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Removal of ronidazole and sulfamethoxazole from water solutions by adsorption on granular activated carbon: equilibrium and intraparticle diffusion mechanisms

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Abstract

The equilibrium and intraparticle diffusion of ronidazole (RNZ) and sulfamethoxazole (SMX) during the adsorption on granular activated carbon (GAC) from aqueous solution was investigated in this work. The solution pH, temperature, ionic strength and water matrix affected the adsorption capacity of GAC towards SMX, but no effect was observed for the adsorption of RNZ. This behavior was due to the different mechanism involved in the adsorption of both antibiotics. The adsorption capacity of GAC towards RNZ was greater than that towards SMX. Molecular computation allowed the estimation of the binding free energy and confirmed that the adsorption of RNZ was more favorable than the adsorption of SMX. The adsorption mechanism of both antibiotics is governed by π–π dispersive interactions, and molecular simulation demonstrated that the coulombic interactions did not affect, but the solvation and nonpolar interactions play a significant role on the adsorption of both antibiotics. The application of diffusional models revealed that the overall adsorption rate of both antibiotics is controlled by intraparticle diffusion. Moreover, the surface diffusion was more predominant than the pore volume diffusion. Besides, surface diffusion coefficient, Ds, for RNZ was not a function of the aqueous matrix, whereas Ds for SMX was highly dependent on the water matrix.

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Notes

  1. TCB Group, http://www.ks.uiuc.edu/Training/Tutorials/science/forces/forces-tutorialfiles/gridForceFiles/graphene/.

  2. Chemical Computing Group, Montreal, Canada, http://www.chemcomp.com.s

Abbreviations

a:

Radke–Prausnitz isotherm constant (L g−1)

Ap :

Projected area of an antibiotic molecule (m2 molecule−1)

b:

Radke–Prausnitz isotherm constant (mmol−β Lβ)

Ce :

Concentration of antibiotic at equilibrium (mmol L−1)

C A :

Concentration of antibiotic in aqueous solution (mg L−1)

C A,pred :

Predicted concentration of antibiotic in aqueous solution (mg L−1)

C A0 :

Initial concentration of antibiotic in aqueous solution (mg L−1)

C Ar :

Concentration of antibiotic within the particle at distance r (mg L−1)

C Ar|r=R :

Concentration of antibiotic at the external surface of the GAC particle at r = Rp (mg L−1)

dp :

Average pore diameter (nm)

D AB :

Molecular diffusion coefficient at infinite dilution (cm2 s−1)

D ep :

Effective pore volume diffusion coefficient (cm2 s−1)

D s :

Surface diffusion coefficient (cm2 s−1)

K:

Constant of the Langmuir isotherm related to adsorption enthalpy (L mmol−1)

k L :

External mass transfer coefficient in liquid phase (cm s−1)

L0 :

Average width of the micropores

m :

Mass of adsorbent (g)

N:

Number of experimental data

NA :

Avogadro’s number, 6.022 × 1023 (molecules mol−1)

N AP :

Mass transport due to pore volume diffusion, mg cm−2 s−1

N AS :

Mass transport due to surface diffusion, mg cm−2 s−1

\( N_{\text{AS,r}} \) :

Radial average contribution of superficial contribution

pKow :

Octanol–water partition coefficient

pKa:

Acid dissociation constant

pHPZC :

pH of Point Zero Charge

q :

Uptake of antibiotic adsorbed (mmol g−1)

qpred :

Uptake of antibiotic adsorbed predicted with the isotherm model (mmol g−1)

qm :

Maximum adsorption capacity of GAC towards an antibiotic (mmol g−1)

r :

Radial distance (cm)

Rp :

Radius of the particle (cm)

R :

Universal gas law constant, 8.314 (J mol−1 K−1)

S:

External surface area per mass of adsorbent (cm2 g−1)

SBET :

Surface area (m2 g−1)

T:

Temperature (K)

V:

Volume of the solution in adsorber (mL)

VP :

Total pore volume (cm3 g−1)

Vmic :

Micropore volume (cm3 g−1)

β:

Radke–Prausnitz isotherm constant

ɛ p :

Void fraction of GAC particles

ρp :

Density of adsorbent particles (g mL−1)

τ:

Tortuosity factor

ΔHads :

Heat of adsorption (J mol−1)

% D:

Average percentage of deviation

% SOc :

Percentage of surface area occupied by antibiotic molecule adsorbed

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Acknowledgments

This work was funded by Consejo Nacional de Ciencia y Tecnologia, CONACyT, Mexico, through Grants Nos. INFR-2012-01-188381 (R. Leyva-Ramos), CB-2012-02-182779 (R. Leyva-Ramos) and CB-2013-01 221757 (R. Ocampo-Perez).

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Authors and Affiliations

  1. Centro de Investigación y Estudios de Posgrado, Facultad de Ciencias Químicas, Universidad Autónoma de San Luis Potosí, Av. Dr. M. Nava No. 6, 78210, San Luis Potosí, SLP, Mexico

    A. I. Moral-Rodríguez, R. Leyva-Ramos, R. Ocampo-Pérez, J. Mendoza-Barron & J. J. Salazar-Rabago

  2. Departamento de Química, Universidad Autónoma Metropolitana-Iztapalapa, 09340, Iztapalapa, D. F., Mexico

    I. N. Serratos-Alvarez

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  1. A. I. Moral-Rodríguez
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Correspondence to R. Ocampo-Pérez.

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Moral-Rodríguez, A.I., Leyva-Ramos, R., Ocampo-Pérez, R. et al. Removal of ronidazole and sulfamethoxazole from water solutions by adsorption on granular activated carbon: equilibrium and intraparticle diffusion mechanisms. Adsorption 22, 89–103 (2016). https://doi.org/10.1007/s10450-016-9758-0

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