Removal of fluoride from water using titanium-based adsorbents

Abstract

Three adsorbents including TiO₂, Ti-Ce, and Ti-La hybrid oxides were prepared to remove fluoride from aqueous solution. The Ti-Ce and Ti-La hybrid adsorbents obtained by the hydrolysis-precipitation method had much higher sorption capacity for fluoride than the TiO₂ adsorbent prepared through hydrolysis. Rare earth (Ce and La) oxides and TiO₂ exhibited a synergistic effect in the hybrid adsorbents for fluoride sorption. The sorption equilibrium of fluoride on the three adsorbents was achieved within 4 h, and the pseudo-second-order model described the sorption kinetics well. The sorption isotherms fitted the Langmuir model well, and the adsorption capacities of fluoride on the Ti-Ce and Ti-La adsorbents were about 9.6 and 15.1 mg·g^-1, respectively, at the equilibrium fluoride concentration of 1.0 mg·L^-1, much higher than the 1.7 mg·g^-1 on the TiO₂. The sorption capacities of fluoride on the three adsorbents decreased significantly when the solution pH increased from 3 to 9.5. The electrostatic interaction played an important role in fluoride removal by the three adsorbents, and Fourier transform infrared (FTIR) analysis indicated that the hydroxyl groups on the adsorbent surface were involved in fluoride adsorption.

Keywords

fluoride adsorption / titanium dioxide / titanium-based adsorbent / sorption mechanism

References

[1] Ayoob S, Gupta A K. Fluoride in drinking water: a review on the status and stress effects. Critical Reviews in Environmental Science and Technology, 2006, 36(6): 433-487

[2] WHO. Chemical fact sheets: fluoride. In: Guidelines for drinking water quality: incorporation first addendum. Recommendations, vol. 1, 3ed., Geneva. 2006, 375-377

[3] Meenakshi, Maheshwari R C. Fluoride in drinking water and its removal. Journal of Hazardous Materials, 2006, 137(1): 456-463

[4] Wajima T, Umeta Y, Narita S, Sugawara K. Adsorption behavior of fluoride ions using a titanium hydroxide-derived adsorbent. Desalination, 2009, 249(1): 323-330

[5] Medellin-Castillo N A, Leyva-Ramos R, Ocampo-Perez R, Garcia de la Cruz R F, Aragon-Piña A, Martinez-Rosales J M, Guerrero-Coronado R M, Fuentes-Rubio L. Adsorption of fluoride from water solution on bone char. Industrial & Engineering Chemistry Research, 2007, 46(26): 9205-9212

[6] Tang Y, Guan X, Wang J, Gao N, McPhail M R, Chusuei C C. Fluoride adsorption onto granular ferric hydroxide: effects of ionic strength, pH, surface loading, and major co-existing anions. Journal of Hazardous Materials, 2009, 171(1-3): 774-779

[7] Lv L, He J, Wei M, Evans D G, Zhou Z L. Treatment of high fluoride concentration water by MgAl-CO3 layered double hydroxides: kinetic and equilibrium studies. Water Research, 2007, 41(7): 1534-1542

[8] Biswas K, Gupta K, Ghosh U C. Adsorption of fluoride by hydrous iron(III)-tin(IV) bimetal mixed oxide from the aqueous solutions. Chemical Engineering Journal, 2009, 149(1-3): 196-206

[9] Meenakshi S, Sundaram C S, Sukumar R. Enhanced fluoride sorption by mechanochemically activated kaolinites. Journal of Hazardous Materials, 2008, 153(1-2): 164-172

[10] Ho L N, Ishihara T, Ueshima S, Nishiguchi H, Takita Y. Removal of fluoride from water through ion exchange by mesoporous Ti oxohydroxide. Journal of Colloid and Interface Science, 2004, 272(2): 399-403

[11] Pena M E, Korfiatis G P, Patel M, Lippincott L, Meng X. Adsorption of As(V) and As(III) by nanocrystalline titanium dioxide. Water Research, 2005, 39(11): 2327-2337

