Abstract
A 3D flower-shaped bimetallic nanocomposite zirconium magnesium oxide (ZMO) was prepared first time by the controlled solution combustion method using triethanolamine (TEA) as a fuel and chelating agent. The composite material was used to remove excess fluoride via adsorption. The thermal stability of the adsorbent was characterized by thermogravimetric analysis (TGA). Fourier transform infrared spectroscopy (FTIR), field emission scanning electron microscopy (FESEM), energy-dispersive X-ray (EDX), and X-ray diffraction (XRD) were used to characterize the adsorbent. The surface charge of the nano adsorbent was determined by Zeta Sizer. The surface area and pore volume of the adsorbent were determined by Brunauer–Emmett–Teller (BET) isotherm and Barrett-Joyner-Halenda (BJH) methods. The adsorption behavior of fluoride was studied systematically varying the pH, contact time, adsorbent dose, and initial fluoride concentration. The adsorption followed the Langmuir isotherm model with a maximum adsorption capacity of 42.14 mg/g. The pseudo-second-order kinetic model was confirmed by the adsorption study. The maximum adsorption efficiency was in the 6–10 pH range. The reaction mechanism was mainly based on ion exchange between hydroxy and fluoride ions which was proven by X-ray photoelectron spectroscopy (XPS). Real water tests indicated that ZMO could be used as a potential defluoridation agent for fluoride containing groundwater treatment.
This is a preview of subscription content, log in via an institution to check access.
Similar content being viewed by others
Data availability
All authors make sure that all data and materials as well as a software application or custom code support their published claims and comply with field standards.
References
Adak MK, Sen A, Mukherjee A et al (2017) Removal of fluoride from drinking water using highly efficient nano-adsorbent, Al(III)-Fe(III)-La(III) trimetallic oxide prepared by chemical route. J Alloys Compd 719:460–469. https://doi.org/10.1016/j.jallcom.2017.05.149
Araga R, Sharma CS (2019) Amine functionalized electrospun cellulose nanofibers for fluoride adsorption from drinking water. J Polym Environ 27:816–826. https://doi.org/10.1007/s10924-019-01394-2
Chaudhary M, Maiti A (2019) Defluoridation by highly efficient calcium hydroxide nanorods from synthetic and industrial wastewater. Colloids Surfaces A Physicochem Eng Asp 561:79–88. https://doi.org/10.1016/j.colsurfa.2018.10.052
Chigondo M, Paumo HK, Bhaumik M et al (2018) Rapid high adsorption performance of hydrous cerium-magnesium oxides for removal of fluoride from water. J Mol Liq 265:496–509. https://doi.org/10.1016/j.molliq.2018.06.015
Contreras M, Martín MI, Gázquez MJ et al (2014) Valorisation of ilmenite mud waste in the manufacture of commercial ceramic. Constr Build Mater 72:31–40. https://doi.org/10.1016/j.conbuildmat.2014.08.091
Damtie MM, Woo YC, Kim B et al (2019) Removal of fluoride in membrane-based water and wastewater treatment technologies: performance review. J Environ Manage 251:109524. https://doi.org/10.1016/j.jenvman.2019.109524
Delir Kheyrollahi Nezhad P, Haghighi M, Rahmani F (2018) CO2/O2-enhanced ethane dehydrogenation over a sol–gel synthesized Ni/ZrO2–MgO nanocatalyst: effects of Mgo, ZrO2, and NiO on the catalytic performance. Part Sci Technol 36:1017–1028. https://doi.org/10.1080/02726351.2017.1340376
Devi RR, Umlong IM, Raul PK et al (2014) Defluoridation of water using nano-magnesium oxide. J Exp Nanosci 9:512–524. https://doi.org/10.1080/17458080.2012.675522
