Synthesis of Dendritic Magnetic Graphene Oxide by Radical Polymerization as Adsorbent for Rapid Removal of Dye from Aqueous Solutions

Document Type : Research Paper


1 PhD. Student, Dept. of Chemical Engineering, Yasuj Branch, Islamic Azad University, Yasuj, Iran

2 Assist. Prof., Dept. of Chemical Engineering, Yasuj Branch, Islamic Azad University, Yasuj, Iran

3 Assist. Prof., Dept. of Chemical Engineering, Gachsaran Branch, Islamic Azad University, Gachsaran, Iran

4 Prof., Dept. of Chemical Engineering, College of Engineering, Yasuj University, Yasuj, Iran


Disposal of dyes containing dyes from related industries has caused global concern. Therefore, removing dyes from aqueous solution is very important and necessary. In this work, a novel magnetic glycodendrimer is introduced as effective adsorbent for malachite green adsorption. Firstly, magnetic graphene oxide was prepared by co-precipitation method and then modified with ethylenediamine to generate amine group on the surface which was further reacted with mercaptoacetic acid to provide polymerizable MGO nanosheets. Thereafter, Allylamine was grafted onto nanosheets and subsequently, reacted with methacrylate in a Michael type reaction to generate methyl ester groups. Finally, amidation of the terminal methyl ester groups with chitosan resulted in the formation of glycodendrimer. The properties of the synthesized adsorbent were investigated using XRD, FTIR, BET, FESEM and TEM. The results showed that pH=5, temperature of 40 °C, initial concentration of 600 mg/mL and contact time of 10 min as optimal values for removing malachite green dye with nanosorbent (MGD) were obtained. The maximum adsorption capacity of green malachite was 452.97 μg/mg. The high correlation coefficient (R2=0.9947) for the Freundlich model confirms that the Freundlich model is suitable for fitting laboratory data. According to the compliance model, the heat absorption for malachite green is B=8.1447 j/mol and indicates that the process of dye adsorption with nanosorbent is physical. According to the results of fitting the kinetic models of dye adsorption kinetics by nanosorbent shows that Hu and McKay model with higher correlation coefficient (R2=0.994) than other models is more consistent with experimental data. Due to the fact that a large decrease in dye removal is not observed in 10 consecutive recovery cycles and therefore nanosorbent has a high stability and can be used several times.


