Application of Fe₃O₄@Carbon/Graphene Oxide Nanocomposites for Cu(II) Removal from Wastewater

Abstract:

The Cu²⁺ in the drinking water has a very serious impact on human health and social ecology. Many countries have the policy on the Cu²⁺ concentration limitation in drinking water and the industrial Cu²⁺ emission standards for the treated wastewater. Scientists have developed many methods to remove Cu²⁺ from wastewater. Among all the adsorption method is widely used due to its high efficacy, feasibility and low cost. The adsorbent is critical to achieving superior Cu²⁺ removal result. In this paper, Fe₃O₄/carbon-graphene oxide nanocomposites (Fe₃O₄@C-GO) were prepared by a hydrothermal method. The Fe₃O₄@C-GO is the main absorbent to Cu²⁺ through chemisorption. The specific surface area of Fe₃O₄@C-GO dramatically increases from 16 m²/g of Fe₃O₄@C to 62 m²/g, which expands the Cu²⁺ absorption capacity up to 350 mg/g. Fe₃O₄ nanoparticles with about 12 nm in diameter are uniformly encapsulated in the C-GO matrix, and therefore the Fe₃O₄@C-GO can be easily separated from the solution via magnetics. This adsorbent is also very easily recovered by an external magnetic field from the treated wastewater and has high reusability.

• Periodical: Journal of Nano Research (Volume 75)
• Pages: 41-58
• DOI: https://doi.org/10.4028/p-309506
• Online since: September 2022
• Authors: Meng Ya Wu, Ri Liang Wu, Chuang Qi Zang, Chang Yuan Yu, Yun Fang Liu*
• Keywords: Adsorption, Cu²⁺ Removal, Graphene Oxide, Magnetite Nanoparticle, Nanocomposite

References

[1] Agency for toxic substances and disease registry, Public health statement: Copper. (2004-09-26). https://www.atsdr.cdc.gov/ToxProfiles/tp132-c1-b.

[2] E.G. Farmaki, N.S. Thomaidis, I.N. Pasias, C. Baulard, L. Papaharisis, C.E. Efstathiou, Environmental impact of intensive aquaculture: Investigation on the accumulation of metals and nutrients in marine sediments of Greece, Sci. Total Environ. 485 (2014) 554-562.

DOI: 10.1016/j.scitotenv.2014.03.125

[3] T. Kameda, Y. Suzuki, T. Yoshioka, Removal of arsenic from an aqueous solution by coprecipitation with manganese oxide, J. Environ. Chem. Eng. 2 (2014) 2045-2049.

DOI: 10.1016/j.jece.2014.09.004

[4] A. Abejón, A. Garea, A. Irabien, Arsenic removal from drinking water by reverse osmosis: Minimization of costs and energy consumption, Sep. Purif. Technol. 144 (2015) 46-53.

DOI: 10.1016/j.seppur.2015.02.017

[5] X.P. Pei, L. Gan, Z.H. Tong, H.P. Gao, S.Y. Meng, W.L. Zhang, P.X. Wang, Y.S. Chen, Robust cellulose-based composite adsorption membrane for heavy metal removal, J. Hazard. Mater. 406 (2021) 124746.

DOI: 10.1016/j.jhazmat.2020.124746

[6] W.J. Wang, Z.L. Xu, X.X. Zhang, W. Andreas, S. En, Y. Qin, X.P. Zhao, B.C. Zhou, L.X.Y. Li, Rapid and efficient removal of organic micropollutants from environmental water using a magnetic nanoparticles-attached fluorographene-based sorbent, Chem. Eng. J. 343 (2018) 61-68.

DOI: 10.1016/j.cej.2018.02.101

[7] D. Kołodyńska, J. Krukowska, P. Thomas, Comparison of sorption and desorption studies of heavy metal ions from biochar and commercial active carbon, Chem. Eng. J. 307 (2017) 353-363.

DOI: 10.1016/j.cej.2016.08.088

[8] L.G. Ching, S. Sumathi, J.K. Mohammed, A. Waseem, Adsorptive behaviour of palm oil mill sludge biochar pyrolyzed at low temperature for copper and cadmium removal, J. Environ. Manage. 237 (2019) 281-288.

