphene Nano-sorbent
- School of Chemistry and Chemical Engineering Yulin University; Yulin, 719000, China
- Department of Industrial Engineering, Na.C., Islamic Azad University, Najafabad, Iran
- Department of Industrial Engineering, Faculty of Engineering Science, Quchan University of Technology, Quchan, Iran
Received: 04-03-2025
Revised: 30-03-2025
Accepted: 29-04-2025
Published in Issue 30-04-2025
Copyright (c) 2025 Jieying Liu, Yong Go, Ali Behmaneshfar, Abdolhossein Sadrnia, Zhifang Zhang, Rui Dang (Author)

This work is licensed under a Creative Commons Attribution 4.0 International License.
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Abstract
Removing toxic pollutants, especially colored compounds, from water samples and surface wastewater is one of the most significant and challenging issues in the environmental field. This paper aims to develop a new model for optimizing responses in the Design of Experiments (DoE) by dividing the process into different stages. The process is broken down into several stages based on consumable factors such as time and adsorbent weight. The number of stages increases until the stopping criteria are met. These criteria include restrictions on the cost of adding a new stage and obtaining an unsatisfactory response in the subsequent stage. In this regard, Fe3O4/graphene adsorbent was synthesized using a chemical precipitation strategy and characterized by FESEM, XRD, EDS, and mapping analysis methods. The presence of (220); (400); (422); (511); (440) and (533) layers in XRD pattern confirm Fe3O4 nanoparticle with high purity and crystallinity structure and particle size 45 nm. The removal of Sudan I by the Fe3O4/graphene adsorbent was optimized using Response Surface Methodology (RSM) based on the Box-Behnken design. The four effective factors are the weight of the adsorbent, time (both consumable factors), pH, and temperature. The proposed model increased the removal percentage significantly, from 65.4% in a single-stage process to 88.67% in a four-stage process. Therefore, it can be concluded that the pollutant removal in this study is much more efficient than the existing method at the same factor levels. It is important to note that increasing the process duration and adsorbent weight will result in higher costs. However, in this model, the high levels of factors remain unchanged due to the increased number of stages. As a result, the costs associated with establishing these factors remain constant. The results show a recovery percentage between 84.1% and 87.5%, for groundwater (well water) and drinking removal that confirming the effectiveness of both the adsorbent and the method for real-world applications.
Keywords
- Fe3O4/graphene adsorbent,
- Sudan I,
- Removal,
- Response Surface Methodology,
- Design of Experiments,
- Consumable Factors
References
- Rostami, M., Badiei, A., Alijani, M. et al. Nanoarchitectonic MOF-derived materials for enhanced photocatalytic activity in organic contaminant removal: A review. Alex Eng J 126, 448-479 (2025).
- Madhav, S., Ahamad, A., Singh, A.K. et al. 2020. Water pollutants: sources and impact on the environment and human health. Sensors in water pollutants monitoring: Role of Material. Advanced Functional Materials and Sensors. Springer, Singapore. pp. 43-62.
- Bafana, A., Devi, S.S. & Chakrabarti, T. Azo dyes: past, present and the future. Environ Rev 19, 350-371 (2011).
- Shah M.P., Azo dye removal technologies. Adv Res Appl 5(1), 1090 (2018).
- Behmaneshfar, A., Ghashang, M., Reza Mohammad Shafiee, M. et al. Optimization of the preparation condition of 2, 4, 5-triphenyl-1H-imidazole over BaSO4 nanoparticles as catalyst using a response surface methodology (RSM). Curr Nanosci 11, 56-63 (2015).
- Karimifard, S. & Moghaddam. M.R.A. Application of response surface methodology in physicochemical removal of dyes from wastewater: a critical review. Sci Total Environ 640, 772-797 (2018).
- Naboulsi, A., Naboulsi, I., Bouzid, T. et al. Tetracycline removal by a natural biosorbent: optimization by response surface methods employing DOE/FFD design of the experiment. Int J Environ Anal Chem 105, 223-244 (2025).
