Environmental Science and Pollution Research

, Volume 25, Issue 18, pp 17473–17489 | Cite as

A comparative study on defluoridation capabilities of biosorbents: isotherm, kinetics, thermodynamics, cost estimation, and eco-toxicological study

  • Shraboni Mukherjee
  • Sujata Dutta
  • Sourjya Ray
  • Gopinath HalderEmail author
Research Article


The present study aims towards fluoride remediation from synthetic water using steam-activated carbon of Aegle marmelos (bael shell/wood apple) (BAC) and Parthenium hysterophorus (PHAC) according to batch sorption techniques. The impact of different parametric conditions viz. initial fluoride concentration (4–12 mg/L), time (0–5 h), temperature (293.15–333.15 K), adsorbent dosage (4–14 g/L), pH (4–9), and RPM (150–350) were considered for both the adsorbents. Maximum defluoridation of 89% was achieved by BAC at a concentration of 10 mg/L, adsorbent dose 6 g/L, pH 5, temperature 313.15 K, agitation speed 250 rpm, and contact time 9 h, whereas PHAC attained maximum removal of 78% at an initial concentration of 8 mg/L, adsorbent dose 10 g/L, pH 4, temperature 313.15 K, and contact time 12 h. Instrumental analysis by SEM, EDX, and FTIR confirmed about the fluoride binding ability of the adsorbents. The Langmuir isotherm model provided the best fit (R2 = 0.9962 and 0.9945) to the removal process with maximum adsorptive uptake of 16.85 and 6.22 mg/g by BAC and PHAC respectively. The adsorption phenomenon was found to obey pseudo-second-order kinetics. The endothermic, spontaneous, and feasible nature of the sorption process was confirmed by the thermodynamic study. The total costs of 1 kg adsorbent preparation were calculated as 1.122 USD and 1.0615 USD which helped us in determining the economic feasibility of the adsorbents in large-scale applications. The growth of Chlorella sorokiniana BTA 9031 was also observed to be affected by the fluoride solution. Comparing the removal efficiencies of both the adsorbents, it can be concluded that BAC shell proved to be an efficient adsorbent over PHAC for fluoride elimination from aqueous solution.

Graphical abstract

Defluoridation of aqueous solution using biochar derived from Aegle marmelos shell and Parthenium hysterophorus.


Defluoridation Aegle marmelos Parthenium hysterophorus Adsorption Cost estimation Eco-toxicological study 



The authors would like to acknowledge the Department of Biotechnology, Government of West Bengal, India, through research project BT (Estt.) R & D – 23/13 for providing financial support. The authors also express their gratitude to the Department of Chemical Engineering, University of Calcutta, for providing instrumentation facilities.


