Removal and recovery of toxic nanosized Cerium Oxide using eco-friendly Iron Oxide Nanoparticles

Highlights

• Eco-friendly IONPs were synthesized through solvothermal method.

• IONPs show very high removal efficiency for CeO₂ NPs i.e. 688 mg/g.

• Removal was >90% in all synthetic and real water samples.

• >80% recovery of CeO₂ NPs through sonication confirms reusability of IONPs.

Abstract

Increasing applications of metal oxide nanoparticles and their release in the natural environment is a serious concern due to their toxic nature. Therefore, it is essential to have eco-friendly solutions for the remediation of toxic metal oxides in an aqueous environment. In the present study, eco-friendly Iron Oxide Nanoparticles (IONPs) are synthesized using solvothermal technique and successfully characterized using scanning and transmission electron microscopy (SEM and TEM respectively) and powder X-Ray diffraction (PXRD). These IONPs were further utilized for the remediation of toxic metal oxide nanoparticle, i.e., CeO₂. Sorption experiments were also performed in complex aqueous solutions and real water samples to check its applicability in the natural environment. Reusability study was performed to show cost-effectiveness. Results show that these 200 nm-sized spherical IONPs, as revealed by SEM and TEM analysis, were magnetite (Fe₃O₄) and contained short-range crystallinity as confirmed from XRD spectra. Sorption experiments show that the composite follows the pseudo-second-order kinetic model. Further R²>0.99 for Langmuir sorption isotherm suggests chemisorption as probable removal mechanism with monolayer sorption of CeO₂ NPs on IONP. More than 80% recovery of adsorbed CeO₂ NPs through ultrasonication and magnetic separation of reaction precipitate confirms reusability of IONPs. Obtained removal % of CeO₂ in various synthetic and real water samples was>90% signifying that IONPs are candidate adsorbent for the removal and recovery of toxic metal oxide nanoparticles from contaminated environmental water samples.

Graphical abstract

Keywords

Adsorption / toxic metal oxide remediation / eco-friendly IONP / Iron oxide / CeO₂ removal

References

[1] Ali A, Zafar H, Zia M, Ul Haq I, Phull A R, Ali J S, Hussain A (2016). Synthesis, characterization, applications, and challenges of iron oxide nanoparticles. Nanotechnology, Science and Applications, 9: 49–67

[2] Chang M R, Lee D J, Lai J Y (2007). Nanoparticles in wastewater from a science-based industrial park: Coagulation using polyaluminum chloride. Journal of Environmental Management, 85(4): 1009–1014

[3] Chen Y, Bylaska E J, Weare J H (2017). Weakly bound water structure, bond valence saturation and water dynamics at the goethite (100) surface/aqueous interface: ab initio dynamical simulations. Geochemical Transactions, 18(1): 3

[4] Chien S H, Clayton W R, Mcclellan G H (1980). Kinetics of dissolution of phosphate rocks in soils. Soil Science Society of America Journal, 44(2): 260–264

[5] Darbha G K, Fischer C, Luetzenkirchen J, Schäfer T (2012). Site-specific retention of colloids at rough rock surfaces. Environmental Science & Technology, 46(17): 9378–9387

[6] Darbha G K, Schäfer T, Heberling F, Lüttge A, Fischer C (2010). Retention of latex colloids on calcite as a function of surface roughness and topography. Langmuir, 26(7): 4743–4752

[7] Darbha G K, Singh A K, Rai U S, Yu E, Yu H, Chandra Ray P (2008). Selective detection of mercury (II) ion using nonlinear optical properties of gold nanoparticles. Journal of the American Chemical Society, 130(25): 8038–8043

[8] Deng Y, Qi D, Deng C, Zhang X, Zhao D (2008). Superparamagnetic high-magnetization microspheres with an Fe₃O₄@SiO₂ core and perpendicularly aligned mesoporous SiO₂ shell for removal of microcystins. Journal of the American Chemical Society, 130(1): 28–29

[9] Dvořák F, Szabová L, Johánek V, Farnesi Camellone M, Stetsovych V, Vorokhta M, Tovt A, Skála T, Matolínová I, Tateyama Y, Mysliveček J, Fabris S, Matolín V (2018). Bulk hydroxylation and effective water splitting by highly reduced cerium oxide: The role of O vacancy coordination. ACS Catalysis, 8(5): 4354–4363