- Bayuo, J., Rwiza, M.J. & Mtei. K.M. Modeling and optimization of trivalent arsenic removal from wastewater using activated carbon produced from maize plant biomass: a multivariate experimental design approach. Biomass Convers Biorefin 14, 24809-24832 (2024).
- Shamsudin, N.A., Omar, Q., Ismail, I. et al. Oil palm fronds activated carbon via microwave-assisted H3PO4 activation: Box-Behnken optimization for crystal violet dye removal. AUIQ complement biol syst 1(1), 77-88 (2024).
- Dhiman, P., Goyal, D., Rana, G. at al. Recent advances on carbon-based nanomaterials supported single-atom photo-catalysts for waste water remediation. J Nanostruct Chem 14(1), 21-52 (2014).
- Yang, H., Choi, G.R., Choi, D. et al. Textile waste-derived functional carbon materials for selective pharmaceutical pollutant removal. Alex Eng J 116, 321-330 (2025).
- Şenol, Z.M., El Messaoudi, N., Ciğeroglu, Z. et al. Removal of food dyes using biological materials via adsorption: a review. Food Chem 450, 139398 (2024).
- Hamid, N., Junaid, M., Sultan, M. et al. The untold story of PFAS alternatives: Insights into the occurrence, ecotoxicological impacts, and removal strategies in the aquatic environment. Water Res 250, 121044 (2024).
- Mehta, J., Dhaka, R.K., Dilbaghi, N. et al. Recent advancements in adsorptive removal of organophosphate pesticides from aqueous phase using nanomaterials. J Nanostruct Chem 14, 53-70 (2024).
- Behmaneshfar, A., Sadrnia, A. & Karimi-Maleh, H. A review of different types of DOE methods as a useful platform for improving the performance of nano adsorbents in removal systems of pollutants. Nanosci Nanotechnol Asia 10, 219-227 (2020).
- Aghaa, H.M., Musa, S.A., Hapiz, A. et al. Biocomposite adsorbent of grafted Chitosan-benzaldehyde/Lactobacillus Casei Bacteria for removal of acid Red 88 Dye: box-benken design optimization and mechanism approach. AUIQ complement biol syst 2, 1-14 (2025).
- Kyzas, G.Z. & Matis, K.A. Nanoadsorbents for pollutants removal: a review. J Mol Liq 203, 159-168 (2015).
- Wu, T., Karimi-Maleh, H., Li, Y. et al. 3D printed porous chitosan/metal–organic framework composites as effective adsorbents to remove heavy metals from wastewater. Chem Eng J 493, 152780 (2024).
- Fu F. & Wang, Q. Removal of heavy metal ions from wastewaters: a review. J Environ Manage 92, 407-418 (2011).
- Joo, J.H., Kim, S.H., Kim, J.H. et al. Recent advances in activated carbon fibers for pollutant removal. Carbon Lett 35, 21-44 (2025).
- Verma, A., Sharma, G., Wang, T. et al. Graphitic carbon nitride (g-C3N4)-based magnetic photocatalysts for removal of antibiotics. Carbon Lett 35, 45-73 (2025).
- Ruparelia, J., Duttagupta, S., Chatterjee, A. et al. Potential of carbon nanomaterials for removal of heavy metals from water. Desalination 232, 145-156 (2008).
- Almomani, F., Bhosale, R., Khraisheh, M. et al. Heavy metal ions removal from industrial wastewater using magnetic nanoparticles (MNP). Appl Surf Sci 506, 144924 (2020).
- Kumar, J.A., Sathish, S., Prabu, D. et al. Waste shrimp shell mediated Chitosan-Magnesium Oxide nanocomposite: Synthesis, characterization and exploitation towards acenaphthene removal from aqueous solution. Alex Eng J 104, 124-135 (2024).