Durmaz F, Kara H, Cengeloglu Y, Ersoz M (2005) Fluoride removal by donnan dialysis with anion exchange membranes. Desalination 177:51–57. https://doi.org/10.1016/j.desal.2004.11.016
Ezzeddine A, Bedoui A, Hannachi A, Bensalah N (2015) Removal of fluoride from aluminum fluoride manufacturing wastewater by precipitation and adsorption processes. Desalin Water Treat 54:2280–2292. https://doi.org/10.1080/19443994.2014.899515
Gao M, Wang W, Cao M et al (2020) Hierarchical hollow manganese-magnesium-aluminum ternary metal oxide for fluoride elimination. Environ Res 188:109735. https://doi.org/10.1016/j.envres.2020.109735
Gao M, Wang W, Yang H, Ye B-C (2020) Efficient removal of fluoride from aqueous solutions using 3D flower-like hierarchical zinc-magnesium-aluminum ternary oxide microspheres. Chem Eng J 380:122459. https://doi.org/10.1016/j.cej.2019.122459
Gao Y, Li M, Ru Y, Fu J (2021) Fluoride removal from water by using micron zirconia/zeolite molecular sieve: characterization and mechanism. Groundw Sustain Dev 13:100567. https://doi.org/10.1016/j.gsd.2021.100567
Ghosh A, Chakrabarti S, Biswas K, Ghosh UC (2014) Agglomerated nanoparticles of hydrous Ce(IV) + Zr(IV) mixed oxide: preparation, characterization and physicochemical aspects on fluoride adsorption. Appl Surf Sci 307:665–676. https://doi.org/10.1016/j.apsusc.2014.04.095
Gouamid M, Ouahrani MR, Bensaci MB (2013) Adsorption equilibrium, kinetics and thermodynamics of methylene blue from aqueous solutions using date palm leaves. Energy Procedia 36:898–907. https://doi.org/10.1016/j.egypro.2013.07.103
Guan W, Zhao X (2016) Fluoride recovery using porous calcium silicate hydrates via spontaneous Ca2+ and OH− release. Sep Purif Technol 165:71–77. https://doi.org/10.1016/j.seppur.2016.03.050
Hasan R, Bukhari SN, Jusoh R et al (2018) Adsorption of Pb(II) onto KCC-1 from aqueous solution: Isotherm and kinetic study. Mater Today Proc 5:21574–21583. https://doi.org/10.1016/j.matpr.2018.07.006
He Y, Zhang L, An X et al (2019) Enhanced fluoride removal from water by rare earth (La and Ce) modified alumina: adsorption isotherms, kinetics, thermodynamics and mechanism. Sci Total Environ 688:184–198. https://doi.org/10.1016/j.scitotenv.2019.06.175
Hettithanthri O, Rajapaksha AU, Nanayakkara N, Vithanage M (2023) Temperature influence on layered double hydroxide tailored corncob biochar and its application for fluoride removal in aqueous media. Environ Pollut 320:121054. https://doi.org/10.1016/j.envpol.2023.121054
Huang H, Liu J, Zhang P et al (2017) Investigation on the simultaneous removal of fluoride, ammonia nitrogen and phosphate from semiconductor wastewater using chemical precipitation. Chem Eng J 307:696–706. https://doi.org/10.1016/j.cej.2016.08.134
Isinkaralar K (2022) Theoretical removal study of gas BTEX onto activated carbon produced from Digitalis purpurea L. biomass. Biomass Convers Biorefinery 12:4171–4181. https://doi.org/10.1007/s13399-022-02558-2
Isinkaralar K (2023) Experimental evaluation of benzene adsorption in the gas phase using activated carbon from waste biomass. Biomass Convers Biorefinery. https://doi.org/10.1007/s13399-023-03979-3
Isinkaralar K (2023) Comparison of the gaseous benzene adsorption capacity by activated carbons from Fraxinus excelsior L. as a lignocellulosic residual. Chem Pap 77:6111–6124. https://doi.org/10.1007/s11696-023-02925-x
