Abstract
Using groundwater for human consumption is an alternative for places with no nearby surface water resources. Fluoride is commonly found in groundwater, and the consumption of this water for a prolonged time in concentrations that exceed established limits by WHO and Brazilian legislation on water potability (1.5 mg L−1) can cause harmful problems to human health. For this reason, fluoride removal is an important step before water consumption. In this work, activated alumina was impregnated with Fe-Al-La composite and employed for the first time as an adsorbent for fluoride removal from an aqueous environment. XRD, SEM/EDS, FT-IR, and point of zero charge were used to characterize the prepared adsorbent. The adsorptive performance of adsorbent material was investigated by employing a 23-central composite design (CCD), and the obtained experimental conditions were pH = 6.5 and adsorbent dosage = 3.0 g L−1. A maximum adsorption capacity of 8.17 mg g−1 at 298 K and pH = 6.5 was achieved by Langmuir isotherm to describe the adsorption. The kinetic model that better described experimental data was Avrami, with the kav parameter increasing with the initial concentration from 0.076 to 0.231 (min−1)nav. The nature of adsorption was found to be homogeneous, and it occurs in a monolayer. The fluoride removal performance for the prepared adsorbent was higher than granular activated alumina, showing that supporting Fe-Al-La at the alumina surface increased its fluoride adsorption capacity from 16 to 42% at the same experimental conditions. Finally, the influence of co-existing ions Cl−, SO42−, and NO3− was evaluated in fluoride adsorption, and the material presented great selectivity to fluoride. Thus, Fe-Al-La/AA adsorbent is a promising material for fluoride removal from water.
Graphical Abstract
Similar content being viewed by others
Data availability
The datasets used and analyzed during the current study are available from the corresponding author upon reasonable request.
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
Awual MR, Hossain MA, Shenashen MA, Yaita T, Suzuki S, Jyo A (2012) Evaluating of arsenic(V) removal from water by weak-base anion exchange adsorbents. Environ Sci Pollut Res 20:421–430 (https://link.springer.com/article/10.1007/2Fs11356-012-0936-7)
Awual MdR, Hossain A, Shenashen MA, Yata T, Suzuki S, Jyo A (2013) Evaluating of arsenic(V) removal from water by weak-base anion exchange adsorbents. Environ Sci Pollut Res 20:421–430 (https://link.springer.com/article/10.1007/s11356-012-0936-7)
Bansiwal A, Pillewan P, Biniwale RB, Rayalu SS (2010) Copper oxide incorporated mesoporous alumina for defluoridation of drinking water. Micropor Mesopor Mater 129:54–61. https://doi.org/10.1016/j.micromeso.2009.08.032
Chai L, Wang Y, Zhao N et al (2013) Sulfate-doped Fe3O4/Al2O3 nanoparticles as a novel adsorbent for fluoride removal from drinking water. Water Res 47:4040–4049. https://doi.org/10.1016/j.watres.2013.02.057
Chang MF, Liu JC (2007) Precipitation removal of fluoride from semiconductor wastewater. J Environ Eng 133:419–425. https://doi.org/10.1061/(asce)0733-9372(2007)133:4(419)
Chen T, Yu K, Dong C et al (2022a) Advanced photocatalysts for uranium extraction: elaborate design and future perspectives. Coord Chem Rev 467:214–615. https://doi.org/10.1016/j.apcatb.2022.121815
Chen T, Lui T, Zhou L et al (2022b) Ternary boron carbon nitrides hollow nanotubes with tunable p-n homojunction for photo-assisted uranium extraction: a combined batch, EXAFS and DFT calculations. Appl Catal B: Environmental 318:121–815. https://doi.org/10.1016/j.ccr.2022.214615
Cheng J, Meng X, Jing C, Hao J (2014) La3+-modified activated alumina for fluoride removal from water. J Hazard Mater 278:343–349. https://doi.org/10.1016/j.jhazmat.2014.06.008
Dayananda D, Sarva VR, Prasad SV, Arunachalam J, Ghosh NN (2014) Preparation of CaO loaded mesoporous Al2O3: efficient adsorbent for fluoride removal from water. Chem Eng J 248:430–439. https://doi.org/10.1016/j.cej.2014.03.064
Dou X, Zhang Y, Wang H et al (2011) Performance of granular zirconium-iron oxide in the removal of fluoride from drinking water. Water Res 45:3571–3578. https://doi.org/10.1016/j.watres.2011.04.002
Freundlich H (1907) Über die Adsorption in Lösungen. Zeitschrift für Phys Chemie 57U. https://doi.org/10.1515/zpch-1907-5723