- Liu, X., Li, Y., Z. Chen, et al. Advanced porous nanomaterials as superior adsorbents for environmental pollutants removal from aqueous solutions. Crit Rev Env Sci Tec 53, 1289-1309 (2023).
- Thakur, K. & Kandasubramanian, B. Graphene and graphene oxide-based composites for removal of organic pollutants: a review. J Chem Eng Data 64, 833-867 (2019).
- Tang, S.C. & Lo, I.M. Magnetic nanoparticles: essential factors for sustainable environmental applications. Water Res 47, 2613-2632 (2013).
- Sadrnia, A., Orooji, Y., Behmaneshfar, A. et al. Developing a simple box–beh nken experimental design on the removal of doxorubicin anticancer drug using Fe3O4/graphene nanoribbons adsorbent. Environ Res 200, 111522 (2021).
- Boruah, P.K., Sharma, B., Hussain, N. et al. Magnetically recoverable Fe3O4/graphene nanocomposite towards efficient removal of triazine pesticides from aqueous solution: Investigation of the adsorption phenomenon and specific ion effect. Chemosphere 168, 1058-1067 (2017).
- Guo, L., Ye, P., Wang, J. et al. Three-dimensional Fe3O4-graphene macroscopic composites for arsenic and arsenate removal. J Hazard Mater 298, 28-35 (2015).
- Lv, X., Xue, X., Jiang, G. et al. Nanoscale zero-valent iron (nZVI) assembled on magnetic Fe3O4/graphene for chromium (VI) removal from aqueous solution. J Colloid Interface Sci 417, 51-59 (2014).
- You, N., Wang, X.F., Li, J.Y., et al. Synergistic removal of arsanilic acid using adsorption and magnetic separation technique based on Fe3O4@ graphene nanocomposite. J Ind Eng Chem 70, 346-354 (2019).
- Behmaneshfar, A., Sadrnia, A. & Karimi-Maleh, H. Application of box–behnken experimental design for optimizing the performance of reduced graphene/Fe3O4 nano adsorbent for removal of raloxifene anticancer drug. Chem Methodol 4, 679-694 (2020).
- Lanjwani, M.F., Tuzen, M. & Khuhawar, M.Y. Photocatalytic degradation of Sudan black B dye by using synthesized SnO2 nanoparticles as a catalyst: factorial design, kinetic and isotherm models. Chem Pap 78, 4813-4826 (2024).
- Angulakshmi, V., Mageswari, S., Kalaiselvan, S. et al. Box-Behnken design for photocatalytic degradation of Sudan black b by catalyst-embedded multiwalled carbon nanotubes. J Environ Nanotech 13, 213-225 (2024).
- Frieri, R., Mariti, M. & Paludi, M. Design of experiments and manufacturing design space for multi‐step processes. Appl Stoch Models Bus Ind 37, 942-960 (2021).
- Karimi-Maleh, H., Shafieizadeh, M., Taher, M.A. et al. The role of magnetite/graphene oxide nano-composite as a high-efficiency adsorbent for removal of phenazopyridine residues from water samples, an experimental/theoretical investigation. J Mol Liq 298, 112040 (2020).
- Box, G.E. & Wilson. K.B. 1992. On the experimental attainment of optimum conditions, Breakthroughs in statistics: methodology and distribution. Springer pp. 270-310.
- Abdulhameed, A.S., Wu, R., Reghioua, A. et al. Activated carbon derived from rice husk biomass using pyrolysis-assisted tartaric acid activation for removal of reactive orange 16 dye: adsorption modeling using response surface methodology. AUIQ complement biol syst 1(1), 89-95 (2024).
- Shi J. & Zhou, S. Quality control and improvement for multistage systems: A survey. IIE Trans 41, 744-753 (2009).
- Yew, Y.P., Shameli, K., Miyake, M. et al. Green synthesis of magnetite (Fe3O4) nanoparticles using seaweed (Kappaphycus alvarezii) extract. Nanoscale Res 11, 1-7 (2016).
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