DOI: 10.1016/j.jenvman.2018.12.103

[9] X. Wei, X.Y. Zhang, J.J. Chen, W.X. Zou, F. He, X. Hu, C.W. Daniel, Y. S.O. Tsang, B. Gao, Biochar technology in wastewater treatment: A critical review, Chemosphere. 252 (2020) 126539.

DOI: 10.1016/j.chemosphere.2020.126539

[10] Z.X. Xiao, L.J. Zhang, L. Wu, D. Chen, Adsorptive removal of Cu(II) from aqueous solutions using a novel macroporous bead adsorbent based on poly(vinyl alcohol)/sodium alginate/KMnO4 modified biochar, J. Taiwan. Inst. Chem. E. 102 (2019) 110-117.

DOI: 10.1016/j.jtice.2019.05.010

[11] Y.M. Hao, M. Chen, Z.B. Hu, Effective removal of Cu (II) ions from aqueous solution by amino-functionalized magnetic nanoparticles, J. Hazard. Mater. 184 (2010) 392-399.

DOI: 10.1016/j.jhazmat.2010.08.048

[12] V. Antochshuk, M. Jaroniec, 1-Allyl-3-propylthiourea modified mesoporous silica for mercury removal, Chem. Commun. (2002) 258-259.

DOI: 10.1039/b108789d

[13] Y.M. Ren, X.Z. Wei, M.L. Zhang, Adsorption character for removal Cu(II) by magnetic Cu(II) ion imprinted composite adsorbent, J. Hazard. Mater. 158 (2008) 14-22.

DOI: 10.1016/j.jhazmat.2008.01.044

[14] Y.W. Chen, J.L. Wang, Preparation and characterization of magnetic chitosan nanoparticles and its application for Cu(II) removal, Chem. Eng. J. 168 (2011) 286-292.

[15] O. Ozay, S. Ekici, Y. Baran, N. Aktas, N. Sahiner, Removal of toxic metal ions with magnetic hydrogels, Water. Res. 43 (2009) 4403-4411.

DOI: 10.1016/j.watres.2009.06.058

[16] P. Lu, Y.H. Chen, F.W. Wang, Synthesis of nanostructured M/Fe3O4 (M = Ag, Cu) composites using hexamethylentetramine and their electrocatalytic properties, Mater. Chem. Phys. 134 (2012) 177-182.

DOI: 10.1016/j.matchemphys.2012.02.048

[17] D. Wan, W.B. Li, G.H. Wang, L.L. Lu, X.B. Wei, Degradation of p-Nitrophenol using magnetic Fe0/Fe3O4/Coke composite as a heterogeneous Fenton-like catalyst, Sci. Total. Environ. 574 (2017) 1326-1334.

DOI: 10.1016/j.scitotenv.2016.08.042

[18] W.J. Han, X.Z. Shao, Q. Zhang, G.H. Tian, Preparation of mesoporous magnetic Fe2O3, nanoparticle and its application for organic dyes removal, J. Mol. Liq. 248 (2017) 13-18.

DOI: 10.1016/j.molliq.2017.10.026

[19] Z.G. Liu, F.S. Zhang, Removal of copper (II) and phenol from aqueous solution using porous carbons derived from hydrothermal chars, Desalination. 267 (2010) 101-106.

DOI: 10.1016/j.desal.2010.09.013

[20] K. Kadirvelu, K. Thamaraiselvi, C. Namasivayam, Removal of heavy metals from industrial wastewaters by adsorption onto activated carbon prepared from an agricultural solid waste, Bioresour. Technol. 76 (2001) 63–65.

DOI: 10.1016/s0960-8524(00)00072-9

[21] K. Kadirvelu, P. Senthilkumar, K. Thamaraiselvi, V. Subburam, Activated carbon prepared from biomass as adsorbent: elimination of Ni(II) from aqueous solution, Bioresour. Technol. 81 (2001) 87–90.

DOI: 10.1016/s0960-8524(01)00093-1

[22] M. Zakaria, S.B. Salima, L. Noureddine, E. Abdelhamid, Magnetic monolithic polymers prepared from high internal phase emulsions and Fe3O4 triazole-functionalized nanoparticles for Pb2+, Cu2+ and Zn2+ removal, React. Funct. Polym. 155 (2020) 104693.

DOI: 10.1016/j.reactfunctpolym.2020.104693

[23] A.I.A. Sherlala, A.A.A. Raman, M.M. Bello, A. Asghar, A review of the applications of organo-functionalized magnetic graphene oxide nanocomposites for heavy metal adsorption, Chemosphere. 193 (2018) 1004-1017.