[10] Gan G, Liu J, Zhu Z, Yang Z, Zhang C, Hou X (2017). A novel magnetic nanoscaled Fe₃O₄/CeO₂ composite prepared by oxidation-precipitation process and its application for degradation of orange G in aqueous solution as Fenton-like heterogeneous catalyst. Chemosphere, 168: 254–263

[11] Ganesh R, Smeraldi J, Hosseini T, Khatib L, Olson B H, Rosso D (2010). Evaluation of nanocopper removal and toxicity in municipal wastewaters. Environmental Science & Technology, 44(20): 7808–7813

[12] Gunawan C, Lord M S, Lovell E, Wong R J, Jung M S, Oscar D, Mann R, Amal R (2019). Oxygen-vacancy engineering of cerium-oxide nanoparticles for antioxidant activity. Acs Omega, 4(5): 9473–9479

[13] He Q G, Liu J, Liang J, Liu X P, Ding Z Y, Tuo D, Li W (2018). Sodium acetate orientated hollow/mesoporous magnetite nanoparticles: Facile synthesis, characterization and formation mechanism. Applied Sciences-Basel, 8(2): 10.3390/app8020292 

[14] Ho Y S, Mckay G (1999). Pseudo-second order model for sorption processes. Process Biochemistry, 34(5): 451–465

[15] Hua M, Zhang S, Pan B, Zhang W, Lv L, Zhang Q (2012). Heavy metal removal from water/wastewater by nanosized metal oxides: A review. Journal of Hazardous Materials, 211– 212: 317–331

[16] Juganson K, Ivask A, Blinova I, Mortimer M, Kahru A (2015). NanoE-Tox: New and in-depth database concerning ecotoxicity of nanomaterials. Beilstein Journal of Nanotechnology, 6: 1788–1804

[17] Kaegi R (2009). Nanoparticles in drinking water. EAWAG News, 66

[18] Khandelwal N, Singh N, Tiwari E, Darbha G K (2019). Novel synthesis of a clay supported amorphous aluminum nanocomposite and its application in removal of hexavalent chromium from aqueous solutions. RSC Advances, 9(20): 11160–11169

[19] Kumari M, Singh S P, Chinde S, Rahman M F, Mahboob M, Grover P (2014). Toxicity study of cerium oxide nanoparticles in human neuroblastoma cells. International Journal of Toxicology, 33(2): 86–97

[20] Langmuir I (1918). The adsorption of gases on plane surfaces of glass, mica and platinum. Journal of the American Chemical Society, 40(9): 1361–1403

[21] Largitte L, Pasquier R (2016). A review of the kinetics adsorption models and their application to the adsorption of lead by an activated carbon. Chemical Engineering Research & Design, 109: 495–504

[22] Lin W, Huang Y W, Zhou X D, Ma Y (2006). Toxicity of cerium oxide nanoparticles in human lung cancer cells. International Journal of Toxicology, 25(6): 451–457

[23] Lin Y T, Sung M, Sanders P F, Marinucci A, Huang C P (2007). Separation of nano-sized colloidal particles using cross-flow electro-filtration. Separation and Purification Technology, 58(1): 138–147

[24] Liu J F, Sun J, Jiang G B (2010). Use of cloud point extraction for removal of nanosized copper oxide from wastewater. Chinese Science Bulletin, 55(4–5): 346–349

[25] Masserini M (2013). Nanoparticles for brain drug delivery. ISRN Biochemistry, 2013: 238428–238428

[26] Morales M I, Rico C M, Hernandez-Viezcas J A, Nunez J E, Barrios A C, Tafoya A, Flores-Marges J P, Peralta-Videa J R, Gardea-Torresdey J L (2013). Toxicity assessment of cerium oxide nanoparticles in cilantro (Coriandrum sativum L.) plants grown in organic soil. Journal of Agricultural and Food Chemistry, 61(26): 6224–6230

[27] Omar S (2019). Doped ceria for solid oxide fuel cells. Intech Open, Chapter 4:43– 59

[28] Pang L, Liu J F (2013). Use of Fe₃O₄@nSiO₂@mSiO₂ magnetic mesoporous microspheres for fast determination of the sorption coefficients of polycyclic aromatic hydrocarbons to bovine serum albumin in aqueous phase. Acta Chimica Sinica, 71(3): 339–342