[12] Viswanathan N, Meenakshi S. Enhanced fluoride sorption using La(III) incorporated carboxylated chitosan beads. Journal of Colloid and Interface Science, 2008, 322(2): 375-383

[13] Alagumuthu G, Rajan M. Equilibrium and kinetics of adsorption of fluoride onto zirconium impregnated cashew nut shell carbon. Chemical Engineering Journal, 2010, 158(3): 451-457

[14] Deng S B, Li Z J, Huang J, Yu G. Preparation, characterization and application of a Ce-Ti oxide adsorbent for enhanced removal of arsenate from water. Journal of Hazardous Materials, 2010, 179(1-3): 1014-1021

[15] Wu X, Zhang Y, Dou X, Yang M. Fluoride removal performance of a novel Fe-Al-Ce trimetal oxide adsorbent. Chemosphere, 2007, 69(11): 1758-1764

[16] Gao S, Sun R, Wei Z, Zhao H, Li H, Hu F. Size-dependent defluoridation properties of synthetic hydroxyapatite. Journal of Fluorine Chemistry, 2009, 130(6): 550-556

[17] Daifullah A A M, Yakout S M, Elreefy S A. Adsorption of fluoride in aqueous solutions using KMnO4-modified activated carbon derived from steam pyrolysis of rice straw. Journal of Hazardous Materials, 2007, 147(1-2): 633-643

[18] Eskandarpour A, Onyango M S, Ochieng A, Asai S. Removal of fluoride ions from aqueous solution at low pH using schwertmannite. Journal of Hazardous Materials, 2008, 152(2): 571-579

[19] Ho Y S. Review of second-order models for adsorption systems. Journal of Hazardous Materials, 2006, 136(3): 681-689

[20] Deng S B, Ting Y P. Fungal biomass with grafted poly(acrylic acid) for enhancement of Cu(II) and Cd(II) biosorption. Langmuir, 2005, 21(13): 5940-5948

[21] Liu H, Deng S, Li Z, Yu G, Huang J. Preparation of Al-Ce hybrid adsorbent and its application for defluoridation of drinking water. Journal of Hazardous Materials, 2010, 179(1-3): 424-430

[22] Burgos M, Langlet M. Condensation and densification mechanism of sol-gel TiO2 layers at low temperature. Journal of Sol-Gel Science and Technology, 1999, 16(3): 267-276

[23] Rocha R A, Muccillo E N S. Physical and chemical properties of nanosized powders of gadolinia-doped ceria prepared by the cation complexation technique. Materials Research Bulletin, 2003, 38(15): 1979-1986

[24] Zhang Y, Yang M, Dou X M, He H, Wang D S. Arsenate adsorption on an Fe-Ce bimetal oxide adsorbent: role of surface properties. Environmental Science & Technology, 2005, 39(18): 7246-7253

[25] Abdelaziz M, Abdelrazek E M. Effect of dopant mixture on structural, optical and electron spin resonance properties of polyvinyl alcohol. Physica B, Condensed Matter, 2007, 390(1-2): 1-9

[26] Seoudi R, Abdelmongy S, Shabaka A A. Effect of polyvinyl alcohol matrices on the structural and spectroscopic studies of CdSe nanoparticles. Physica B, Condensed Matter, 2008, 403(10-11): 1781-1786

[27] Chen L, Wu H, Wang T, Jin Y, Zhang Y, Dou X. Granulation of Fe-Al-Ce nano-adsorbent for fluoride removal from drinking water by spray coating on sand in a fluidized bed. Powder Technology, 2009, 193(1): 59-64

[28] Sujana M G, Soma G, Vasumathi N, Anand S. Studies on fluoride adsorption capacities of amorphous Fe/Al mixed hydroxides from aqueous solutions. Journal of Fluorine Chemistry, 2009, 130(8): 749-754

[29] Ayoob S, Gupta A K, Bhakat P B, Bhat V T. Investigations on the kinetics and mechanisms of sorptive removal of fluoride from water using alumina cement granules. Chemical Engineering Journal, 2008, 140(1-3): 6-14

RIGHTS & PERMISSIONS

Higher Education Press and Springer-Verlag Berlin Heidelberg