Gasparotto JM, Roth D, Perilli ALO, Franco DSP, Carissimi E, Foletto EL, Jahn SL, Dotto GL (2021) A novel Fe-Al-La trioxide composite: synthesis, characterization, and application for fluoride ions removal from the water supply. J Environ Chem Eng 9:2213–3437. https://doi.org/10.1016/j.jece.2021.106350
Habuda-Stanić M, Ravančić M, Flanagan A (2014) A review on adsorption of fluoride from aqueous solution. Materials (Basel) 7:6317–6366. https://doi.org/10.3390/ma7096317
He P, Zhang L, Wu L, Chen T et al (2022) Synergistic effect of the sulfur vacancy and schottky heterojunction on photocatalytic uranium immobilization: the thermodynamics and kinetics. Inorg Chem 61:2242–2250. https://doi.org/10.1021/acs.inorgchem.1c03552
Kumar E, Bhatnagar A, Ji M, Jung W, Lee S, Kim SJ, Lee G, Song H, Choi JY, Yang Y, Jeon BH (2009) Defluoridation from aqueous solutions by granular ferric hydroxide (GFH). Water Res 43:490–498. https://doi.org/10.1016/j.watres.2008.10.031
Kumar E, Bhatnagar A, Kumar U, Sillanpää M (2011) Defluoridation from aqueous solutions by nano-alumina: characterization and sorption studies. J Hazard Mater 186:1042–1049. https://doi.org/10.1016/j.jhazmat.2010.11.102
Kumari U, Behera SK, Meikap BC (2019) A novel acid modified alumina adsorbent with enhanced defluoridation property: kinetics, isotherm study and applicability on industrial wastewater. J Hazard Mater 365:868–882. https://doi.org/10.1016/j.jhazmat.2018.11.064
Langmuir I (1918) The adsorption of gases on plane surfaces of glass, mica and platinum. J Am Chem Soc 40:1361–1403. https://doi.org/10.1021/ja02242a004
Li L, Zhu Q, Man K, Xing Z (2017) Fluoride removal from liquid phase by Fe-Al-La trimetal hydroxides adsorbent prepared by iron and aluminum leaching from red mud. J Mol Liq 237:164–172. https://doi.org/10.1016/j.molliq.2017.04.097
Liu J, Zhao P, Xu Y, Jia X (2019) Mg-Al mixed oxide adsorbent synthesized using FCT template for fluoride removal from drinking water. Bioinorg Chem Appl 2019:1–11. https://doi.org/10.1155/2019/5840205
Mendoza-Castillo DI, Reynel-Ávila HE, Bonilla-Petriciolet A, Silvestre-Albero J (2016) Synthesis of denim waste-based adsorbents and their application in water defluoridation. J Mol Liq 221:469–478. https://doi.org/10.1016/j.molliq.2016.06.005
Mohapatra M, Hariprasad D, Mohapatra L et al (2012) Mg-doped nano ferrihydrite - a new adsorbent for fluoride removal from aqueous solutions. Appl Surf Sci 258:4228–4236. https://doi.org/10.1016/j.apsusc.2011.12.047
Netto MS, Silva NF, Mallmann ES, Dotto EL, Foletto EL (2019) Effect of salinity on the adsorption behavior of methylene blue onto comminuted raw avocado residue: CCD-RSM design. Water Air Soil Pollut 230(187):2–17. https://doi.org/10.1007/s11270-019-4230-x
Nur T, Loganathan P, Nguyen TC et al (2014) Batch and column adsorption and desorption of fluoride using hydrous ferric oxide: solution chemistry and modeling. Chem Eng J 247:93–102. https://doi.org/10.1016/j.cej.2014.03.009
Peres MA, Cury JA (2011) Drinking water quality and fluoride concentration. Rev Saúde Pública 45:964–973. https://doi.org/10.1590/S0034-89102011005000046
Pigatto RS, Franco DSP, Netto MS et al (2020) An eco-friendly and low-cost strategy for groundwater defluorination: adsorption of fluoride onto calcinated sludge. J Environ Chem Eng 8:104546. https://doi.org/10.1016/j.jece.2020.104546
Redlich O, Peterson DL (1959) A useful adsorption isotherm. J Phys Chem 63:1024–1026
Rojas-Mayorga CKR, Petriciolet AB, Albero JS, Voillareal IAA (2015) Physico-chemical characterization of metal-doped bone chars and their adsorption behavior for water defluoridation. Appl Surf Sci 355:748–760. https://doi.org/10.1016/j.apsusc.2015.07.163
Salleh MAM, Mahmoud DK, Karim WAWA, Idris A (2011) Cationic and anionic dye adsorption by agricultural solid wastes: a comprehensive review. Desalination 280(1–3):1–13. https://doi.org/10.1016/j.desal.2011.07.019
Samarghandi MR, Khiadani M, Foroughi M, Nasab HZ (2016) Defluoridation of water using activated alumina in presence of natural organic matter via response surface methodology. Environ Sci Pollut Res 23:887–897. https://doi.org/10.1007/s11356-015-5293-x
Singh K, Lataye DH, Wasewar KL, Yoo CK (2013) Removal of fluoride from aqueous solution: status and techniques. Desalin Water Treat 51:3233–3247. https://doi.org/10.1080/19443994.2012.749036