[29] Pujar M S, Hunagund S M, Desai V R, Patil S, Sidarai A H (2018). One-step synthesis and characterizations of cerium oxide nanoparticles in an ambient temperature via Co-precipitation method. AIP Conference Proceedings, 1942(1): 050026

[30] Ranjit K, Ahmed A (2013). Nanoparticle: An overview of preparation, characterization, and application. Journal of Applied Pharmaceutical Science, 1(6):228– 234

[31] Sen Gupta S, Bhattacharyya K G (2011). Kinetics of adsorption of metal ions on inorganic materials: A review. Advances in Colloid and Interface Science, 162(1–2): 39–58

[32] Smith E J, Davison W, Hamilton-Taylor J (2002). Methods for preparing synthetic freshwaters. Water Research, 36(5): 1286–1296

[33] Springer F, Laborie S, Guigui C (2013). Removal of SiO₂ nanoparticles from industry wastewaters and subsurface waters by ultrafiltration: Investigation of process efficiency, deposit properties and fouling mechanism. Separation and Purification Technology, 108: 6–14

[34] Srinivas A, Rao P J, Selvam G, Murthy P B, Reddy P N (2011). Acute inhalation toxicity of cerium oxide nanoparticles in rats. Toxicology Letters, 205(2): 105–115

[35] Srivastava S K, Tyagi R, Pant N (1989). Adsorption of heavy-metal ions on carbonaceous material developed from the waste slurry generated in local fertilizer plants. Water Research, 23(9): 1161–1165

[36] Stachowicz M, Hiemstra T, van Riemsdijk W H (2007). Arsenic-bicarbonate interaction on goethite particles. Environmental Science & Technology, 41(16): 5620–5625

[37] Suzuki T, Kosacki I, Anderson H U (2002). Defect and mixed conductivity in nanocrystalline doped cerium oxide. Journal of the American Ceramic Society, 85(6): 1492–1498

[38] Teng W Y, Jeng S C, Kuo C W, Lin Y R, Liao C C, Chin W K (2008). Nanoparticles-doped guest-host liquid crystal displays. Optics Letters, 33(15): 1663–1665

[39] Trovarelli A (1996). Catalytic properties of ceria and CeO₂-containing materials. Catalysis Reviews, 38(4): 439–520

[40] Wiechers J W, Musee N (2010). Engineered inorganic nanoparticles and cosmetics: facts, issues, knowledge gaps and challenges. Journal of Biomedical Nanotechnology, 6(5): 408–431

[41] Xu H, Sun Y, Li J, Li F, Guan X (2016). Aging of zerovalent iron in synthetic groundwater: X-ray photoelectron spectroscopy depth profiling characterization and depassivation with uniform magnetic field. Environmental Science & Technology, 50(15): 8214–8222

[42] Yang S, Zeng T, Li Y, Liu J, Chen Q, Zhou J, Ye Y, Tang B (2015). Preparation of graphene oxide decorated Fe₃O₄@SiO₂ nanocomposites with superior adsorption capacity and SERS detection for organic dyes. Journal of Nanomaterials, 2015: 8

[43] Zachara J M, Girvin D C, Schmidt R L, Resch C T (1987). Chromate adsorption on amorphous iron oxyhydroxide in the presence of major groundwater ions. Environmental Science & Technology, 21(6): 589–594

[44] Zamiri R, Abbastabar Ahangar H, Kaushal A, Zakaria A, Zamiri G, Tobaldi D, Ferreira J M F (2015). Dielectrical properties of CeO₂ nanoparticles at different temperatures. Plos One, 10(4): e0122989

[45] Zargoosh K, Abedini H, Abdolmaleki A, Molavian M R (2013). Effective removal of heavy metal ions from industrial wastes using thiosalicylhydrazide-modified magnetic nanoparticles. Industrial & Engineering Chemistry Research, 52(42): 14944–14954

[46] Zhou X X, Li Y J, Liu J F (2017). Highly efficient removal of silver-containing nanoparticles in waters by aged iron oxide magnetic particles. ACS Sustainable Chemistry & Engineering, 5(6): 5468–5476

Acknowledgements

We recognize financial support from the SERB-Ramanujan Fellowship grant (SB/S2/RJN-006/2016) and SERB-ECR project grant (ECR/2017/000707) from Department of Science and Technology (DST), India. We are also thankful to the Indian Institute of Science Education and Research Kolkata’s central instrumentation facility for TEM, FESEM, and PXRD analysis.

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