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Cow bones char as a green sorbent for fluorides removal from aqueous solutions: batch and fixed-bed studies

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Abstract

Cow bone char was investigated as sorbent for the defluoridation of aqueous solutions. The cow bone char was characterized in terms of its morphology, chemical composition, and functional groups present on the bone char surface using different analytical techniques: SEM, EDS, N2-BET method, and FTIR. Batch equilibrium studies were performed for the bone chars prepared using different procedures. The highest sorption capacities for fluoride were obtained for the acid washed (q = 6.2 ± 0.5 mg/g) and Al-doped (q = 6.4 ± 0.3 mg/g) bone chars. Langmuir and Freundlich models fitted well the equilibrium sorption data. Fluoride removal rate in batch system is fast in the first 5 h, decreasing after this time until achieving equilibrium due to pore diffusion. The presence of carbonate and bicarbonate ions in the aqueous solution contributes to a decrease of the fluoride sorption capacity of the bone char by 79 and 31 %, respectively. Regeneration of the F-loaded bone char using 0.5 M NaOH solution leads to a sorption capacity for fluoride of 3.1 mg/g in the second loading cycle. Fluoride breakthrough curve obtained in a fixed-bed column presents an asymmetrical S-shaped form, with a slow approach of C/C 0 → 1.0 due to pore diffusion phenomena. Considering the guideline value for drinking water of 1.5 mg F−/L, as recommended by World Health Organization, the service cycle for fluoride removal was of 71.0 h ([F−]feed ∼ 9 mg/L; flow rate = 1 mL/min; m sorbent = 12.6 g). A mass transfer model considering the pore diffusion was able to satisfactorily describe the experimental data obtained in batch and continuous systems.

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Abbreviations

Bi :

Biot number

C :

Fluoride concentration in the column output at time t (mg/L)

C 0 :

Fluoride feed concentration (mg/L)

C b :

Fluoride concentration in the liquid phase at time t (mg/L)

\( {C}_{b_o} \) :

Initial concentration of fluoride in the liquid phase (mg/L)

C eq :

Equilibrium fluoride concentration in the liquid phase (mg/L)

\( {C}_m^{obs} \) :

Experimental concentration of fluoride at the point m (mg/L)

\( {C}_m^{\mathrm{cal}} \) :

Simulated concentration of fluoride at the point m (mg/L)

C p :

Concentration of fluoride in the pores inside the particle (mg/L)

D ax :

Axial dispersion coefficient (cm2/s)

D c :

Column internal diameter (cm)

d p :

Particle diameter (cm)

D pe :

Pore diffusion coefficient for fluoride ions (cm2/s)

f LUB :

Fraction of unused bed (%)

F cal :

Ratio between the variances of models A and B

F α :

Tabulated critical F values

K L :

Equilibrium Langmuir constant (L/mg)

K F :

Indicator of the sorption capacity (mg1–1/nL1/n/g)

k f :

Film mass transfer coefficient (cm/s)

L :

Bed length (cm)

L MTZ :

Length of the mass transfer zone (cm)

m :

Number of observations

n :

Total number of observations

n F :

Empirical parameter of the Freundlich equation

N d :

Number of mass transfer units inside particle

N f :

Number of mass transfer units in the film

p :

Number of adjusted parameters

Pe :

Peclet number

Q :

Flow rate (mL/min)

q :

Fluoride concentration on the solid phase at time t (mg/g of the adsorbent)

q c :

Fluoride sorption capacity in the fixed-bed column (mg/g)

q eq :

Concentration of fluoride in the solid phase (mg/g) in equilibrium with C eq

q max :

Maximum uptake capacity of fluoride per gram of adsorbent (mg/g)

r :

Radial position (cm)

r p :

Radius of particle (cm)

T :

Temperature (K)

t :

Time (h)

t Bp :

Breakthrough time (h)

t e :

Exhaustion time (h)

t st :

Stoichiometric time (h)

u i :

Interstitial fluid velocity (cm/s)

V :

Solution volume (L)

V pore :

Pore volume (cm3/g)

W :

Mass of sorbent (g)

x :

Dimensionless radial coordinate inside particle

y :

Axial position normalized by bed length

y p :

Dimensionless concentration of fluoride in the pores inside particle

y b :

Dimensionless concentration of fluoride in the bulk

z :

Axial position (cm)

α:

Level of significance

ε c :

Column porosity

ε p :

Particle porosity

ε r :

Volumetric fraction of liquid inside the batch adsorber

ρ p :

Particle density (g/cm3)

τ :

Space time (s)

τ d :

Time constant for intraparticle diffusion of fluoride ions (s)

τ f :

Time constant for diffusion of fluoride ions in the film (s)

θ :

Dimensionless time

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Acknowledgments

Financial support was partially provided by (i) UID/EQU/50020/2013 - POCI-01-0145-FEDER-006984 project, co-financed by FCT/MEC (Fundação para a Ciência e a Tecnologia/Ministério da Educação e Ciência), and FEDER (Fundo Europeu de Desenvolvimento Regional) through COMPETE 2020 and (ii) NORTE-07-0124-FEDER-0000008 project, co-financed by QREN (Quadro de Referência Estratégico Nacional), ON2 program (Programa Operacional Regional do Norte) and FEDER. Elbert M. Nigri acknowledges the Erasmus Mundus, CAPES-Brazil, CNPq and FAPEMIG for financial support. Maria A. P. Cechinel acknowledges her Doctoral fellowship provided by ANP-MME/MCT-PFRH09. Diego A. Mayer acknowledges his master scholarship provided by ANP (48610.002724/99-40.) L. P. Mazur acknowledges CAPES (Brazil) for her scholarship (BEX-1012/13-4). V.J.P. Vilar acknowledges the FCT Investigator 2013 Programme (IF/00273/2013).

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Authors and Affiliations

  1. Mining Engineering Department, Universidade Federal de Minas Gerais, Av. Antônio Carlos, 7727, Pampulha, Belo Horizonte, Brazil

    Elbert M. Nigri & Sônia D. F. Rocha

  2. Laboratório de Transferência de Massa e Simulação Numérica de Sistemas Químicos, Federal University of Santa Catarina, PO Box 476, Florianópolis, SC, CEP 88040-900, Brazil

    Maria Alice. P. Cechinel & Diego A. Mayer

  3. Laboratory of Separation and Reaction Engineering - Laboratory of Catalysis and Materials (LSRE-LCM), Chemical Engineering Department, Faculty of Engineering, University of Porto, Rua Dr. Roberto Frias, 4200-465, Porto, Portugal

    Luciana. P. Mazur, José M. Loureiro & Vítor J. P. Vilar

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  1. Elbert M. Nigri
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  2. Maria Alice. P. Cechinel
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  3. Diego A. Mayer
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  4. Luciana. P. Mazur
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Nigri, E.M., Cechinel, M.A.P., Mayer, D.A. et al. Cow bones char as a green sorbent for fluorides removal from aqueous solutions: batch and fixed-bed studies. Environ Sci Pollut Res 24, 2364–2380 (2017). https://doi.org/10.1007/s11356-016-7816-5

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