DOI: 10.1016/j.chemosphere.2017.11.093

[24] S. Guo, G.K. Zhang, Y.D. Guo, J.C. Yu, Graphene oxide–Fe2O3 hybrid material as highly efficient heterogeneous catalyst for degradation of organic contaminants, Carbon. 60 (2013) 437-444.

DOI: 10.1016/j.carbon.2013.04.058

[25] Z. Liang, W.C. Xu, L.M. Chen, Degradation of phenol using Fe3O4-GO nanocomposite as a heterogeneous photo-fenton catalyst, Sep. Purif. Technol. 171 (2016) 80-87.

DOI: 10.1016/j.seppur.2016.07.020

[26] M.D. Rajesh, R.M. Pratap, S.R. Sadhana, A.G. Bhole, S.D. Ashwinkumar, R.D. Shubham, Removal of arsenic(III) from water by magnetic binary oxide particles(MBOP): Experimental studies on fixed bed column, J. Hazard. Mater. 322 (2016) 469-478.

DOI: 10.1016/j.jhazmat.2016.09.075

[27] Q.Q. Peng, Y.G. Liu, G.M. Zeng, W.H. Xu, C.P. Yang, J.J. Zhang, Biosorption of copper(II) by immobilizing Saccharomyces cerevisiae on the surface of chitosancoated magnetic nanoparticles from aqueous solution, J. Hazard. Mater. 177 (2010) 676-682.

DOI: 10.1016/j.jhazmat.2009.12.084

[28] T. Huang, J. Dai, J.H. Yang, N. Zhang, Y. Wang, Z.W. Zhou, Polydopamine coated graphene oxide aerogels and their ultrahigh adsorption ability, Diam. Relat. Mater. 86 (2018) 117-127.

DOI: 10.1016/j.diamond.2018.04.015

[29] Y. Zhu, W.H. Fan, T.T. Zhou, X.M. Li, Removal of chelated heavy metals from aqueous solution: A review of current methods and mechanisms. Sci. Total. Environ. 678 (2019) 253-266.

DOI: 10.1016/j.scitotenv.2019.04.416

[30] A.E. Burakov, E.V. Galunin, I.V. Burakova, A.E. Kucherova, A. Shilpi, A.G. Tkachev, V.K. Gupta, Adsorption of heavy metals on conventional and nanostructured materials for wastewater treatment purposes: A review, Ecotox. Environ. Safe. 148 (2018) 702-712.

DOI: 10.1016/j.ecoenv.2017.11.034

[31] P.T.L. Huong, T.V. Son, V.N. Pham, L.T. Tam, A.T. Le, Microstructure and Chemo-Physical characterizations of functional graphene oxide-iron oxide-silver ternary nanocomposite synthesized by one-pot hydrothermal method, J. Nanosci. Nanotechnol. 18 (2018) 5591-5599.

DOI: 10.1166/jnn.2018.15406

[32] M.C. Liu, T. Wen, C.L. Chen, J. Hu, J. Li, X.K. Wang, Synthesis of porous Fe3O4 hollow microspheres/graphene oxide composite for Cr(VI) removal, Dalton. T. 42 (2013) 14710-14717.

DOI: 10.1039/c3dt50955a

[33] U. Jinendra, D. Bilehal, B.M. Nagabhushana, K.S.J. Kumara, S.P. Kollur, Nano-catalytic behavior of highly efficient and regenerable mussel-inspired Fe3O4@CFR@GO and Fe3O4@CFR@TiO2 magnetic nanospheres in the reduction of Evans blue dye, Heliyon. 7 (2021) 6070-6079.

DOI: 10.1016/j.heliyon.2021.e06070

[34] L. Sun, F. Bunshi, Mass production of graphene oxide from expanded graphite, Mater. Lett. 109 (2013) 1227-1233.

[35] Y.F. Liu, Y.Y. Li, X. Zhao, W.D. Chi, C.Y. Yu, Y. Xiang, Effect of magnetite nanoparticles on dye absorption properties of magnetite@carbon composites, B. Mater. Sci. 40 (2017) 367-373.

DOI: 10.1007/s12034-017-1380-6

[36] T. Mayr, D. Wencel, T. Werner, Fluorimetic determination of copper(II) in aqueous solution using lucifer yellow CH as selective metal reagent, Fresenius J Anal Chem. 60 (2001) 156-162.