  1. Agalakova NI, Gusev GP (2012) Molecular mechanisms of cytotoxicity and apoptosis induced by inorganic fluoride. ISRN Cell Biol 2012(2012):1–16CrossRefGoogle Scholar
  2. Amalraj A, Pius A (2015) Removal of fluoride from drinking water using aluminium hydroxide coated activated carbon prepared from bark of Morinda tinctoria. Appl Water Sci 7:2653–2665. CrossRefGoogle Scholar
  3. Amini M, Abbaspour KC, Berg M, Winkel L, Hug SJ, Hoehn E, Yang H, Johnson CA (2008) Statistical modelling of global geogenic arsenic contamination in groundwater. Environ Sci Technol 42:3669–3675CrossRefGoogle Scholar
  4. Anandkumar J, Mandal B (2009) Removal of Cr (VI) from aqueous solution using Bael fruit (Aegle marmelos correa) shell as an adsorbent. J Hazard Mater 168(2–3):633–640CrossRefGoogle Scholar
  5. Ayoob S, Gupta AK, Bhat VT (2008) A conceptual overview on sustainable technologies for the defluoridation of drinking water. Crit Rev Environ Sci Technol 38(6):401–470CrossRefGoogle Scholar
  6. Banerjee A (2015) Groundwater fluoride contamination: a reappraisal. Geosci Front 6(2):277–284CrossRefGoogle Scholar
  7. Bhatnagar A, Kumar E, Sillanpaa M (2011) Fluoride removal from water by adsorption—a review. Chem Eng J 171:811–840CrossRefGoogle Scholar
  8. Bhaumik R, Mondal NK, Chattoraj S, Datta JK (2013) Application of response surface methodology for optimization of fluoride removal mechanism by newly developed biomaterial. Am J Analyt Chem 4:404–419CrossRefGoogle Scholar
  9. Bibi S, Kamran MA, Sultana J, Farooqi A (2016) Occurrence and methods to remove arsenic and fluoride contamination in water. Environ Chem Lett 15:125–149. CrossRefGoogle Scholar
  10. Chatterjee S, Kumar A, Basu S, Dutta S (2012) Application of response surface methodology for methylene blue dye removal from aqueous solution using low cost adsorbent. Chem Eng J 181:289–299CrossRefGoogle Scholar
  11. Chidambaram S, Ramanathan AL, Vasudevan S (2003) Fluoride removal studies in water using natural materials: technical note. Water SA 29(3):339–344Google Scholar
  12. Dhawane SH, Kumar T, Halder G (2016) Biodiesel synthesis from Hevea brasiliensis oil employing carbon supported heterogeneous catalyst: optimization by Taguchi method. Rene Energy 89:506–514CrossRefGoogle Scholar
  13. Drouiche N, Aoudj S, Lounici H, Drouiche M, Ouslimane T, Ghaffour N (2012) Fluoride removal from pretreated photovoltaic wastewater by electrocoagulation: an investigation of the effect of operational parameters. Process Eng 33:385–391CrossRefGoogle Scholar
  14. Fan X, Parker DJ, Smith MD (2003) Adsorption kinetics of fluoride on low cost materials. Water Res 37:4929–4937CrossRefGoogle Scholar
  15. Fu Y, Viraraghavan T (2002) Removal of Congo red from an aqueous solution by fungus Aspergillus niger. Adv Environ Res 7:239–247CrossRefGoogle Scholar
  16. Gao H, Jin Y, Wei J (2013) Health risk assessment of fluoride in drinking water from Anhui province in China. Environ Monit Assess 185:3687–3695CrossRefGoogle Scholar
  17. Hafshejani LD, Nasab SB, Gholami RM, Moradzadeh M, Izadpanah Z, Hafshejani SB, Bhatnagar A (2015) Removal of zinc and lead from aqueous solution by nanostructured cedar leaf ash as biosorbent. J Mol Liq 211:448–456CrossRefGoogle Scholar
  18. Hiremath PG, Theodore T (2017) Biosorption of fluoride from synthetic and ground water using Chlorella vulgaris immobilized in calcium alginate beads in an upflow packed bed reactor. Period Polytech Chem Eng 61(3):188–199CrossRefGoogle Scholar
  19. Hu C, Luo Q, Huang Q (2014) Ecotoxicological effects of perfluorooctanoic acid on freshwater microalgae Chlamydomonas reinhardtii and Scenedesmus obliquus. Environ Toxicol Chem 33(5):1129–1134CrossRefGoogle Scholar
  20. Iyenger L (2005) Defluoridation of water using activated alumina technology. Indian Institute of Technology, Kanpur for UNICEF, New DelhiGoogle Scholar
  21. Jagtap S, Yenkie MK, Labhteswar N, Rayalu S (2012) Fluoride in drinking water and defluoridation of water. Chem Rev 112(4):2454–2466CrossRefGoogle Scholar
  22. Khan SA, Thakur SK, Sarkar A, Shekhar S (2016) Worldwide contamination of water by fluoride. Environ Chem Lett 14:291–315. CrossRefGoogle Scholar
  23. Lahnid S, Tahaikt M, Elaroui K, Elmidaoui A (2008) Economic evaluation of fluoride removal by electrodialysis. Desalination 231(1):213–219CrossRefGoogle Scholar
  24. Lataye DH, Mishra IM, Mall ID (2011) Removal of 4-Picoline from aqueous solution by adsorption onto bagasse fly ash and rice husk ash: equilibrium, thermodynamic and desorption study. J Environ Eng 137(11):1048–1057CrossRefGoogle Scholar
  25. Maliyekkal SM, Shukla S, Philip L, Nambi IM (2008) Enhanced fluoride removal from drinking water by magnesia-amended activated alumina granules. Chem Eng J 140:183–192CrossRefGoogle Scholar
  26. Meenakshi, Maheshwari RC (2006) Fluoride in drinking water and its removal. J Hazard Mater 137:456–463CrossRefGoogle Scholar
  27. Mohan SV, Ramanaiah SV, Rajkumar B, Sarma PN (2007) Removal of fluoride from aqueous phase by biosorption onto algal biosorbent Spirogyra sp.-IO2: sorption mechanism elucidation. J Hazard Mater 141:465–474CrossRefGoogle Scholar
  28. Mohapatra M, Anand S, Mishra BK, Giles DE, Singh P (2009) Review of fluoride removal from drinking water. J Environ Manag 91:67–77CrossRefGoogle Scholar