Sips R (1948) On the structure of a catalyst surface. J Chem Phys 16:490–495
Thathsara SKT, Cooray PLAT, Mudiyanselage TK et al (2018) A novel Fe-La-Ce tri-metallic composite for the removal of fluoride ions from aqueous media. J Environ Manage 207:387–395. https://doi.org/10.1016/j.jenvman.2017.11.041
Tian Y, Wu M, Liu R, Wang D, Lin X, Liu W, Ma L, Li Y, Huang Y (2011) Modified native cellulose fibers—a novel efficient adsorbent for both fluoride and arsenic. J Hazard Mater 185(1):93–100. https://doi.org/10.1016/j.jhazmat.2010.09.001
Vithanage M, Bhattacharya P (2015) Fluoride in the environment: sources, distribution and defluoridation. Environ Chem Lett 13:131–147. https://doi.org/10.1007/s10311-015-0496-4
Wang Z, Shi M, Li J, Zheng Z (2014) Influence of moderate pre-oxidation treatment on the physical, chemical and phosphate adsorption properties of iron-containing activated carbon. J Environ Sci (China) 26:519–528. https://doi.org/10.1016/S1001-0742(13)60440-4
Wang J, Wu L, Li J et al (2018) Simultaneous and efficient removal of fluoride and phosphate by Fe-La composite: adsorption kinetics and mechanism. J Alloys Compd 753:422–432. https://doi.org/10.1016/j.jallcom.2018.04.177
Wang R, Li M, Liu T et al (2022) Encapsulating carbon-coated nano zero-valent iron particles with biomass-derived carbon aerogel for efficient uranium extraction from uranium-containing wastewater. J Clean Prod 364:132–654. https://doi.org/10.1016/j.jclepro.2022.132654
Wu X, Zhang Y, Dou X, Yang M (2007) Fluoride removal performance of a novel Fe-Al-Ce trimetal oxide adsorbent. Chemosphere 69:1758–1764. https://doi.org/10.1016/j.chemosphere.2007.05.075
Wu X, Zhang Y, Dou X et al (2013) Fluoride adsorption on an 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
Xiang W, Zhang G, Zhang Y, Tang D, Wang J (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
Zhang G, He Z, Xu W (2012) A low-cost and high efficient zirconium-modified-Na-attapulgite adsorbent for fluoride removal from aqueous solutions. Chem Eng J 183:315–324. https://doi.org/10.1016/j.cej.2011.12.085
Zhang S, Lu Y, Lin X et al (2014) Removal of fluoride from groundwater by adsorption onto La(III)-Al(III) loaded scoria adsorbent. Appl Surf Sci 303:1–5. https://doi.org/10.1016/j.apsusc.2014.01.169
Zhang J, Brutus TE, Cheng J, Meng X (2017) Fluoride removal by Al, Ti, and Fe hydroxides and coexisting ion effect. J Environ Sci 57:190–195. https://doi.org/10.1016/j.jes.2017.03.015
Zhou J, Zhu W, Yu J et al (2018) Highly selective and efficient removal of fluoride from ground water by layered Al-Zr-La Tri-metal hydroxide. Appl Surf Sci 435:920–927. https://doi.org/10.1016/j.apsusc.2017.11.108
Acknowledgements
The authors would like to thank CAPES (Coordination for the Improvement of Higher Education Personnel) and CNPq (National Council for Scientific and Technological Development) for their financial support.
Author information
Authors and Affiliations
Contributions
Conceptualization: [J.M. Gasparotto, E.L. Foletto, S.L. Jahn, G. L. Dotto]; Methodology: [D. Pinto, N. de Paula, M. Maraschin], Formal analysis and investigation: [E. Carissimi, D.S.P. Franco]; Writing—original draft preparation: [E.L. Foletto, J.M. Gasparotto, G.L. Dotto]; Writing—review and editing: [E.L. Foletto, J.M. Gasparotto, G.L. Dotto]; Funding acquisition: [E.L. Foletto, L.F.O. Silva, S.L. Jahn, E. Carissimi]; Supervision: [E.L. Foletto, L.F.O. Silva, G. L. Dotto]. All authors read and approved the final manuscript.
Corresponding author
Ethics declarations
Ethical approval
Not applicable.
Consent to participate
Not applicable.
Consent for publication
Not applicable.
Competing interests
The authors declare no competing interests.
Additional information
Responsible Editor: Philippe Garrigues
Publisher's note
Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
Supplementary Information
Below is the link to the electronic supplementary material.
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
Gasparotto, J.M., Pinto, D., de Paula, N. et al. Preparation of alumina-supported Fe-Al-La composite for fluoride removal from an aqueous matrix. Environ Sci Pollut Res 30, 42416–42426 (2023). https://doi.org/10.1007/s11356-023-25231-1
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1007/s11356-023-25231-1