DOI: 10.1007/s002160100891

[37] C. Bing, K.G. Ngoh, S.C. Lian, Determination of copper by zeolite molecular sieve modified electrode, Electrochimca Acta. 42 (1997) 595-604.

DOI: 10.1016/s0013-4686(96)00204-6

[38] J.J. Pinto, C. Moreno, M.G. Vargas, A simple and very sensitive spectrophotometric method for the direct determination of copper ions, Anal Bioanal Chem. 373 (2002) 844-848.

DOI: 10.1007/s00216-002-1403-y

[39] M. Darj, E.R. Malinowski, Determination of the formation constant of the copper chelate of beta-cyclodextrin by spectrophotometric titration with ethylenediaminetetraacetic acid using window factor analysis, Appl Spectrosc. 56 (2002) 257-265.

DOI: 10.1366/0003702021954520

[40] K. Fujimura, T. Odake, H. Takiguchi, N. Watanabe, T. Sawada, Flow injection spectrophotometric determination of sub-mg dm-3 silver(I) in a strongly acidic solution containing concentrated copper(II) using a pyridylazo reagent, Anal Sci. 27 (2012) 1197-1201.

DOI: 10.2116/analsci.27.1197

[41] M.W. Liu, Z.Z. Jia, Y.F. Liu, High catalytic activity of Fe3-xCuxO4/graphene oxide (0≤x≤0.1) nanocomposites as heterogeneous Fenton catalysts for p-nitrophenol degradation, Water. Air. Soil. Pollut. 230 (2019) 64-79.

DOI: 10.1007/s11270-019-4121-1

[42] L.H. Ai, C.Y. Zhang, Z.L. Chen, Removal of methylene blue from aqueous solution by a solvothermal-synthesized graphene/magnetite composite, J. Hazard. Mater. 192 (2011) 1515-1524.

DOI: 10.1016/j.jhazmat.2011.06.068

[43] J.Z. Wang, C. Zhong, D. Wexler, N.H. Idris, Z.X. Wang, L.Q. Chen, H.K. Liu, Graphene-Encapsulated Fe3O4 nanoparticles with 3D laminated structure as superior anode in lithium ion batteries, Eur. J. Med. Chem. 17 (2011) 661–667.

DOI: 10.1002/chem.201001348

[44] G.Y. He, W.F. Liu, X.Q. Sun, Q. Chen, X. Wang, H.Q. Chen, Fe3O4@graphene oxide composite: A magnetically separable and efficient catalyst for the reduction of nitroarenes, Mater. Res. Bull. 48 (2013) 1885–1890.

DOI: 10.1016/j.materresbull.2013.01.038

[45] X.C. Sun, A. Gutierrez, M.J. Yacaman, X.L. Dong, S.R. Jin, Investigations on magnetic properties and structure for carbon encapsulated nanoparticles of Fe, Co, Ni, Mater. Sci. Eng., A. 286 (2000) 157-160.

DOI: 10.1016/s0921-5093(00)00628-6

[46] P.J.F. Harris, S.C. Tsang, A simple technique for the synthesis of filled carbon nanoparticles, Chem. Phys. Lett. 293 (1998) 53-58.

[47] Y. Lu, Z.P. Zhu, Z.Y. Liu, Carbon-encapsulated Fe nanoparticles from detonation-induced pyrolysis of ferrocene, Carbon. 43 (2005) 369-374.

DOI: 10.1016/j.carbon.2004.09.020

[48] B. Ali, S. Aamer, S. Muhammad, I. Shahid, I.B. Muhammad, W. Muhammad, N.H. Muhammad, A. Nasir, Eco-friendly synthesis of magnetite (Fe3O4) nanoparticles with tunable size: Dielectric, magnetic, thermal and optical studies, Mater. Chem. Phys. 198 (2017) 229–235.

[49] M.Z. Kassaee, E. Motamedi, M. Majdi, Magnetic Fe3O4-graphene oxide/polystyrene: Fabrication and characterization of a promising nanocomposite, Chem. Eng. J. 172 (2011) 540-549.

DOI: 10.1016/j.cej.2011.05.093

[50] X.J. Zhu, Y.W. Zhu, S. Murali, M.D. Stoller, R.S. Ruoff, Nanostructured reduced graphene oxide/Fe2O3 composite as a high-performance anode material for lithium ion batteries, ACS Nano. 5 (2011) 3333-3338.