Isinkaralar K, Gullu G, Turkyilmaz A (2023) Experimental study of formaldehyde and BTEX adsorption onto activated carbon from lignocellulosic biomass. Biomass Convers Biorefinery 13:4279–4289. https://doi.org/10.1007/s13399-021-02287-y
Islam M, Patel RK (2007) Evaluation of removal efficiency of fluoride from aqueous solution using quick lime. J Hazard Mater 143:303–310. https://doi.org/10.1016/j.jhazmat.2006.09.030
Jadhao VK, Kodape S, Junghare K (2019) Optimization of electrocoagulation process for fluoride removal: a blending approach using gypsum plaster rich wastewater. Sustain Environ Res 29:6. https://doi.org/10.1186/s42834-019-0002-y
Kong L, Tian Y, Pang Z et al (2020) Needle-like Mg-La bimetal oxide nanocomposites derived from periclase and lanthanum for cost-effective phosphate and fluoride removal: characterization, performance and mechanism. Chem Eng J 382:122963. https://doi.org/10.1016/j.cej.2019.122963
Lacson CFZ, Lu M-C, Huang Y-H (2021) Chemical precipitation at extreme fluoride concentration and potential recovery of CaF2 particles by fluidized-bed homogenous crystallization process. Chem Eng J 415:128917. https://doi.org/10.1016/j.cej.2021.128917
Lei C, Pi M, Xu D et al (2017) Fabrication of hierarchical porous ZnO-Al2O3 microspheres with enhanced adsorption performance. Appl Surf Sci 426:360–368. https://doi.org/10.1016/j.apsusc.2017.07.095
Liu R, Gong W, Lan H et al (2011) Defluoridation by freshly prepared aluminum hydroxides. Chem Eng J 175:144–149. https://doi.org/10.1016/j.cej.2011.09.083
Ma W, Zhao N, Yang G et al (2011) Removal of fluoride ions from aqueous solution by the calcination product of Mg–Al–Fe hydrotalcite-like compound. Desalination 268:20–26. https://doi.org/10.1016/j.desal.2010.09.045
Mahfoudhi N, Boufi S (2020) Porous material from cellulose nanofibrils coated with aluminum hydroxyde as an effective adsorbent for fluoride. J Environ Chem Eng 8:103779. https://doi.org/10.1016/j.jece.2020.103779
Meenakshi MRC, Maheshwari RC (2006) Fluoride in drinking water and its removal. J Hazard Mater 137:456–463. https://doi.org/10.1016/j.jhazmat.2006.02.024
Meenakshi S, Viswanathan N (2007) Identification of selective ion-exchange resin for fluoride sorption. J Colloid Interface Sci 308:438–450. https://doi.org/10.1016/j.jcis.2006.12.032
Minju N, Venkat Swaroop K, Haribabu K et al (2015) Removal of fluoride from aqueous media by magnesium oxide-coated nanoparticles. Desalin Water Treat 53:2905–2914. https://doi.org/10.1080/19443994.2013.868837
Mobarak M, Mohamed EA, Selim AQ et al (2019) Surfactant–modified serpentine for fluoride and Cr(VI) adsorption in single and binary systems: experimental studies and theoretical modeling. Chem Eng J 369:333–343. https://doi.org/10.1016/j.cej.2019.03.086
Mullick A, Neogi S (2019) Ultrasound assisted synthesis of Mg-Mn-Zr impregnated activated carbon for effective fluoride adsorption from water. Ultrason Sonochem 50:126–137. https://doi.org/10.1016/j.ultsonch.2018.09.010
Mureth R, Machunda R, Njau KN, Dodoo-Arhin D (2021) Assessment of fluoride removal in a batch electrocoagulation process: a case study in the Mount Meru Enclave. Sci African 12:e00737. https://doi.org/10.1016/j.sciaf.2021.e00737
Na C-K, Park H-J (2010) Defluoridation from aqueous solution by lanthanum hydroxide. J Hazard Mater 183:512–520. https://doi.org/10.1016/j.jhazmat.2010.07.054
Nehra S, Raghav S, Kumar D (2020) Biomaterial functionalized cerium nanocomposite for removal of fluoride using central composite design optimization study. Environ Pollut 258:113773. https://doi.org/10.1016/j.envpol.2019.113773