  29. Mondal P, George S (2015) A review on adsorbents used for defluoridation of drinking water. Rev in Environ Sci Bio/Technol 14(2):195–210CrossRefGoogle Scholar
  30. Mondal NK, Bhaumik R, Datta JK (2016a) Fluoride adsorption by calcium carbonate, activated alumina and activated sugarcane ash. Environ Proc 3(1):195–216CrossRefGoogle Scholar
  31. Mondal S, Aikat K, Halder G (2016b) Biosorptive uptake of ibuprofen by chemically modified Parthenium hysterophorus derived biochar: equilibrium, kinetics, thermodynamics and modelling. Ecol Eng 92:158–172CrossRefGoogle Scholar
  32. Mondal M, Ghosh A, Tiwari ON, Gayen K, Das P, Mandal MK, Halder GN (2017a) Influence of carbon sources and light intensity on biomass and lipid production of Chlorella sorokiniana BTA 9031 isolated from coalfield under various nutritional modes. Energ Convers Manage 145(1):247–254CrossRefGoogle Scholar
  33. Mondal S, Aikat K, Siddharth K, Sarker K, DasChaudhury R, Mandal G, Halder G (2017b) Optimizing ranitidine hydrochloride uptake of Parthenium hysterophorus derived N-biochar through response surface methodology and artificial neural network. Process Saf Environ Prot 107:388–401CrossRefGoogle Scholar
  34. Mukherjee S, Halder G (2016) Assessment of fluoride uptake performance of raw biomass and activated biochar of Colocasia esculenta stem: optimization through response surface methodology. Environ Prog Sustain Energy 35(5):1305–1316CrossRefGoogle Scholar
  35. Mukherjee S, Mondal M, Banerjee S, Halder G (2017) Elucidation of the sorptive uptake of fluoride by Ca2+-treated and untreated algal biomass of Nostoc sp. (BTA394): isotherm, kinetics, thermodynamics and safe disposal. Process Saf Environ Prot 107:334–345CrossRefGoogle Scholar
  36. Patel S (2011) Harmful and beneficial aspects of Parthenium hysterophorus: an update. 3 Biotech 1(1):1–9CrossRefGoogle Scholar
  37. Rout TK, Verma R, Dennis RV, Banerjee S (2015) Study the removal of fluoride from aqueous medium by using nano-composites. J Encapsul Adsorpt Sci 5:38–52CrossRefGoogle Scholar
  38. Sadaf S, Bhatti HN (2014) Batch and fixed bed column studies for the removal of Indosol Yellow BG dye by peanut husk. J Taiwan Inst Chem Eng 45:541–553CrossRefGoogle Scholar
  39. Schneider TR, Salovey P, Apanovitch AM, Pizarro J, McCarthy D, Zullo J (2001) The effects of message framing and ethnic targeting on mammography use among low-income women. Health Psychol 20(4):256–266CrossRefGoogle Scholar
  40. Sehn P (2008) Fluoride removal with extra low energy reverse osmosis membranes: three years of large scale field experience in Finland. Desalination 223(1):73–84CrossRefGoogle Scholar
  41. Shafique U, Ijaz A, Salman M, Jamil N, Rehman R, Javaid A (2012) Removal of arsenic from water using pine leaves. J Taiwan Inst Chem Eng 43:256–263CrossRefGoogle Scholar
  42. Shekhar S, Pandey AC, Nathawat MS (2012) Evaluation of fluoride contamination in groundwater sources in hard rock terrain in Garhwa district, Jharkhand, India. Int J Environ Sci 3(3):1022–1030Google Scholar
  43. Singh K, Lataye DH, Wasewar KL (2017) Removal of fluoride from aqueous solution by using bael (Aegle marmelos) shell activated carbon: kinetic, equilibrium and thermodynamic study. J Fluor Chem 194:23–32CrossRefGoogle Scholar
  44. Tripathy SS, Bersillon JL, Gopal K (2006) Removal of fluoride from drinking water by adsorption onto alum-impregnated activated alumina. Sep Purif Technol 50:310–317CrossRefGoogle Scholar
  45. Venugopal V, Mohanty K (2011) Biosorptive uptake of Cr (VI) from aqueous solutions by Parthenium hysterophorus weed: equilibrium, kinetics and thermodynamic studies. Chem Eng J 174:151–158CrossRefGoogle Scholar
  46. Wang L, Zhang J, Jhao R, Li Y, Li C, Jhang C (2010) Adsorption of Pb (II) on activated carbon prepared from Polygonum orientale Linn.: kinetics, isotherms, pH and ionic strength studies. Bioresour Technol 101:5808–5814CrossRefGoogle Scholar
  47. WHO (1984) Guidelines for drinking-water quality, vol 2. Health Criteria and Other Supporting Information, GenevaGoogle Scholar
  48. WHO (1985) Guidelines for drinking water quality, vol 3. Drinking-water quality control in small-community supplies, GenevaGoogle Scholar
  49. Xiang QY, Chen LS, Chen XD, Wang CS, Liang YX, Liao QL, Fan DF, Hong P, Zhang MF (2005) Serum fluoride and skeletal fluorosis in two villages in Jiangsu province, China. Fluoride 38(3):178–184Google Scholar
  50. Yadav AK, Kaushik CP, Haritash AK, Kansal A, Rani N (2006) Defluoridation of groundwater using brick powder as an adsorbent. J Hazard Mater 128:289–293CrossRefGoogle Scholar
  51. Zayed AM, Selim AQ, Mohamed EA, Sillanpaa M (2017) Adsorption characteristics of Na-A zeolites synthesized from Egyptian kaolinite for manganese in aqueous solutions: response surface modeling and optimization. Appl Clay Sci 140:17–24CrossRefGoogle Scholar

Copyright information

© Springer-Verlag GmbH Germany, part of Springer Nature 2018

Authors and Affiliations

  • Shraboni Mukherjee
    • 1
  • Sujata Dutta
    • 1
  • Sourjya Ray
    • 1
  • Gopinath Halder
    • 1
    Email author
  1. 1.Chemical Engineering DepartmentNational Institute of TechnologyDurgapurIndia

Personalised recommendations