DOI: 10.1021/nn200493r

[51] G.K. Zhang, Y.Y. Gao, Y.L. Zhang, Y.D. Guo, Fe2O3-pillared rectorite as an efficient and stable Fenton-Like Heterogeneous catalyst for photodegradation of organic contaminants, Environ. Sci. Technol. 44 (2010) 6384-6389.

DOI: 10.1021/es1011093

[52] A. Amini, M. Khajeh, A.R. Oveisi, S. Daliran, M.M. Ghaffari, H.S. Delarami, A porous multifunctional and magnetic layered graphene oxide/3D mesoporous MOF nanocomposite for rapid adsorption of uranium(VI) from aqueous solutions, J. Ind. Eng. Chem. 93 (2020) 322-332.

DOI: 10.1016/j.jiec.2020.10.008

[53] W.J. Zhang, Q.C. Feng, B.B. Zhang, Y.L. Wang, Y.L. Fei, M. Kou, Z.X. Zhang, Y.Y. Shen, X.Y. Du, Nitrogen-Doped mesoporous carbons bearing Fe3O4 as adsorbent for effective Ag(I) removal, Nano. 15 (2020) 13.

DOI: 10.1142/s1793292020501349

[54] A. Gisya, A. Abdolhamid, A. Jhaleh, R. Soraya, S. Gaurav, Polyamine-modified magnetic graphene oxide surface: Feasible adsorbent for removal of dyes, J. Mol. Liq. 289 (2019) 111118.

DOI: 10.1016/j.molliq.2019.111118

[55] Z.H. Lu, Z.Q. Hao, J. Wang, L. Chen, Efficient removal of europium from aqueous solutions using attapulgite-iron oxide magnetic composites, J. Ind. Eng. Chem. 34 (2015) 374-381.

DOI: 10.1016/j.jiec.2015.12.013

[56] J. Hu, M.C.L. Irene, G.H. Chen, Comparative study of various magnetic nanoparticles for Cr(VI) removal, Sep. Purif. Technol. 56 (2007) 249-256.

[57] N.A. Zubir, C. Yacou, J. Motuzas, X.W. Zhang, C.J.C. Diniz, Structural and functional investigation of graphene oxide-Fe3O4 nanocomposites for the heterogeneous Fenton-like reaction, Sci. Rep. 4 (2014) 101-104.

DOI: 10.1038/srep04594

[58] T.L. Hou, L.G. Yan, J. Li, Y.T. Yang, L.X. Shan, X. Meng, X.G. Li, Y.X. Zhao, Adsorption performance and mechanistic study of heavy metals by facile synthesized magnetic layered double oxide/carbon composite from spent adsorbent, Chem. Eng. J. 384 (2020) 123331.

DOI: 10.1016/j.cej.2019.123331

[59] H.J. Zhang, Q. Chang, Y. Jiang, H.L. Li, Y.H. Yang, Synthesis of KMnO4-treated magnetic graphene oxide nanocomposite (Fe3O4@GO/MnOx) and its application for removing of Cu2+ ions from aqueous solution, Nanotechnology. 29 (2018) 135706.

DOI: 10.1088/1361-6528/aaaa2f

[60] Y.C. Wu, G.P. Jiang, Z.P. Cano, G.H. Liu, W.W. Liu, K. Feng, G. Lui, Z.S. Zhang, Z.W. Chen, Highly efficient removal of suspended solid pollutants from wastewater by magnetic Fe3O4-Graphene oxides nanocomposite. Chemistry. Sel. 3 (2018) 11643-11648.

DOI: 10.1002/slct.201802148

[61] L. Yu, J.D. Chen, Z. Liang, W.C. Xu, L.M. Chen, D.Q. Ye, Degradation of phenol using Fe3O4-GO nanocomposite as a heterogeneous photo-fenton catalyst, Sep. Purif. Technol. 171 (2016) 80-87.

DOI: 10.1016/j.seppur.2016.07.020

[62] Y.F. Lin, H.W. Chen, K.L. Lin, B.Y. Chen, C. Chiou, Application of magnetic particles modified with amino groups to adsorb copper ions in aqueous solution, J. Environ. Sci. 23 (2011) 44-50.

DOI: 10.1016/s1001-0742(10)60371-3