Panda B, Mondal D, Mandal S et al (2022) One-pot solution combustion synthesis of porous spherical-shaped magnesium zinc binary oxide for efficient fluoride removal and photocatalytic degradation of methylene blue and Congo red dye. Environ Sci Pollut Res. https://doi.org/10.1007/s11356-022-22551-6
Patel SB, Baker N, Marques I et al (2017) Transparent TiO2 nanotubes on zirconia for biomedical applications. RSC Adv 7:30397–30410. https://doi.org/10.1039/c7ra03940a
Prabhu SM, Meenakshi S (2015) Novel one-pot synthesis of dicarboxylic acids mediated alginate-zirconium biopolymeric complex for defluoridation of water. Carbohydr Polym 120:60–68. https://doi.org/10.1016/j.carbpol.2014.11.058
Raghav S, Kumar D (2019) Comparative kinetics and thermodynamic studies of fluoride adsorption by two novel synthesized biopolymer composites. Carbohydr Polym 203:430–440. https://doi.org/10.1016/j.carbpol.2018.09.054
Sarma GK, Rashid MH (2018) Synthesis of Mg/Al layered double hydroxides for adsorptive removal of fluoride from water: a mechanistic and kinetic study. J Chem Eng Data 63:2957–2965. https://doi.org/10.1021/acs.jced.8b00242
Shao S, Ma B, Chen Y et al (2021) Behavior and mechanism of fluoride removal from aqueous solutions by using synthesized CaSO4·2H2O nanorods. Chem Eng J 426:131364. https://doi.org/10.1016/j.cej.2021.131364
Subramanyam B, Das A (2014) Linearised and non-linearised isotherm models optimization analysis by error functions and statistical means. J Environ Heal Sci Eng 12:1–6. https://doi.org/10.1186/2052-336X-12-92
Swain SK, Patnaik T, Singh VK et al (2011) Kinetics, equilibrium and thermodynamic aspects of removal of fluoride from drinking water using meso-structured zirconium phosphate. Chem Eng J 171:1218–1226. https://doi.org/10.1016/j.cej.2011.05.030
Thakre D, Rayalu S, Kawade R et al (2010) Magnesium incorporated bentonite clay for defluoridation of drinking water. J Hazard Mater 180:122–130. https://doi.org/10.1016/j.jhazmat.2010.04.001
Tkalčec E, Popović J, Orlić S et al (2014) Hydrothermal synthesis and thermal evolution of carbonate-fluorhydroxyapatite scaffold from cuttlefish bones. Mater Sci Eng C 42:578–586. https://doi.org/10.1016/j.msec.2014.05.079
Wang J, Kang D, Yu X et al (2015) Synthesis and characterization of Mg-Fe-La tri-metal composite as an adsorbent for fluoride removal. Chem Eng J 264:506–513. https://doi.org/10.1016/j.cej.2014.11.130
Wang X, Pfeiffer H, Wei J et al (2022) 3D porous Ca-modified Mg-Zr mixed metal oxide for fluoride adsorption. Chem Eng J 428:131371. https://doi.org/10.1016/j.cej.2021.131371
Wen Z, Ke J, Xu J et al (2018) One-step facile hydrothermal synthesis of flowerlike Ce/Fe bimetallic oxides for efficient As(V) and Cr(VI) remediation: performance and mechanism. Chem Eng J 343:416–426. https://doi.org/10.1016/j.cej.2018.03.034
Wu X, Zhang Y, Dou X et al (2013) Fluoride adsorption on a Fe-Al-Ce trimetal hydrous oxide: characterization of adsorption sites and adsorbed fluorine complex species. Chem Eng J 223:364–370. https://doi.org/10.1016/j.cej.2013.03.027
Xia Y, Huang X, Li W et al (2019) Facile defluoridation of drinking water by forming shell@fluorapatite nanoarray during boiling egg shell. J Hazard Mater 361:321–328. https://doi.org/10.1016/j.jhazmat.2018.09.007
Xiang W, Zhang G, Zhang Y et al (2014) Synthesis and characterization of cotton-like Ca-Al-La composite as an adsorbent for fluoride removal. Chem Eng J 250:423–430. https://doi.org/10.1016/j.cej.2014.03.118