Banerjee, S. & Chattopadhyaya, M. 2017. Adsorption characteristics for the removal of a toxic dye, tartrazine from aqueous solutions by a low cost agricultural by-product. Arabian Journal of Chemistry, 10, S1629-S1638.
Banisheykholeslami, F., Hosseini, M. & Darzi, G. N. 2021. Design of PAMAM grafted chitosan dendrimers biosorbent for removal of anionic dyes: adsorption isotherms, kinetics and thermodynamics studies. International Journal of Biological Macromolecules, 177, 306-316.
Bankole, M. T., Abdulkareem, A. S., Mohammed, I. A., Ochigbo, S. S., Tijani, J. O., Abubakre, O. K., et al. 2019. Selected heavy metals removal from electroplating wastewater by purified and polyhydroxylbutyrate functionalized carbon nanotubes adsorbents. Scientific Reports, 9, 1-19.
Ciğeroğlu, Z., Küçükyıldız, G., Erim, B. & Alp, E. 2021. Easy preparation of magnetic nanoparticles-rGO-chitosan composite beads: optimization study on cefixime removal based on RSM and ANN by using genetic algorithm approach. Journal of Molecular Structure, 1224, 129182.
Dehghani, M. H., Tajik, S., Panahi, A., Khezri, M., Zarei, A., Heidarinejad, Z., et al. 2018. Adsorptive removal of noxious cadmium from aqueous solutions using poly urea-formaldehyde: a novel polymer adsorbent. MethodsX, 5, 1148-1155.
Du, Q., Sun, J., Li, Y., Yang, X., Wang, X., Wang, Z., et al. 2014. Highly enhanced adsorption of congo red onto graphene oxide/chitosan fibers by wet-chemical etching off silica nanoparticles. Chemical Engineering Journal, 245, 99-106.
Dubinin, M. 1960. The potential theory of adsorption of gases and vapors for adsorbents with energetically nonuniform surfaces. Chemical Reviews, 60, 235-241.
Elsehly, E. M., Chechenin, N., Makunin, A., Motaweh, H., Vorobyeva, E., Bukunov, K., et al. 2016. Characterization of functionalized multiwalled carbon nanotubes and application as an effective filter for heavy metal removal from aqueous solutions. Chinese Journal of Chemical Engineering, 24, 1695-1702.
Gibson, N., Kuchenbecker, P., Rasmussen, K., Hodoroaba, V. D. & Rauscher, H. 2020. Volume-specific surface area by gas adsorption analysis with the BET method. Characterization of Nanoparticles, 265-294.
Gopinathan, R., Kanhere, J. & Banerjee, J. 2015. Effect of malachite green toxicity on non target soil organisms. Chemosphere, 120, 637-644.
Ho, Y. S. & Mckay, G. 2000. The kinetics of sorption of divalent metal ions onto sphagnum moss peat. Water Research, 34, 735-742.
Hoijang, S., Wangkarn, S., Ieamviteevanich, P., Pinitsoontorn, S., Ananta, S., Lee, T. R., et al. 2020. Silica-coated magnesium ferrite nanoadsorbent for selective removal of methylene blue. Colloids and Surfaces A: Physicochemical and Engineering Aspects, 606, 125483.
Kundu, S. & Gupta, A. 2006. Investigations on the adsorption efficiency of iron oxide coated cement (IOCC) towards As (V)- kinetics, equilibrium and thermodynamic studies. Colloids and Surfaces A: Physicochemical and Engineering Aspects, 273, 121-128.
Mashkoor, F., Nasar, A. & Jeong, C. 2022. Magnetized chitosan nanocomposite as an effective adsorbent for the removal of methylene blue and malachite green dyes. Biomass Conversion and Biorefinery, 1-13.
Mckay, G. 2001. Solution to the homogeneous surface diffusion model for batch adsorption systems using orthogonal collocation. Chemical Engineering Journal, 81, 213-221.
Nechifor, G., Pascu, D. E., Pascu, M., Traistaru, G. A. & Albu, P. C. 2015. Comparative study of Temkin and Flory-huggins isotherms for adsorption of phosphate anion on membranes. UPB Scientific Bulletin, Series B, 77, 63-72.
Parvin, N., Babapoor, A., Nematollahzadeh, A. & Mousavi, S. M. 2020. Removal of phenol and β-naphthol from aqueous solution by decorated graphene oxide with magnetic iron for modified polyrhodanine as nanocomposite adsorbents: kinetic, equilibrium and thermodynamic studies. Reactive and Functional Polymers, 156, 104718.
Periakaruppan, R., Chen, X., Thangaraj, K., Jeyaraj, A., Nguyen, H. H., Yu, Y., et al. 2021. Utilization of tea resources with the production of superparamagnetic biogenic iron oxide nanoparticles and an assessment of their antioxidant activities. Journal of Cleaner Production, 278, 123962.
Pooresmaeil, M., Namazi, H. & Salehi, R. 2020. Synthesis of photoluminescent glycodendrimer with terminal
β-cyclodextrin molecules as a biocompatible pH-sensitive carrier for doxorubicin delivery. Carbohydrate Polymers, 246, 116658.
Radushkevich, L. 1949. Potential theory of sorption and structure of carbons. Zhurnal Fizicheskoi Khimii, 23, 1410-1420.
Shah, H. U. R., Ahmad, K., Naseem, H. A., Parveen, S., Ashfaq, M., Rauf, A., et al. 2021. Water stable graphene oxide metal-organic frameworks composite (ZIF-67@ GO) for efficient removal of malachite green from water. Food and Chemical Toxicology, 154, 112312.
Shen, H., Wang, Z., Zhou, A., Chen, J., Hu, M., Dong, X., et al. 2015. Adsorption of phosphate onto amine functionalized nano-sized magnetic polymer adsorbents: mechanism and magnetic effects. RSC Advances, 5, 22080-22090.
Vakili, M., Rafatullah, M., Salamatinia, B., Abdullah, A. Z., Ibrahim, M. H., Tan, K. B., et al. 2014. Application of chitosan and its derivatives as adsorbents for dye removal from water and wastewater: a review. Carbohydrate Polymers, 113, 115-130.
Wang, Y., Yao, M., Chen, Y., Zuo, Y., Zhang, X. & Cui, L. 2015. General synthesis of magnetic mesoporous FeNi/graphitic carbon nanocomposites and their application for dye adsorption. Journal of Alloys and Compounds, 627, 7-12.
Zhang, Y., Wang, H., Eberhardt, T. L., Gu, Q. & Pan, H. 2021. Preparation of carboxylated lignin-based epoxy resin with excellent mechanical properties. European Polymer Journal, 150, 110389.
Zhu, Y., Xue, J., Xu, T., He, G. & Chen, H. 2017. Enhanced photocatalytic activity of magnetic core–shell Fe3O4@ Bi2O3–RGO heterojunctions for quinolone antibiotics degradation under visible light. Journal of Materials Science: Materials in Electronics, 28, 8519-8528.