Xu J, Deng H, Song J et al (2017) Synthesis of hierarchical flower-like Mg2Al-Cl layered double hydroxide in a surfactant-free reverse microemulsion. J Colloid Interface Sci 505:816–823. https://doi.org/10.1016/j.jcis.2017.06.080
Yang Y, Dang L, Shearer MJ et al (2018) Highly active trimetallic NiFeCr layered double hydroxide electrocatalysts for oxygen evolution reaction. Adv Energy Mater 8:1703189. https://doi.org/10.1002/aenm.201703189
Yousefi M, Gholami M, Oskoei V et al (2021) Comparison of LSSVM and RSM in simulating the removal of ciprofloxacin from aqueous solutions using magnetization of functionalized multi-walled carbon nanotubes: process optimization using GA and RSM techniques. J Environ Chem Eng 9:105677. https://doi.org/10.1016/j.jece.2021.105677
Yu S, Yin L, Pang H et al (2018) Constructing sphere-like cobalt-molybdenum-nickel ternary hydroxide and calcined ternary oxide nanocomposites for efficient removal of U(VI) from aqueous solutions. Chem Eng J 352:360–370. https://doi.org/10.1016/j.cej.2018.07.033
Zhang K, Wu S, Wang X et al (2015) Wide pH range for fluoride removal from water by MHS-MgO/MgCO3 adsorbent: kinetic, thermodynamic and mechanism studies. J Colloid Interface Sci 446:194–202. https://doi.org/10.1016/j.jcis.2015.01.049
Zhang Y, Xu G-S, Xu M-D et al (2021) Preparation of MgO porous nanoplates modified pumice and its adsorption performance on fluoride removal. J Alloys Compd 884:160953. https://doi.org/10.1016/j.jallcom.2021.160953
Funding
The authors are grateful to the Department of Science and Technology (DST) for its financial support (DST STI HUB Project Sanction letter No – SEED/TITE/2019/84) and DST FIST, Govt. of India via Project Sanction Letter No. SR/FST/CS-I/2022/247 dated December 19, 2022, for infrastructural support.
Author information
Authors and Affiliations
Contributions
Supriya Mandal and Bholanath Panda contributed to the study conception, design, material preparation, data collection, and analysis. Debasish Mondal performed the SEM analysis. Julekha Khatun performed the XPS analysis. Prasanta Dhak performs the XRD analysis. The concept and overall supervising of the work as well as preparing the manuscript were carried out by Dr. Debasis Dhak. All authors read and approved the final manuscript.”
Corresponding author
Ethics declarations
Consent to participate
Not applicable.
Consent for publication
Authors will be asked to transfer the copyright of the article to the publisher.
Competing interests
The authors declare no competing interests.
Research involving human participants and/or animals
No human participants and /or animals were involved in this research.
Additional information
Responsible Editor: Tito Roberto Cadaval Jr
Publisher's Note
Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
Both the authors contributed equally and both are to be treated as first authors.
Rights and permissions
Springer Nature or its licensor (e.g. a society or other partner) holds exclusive rights to this article under a publishing agreement with the author(s) or other rightsholder(s); author self-archiving of the accepted manuscript version of this article is solely governed by the terms of such publishing agreement and applicable law.
About this article
Cite this article
Mandal, S., Panda, B., Mondal, D. et al. 3D flower-like zirconium magnesium oxide nanocomposite for efficient fluoride removal. Environ Sci Pollut Res 30, 119491–119505 (2023). https://doi.org/10.1007/s11356-023-30704-4
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1007/s11356-023-30704-4