Surface Complexation of Chromium(VI) on Iron(III) Hydroxide: Mechanisms and Stability Constants of Surfaces Complexes

Mhamed Hmamou; Fatima Ezzahra Maarouf; Bouchaib Ammary; Abdelkebir Bellaouchou

doi:10.22146/ijc.60634

Surface Complexation of Chromium(VI) on Iron(III) Hydroxide: Mechanisms and Stability Constants of Surfaces Complexes

https://doi.org/10.22146/ijc.60634

Mhamed Hmamou^(1*), Fatima Ezzahra Maarouf⁽²⁾, Bouchaib Ammary⁽³⁾, Abdelkebir Bellaouchou⁽⁴⁾

(1) Applied Chemistry Laboratory Materials, University Mohamed V, Faculty of Science, Ibn Batouta Avenue, Rabat, Morocco
(2) Applied Chemistry Laboratory Materials, University Mohamed V, Faculty of Science, Ibn Batouta Avenue, Rabat, Morocco
(3) Applied Chemistry Laboratory Materials, University Mohamed V, Faculty of Science, Ibn Batouta Avenue, Rabat, Morocco
(4) Nanotechnology Laboratory and Environment, University Mohamed V, Faculty of Science, Ibn Batouta Avenue, Rabat, Morocco
(*) Corresponding Author

Abstract

The adsorption of chromate ions H_2-yA (y = 1, 2, and A = CrO₄^2–) on iron(III) hydroxide was conducted as a function of adsorbent mass, solution pH, and hydration time. The surface complexation technique, based on the examination of the chromate distribution between the solid and liquid phases, was adopted to predict the adsorption mechanism. To specify stoichiometry of the chromate surface complexes, the proton (n > 0), and hydroxyl (n < 0) ion-exchange was evaluated at a pH range of 2–12. The obtained “n” values are ranging between -1 and 1. As a result, the sorption process involved specific chemical interaction with surface sites, resulting in 1H⁺ and 1OH^– release of the adsorbate molecule. The surface species identified were ; ; ; ; ; ; ; and . The logarithmic values of their complexing constants were: log K₀₀ = 1.81 ± 0.04; log K₁₁ = -3.53 ± 0.07; log K₂₁ = -1.03 ± 0.23, log K_1-1 = 7.15 ± 0.14 and log K_2-1 = 9.62 ± 0.53. The results showed that the chromate adsorption on Fe(III) hydroxide was of electrostatic and chemical nature at pH lower than 5.5, and only of chemical nature at pH superior to 5.5. Taking into account these considerations, Fe(III) hydroxide could be considered an excellent sorbent for the removal of Cr(VI) from wastewater solutions.

Keywords

chromium(VI); iron(III) hydroxide; adsorption; surface complexes; stability constants

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References

[1] Saha, R., Nandi, R., and Saha, B., 2011, Sources and toxicity of hexavalent chromium, J. Coord. Chem., 64 (10), 1782–1806.

[2] Praveen, P., and Loh, K.C., 2016, Thermodynamic analysis of Cr(VI) extraction using TOPO impregnated membranes, J. Hazard. Mater., 314, 204–210.

[3] Lim, S.F., and Lee, A.Y.W., 2015, Kinetic study on removal of heavy metal ions from aqueous solution by using soil, Environ. Sci. Pollut. Res., 22 (13), 10144–10158.

[4] Gorzin, F., and Abadi, M.M.B.R., 2017, Adsorption of Cr(VI) from aqueous solution by adsorbent prepared from paper mill sludge: Kinetic and thermodynamic studies, Adsorpt. Sci. Technol., 36 (1-2), 149–169.

[5] Nagajyoti, P.C., Lee, K.D., and Sreekanth, T.V.M., 2010, Heavy metals, occurrence and toxicity for plants: A review, Environ. Chem. Lett., 8 (3), 199–216.

[6] Singh, R., Gautam, N., Mishra, A., and Gupta, R., 2011, Heavy Metals and living systems: an overview, Indian J. Pharmacol., 43 (3), 246–253.

[7] Zachara, J.M., Ainsworth, C.C., Brown, G.E., Catalano, J.G., McKinley, J.P., Qafoku, O., Smith, S.C., Szecsody, J.E., Traina, S.J., and Warner, J.A., 2004, Chromium speciation and mobility in a high level nuclear waste vadose zone plume, Geochim. Cosmochim. Acta, 68 (1), 13–30.

[8] Duan, W., Chen, G., Chen, C., Sanghvi, R., Iddya, A., Walker, S., Liu, H., Ronen, A., and Jassby, D., 2017, Electrochemical removal of hexavalent chromium using electrically conducting carbon nanotube/polymer composite ultrafiltration membranes, J. Membr. Sci., 531, 160–171.

[9] Mayasari, H.E., and Sholeh, M., 2016, Kajian adsorpsi krom dalam limbah cair penyamakan kulit, JKM, 13 (2), 50–56.

[10] Daraei, H., Mittal, A., Noorisepehr, M., and Mittal, J., 2015, Separation of chromium from water samples using eggshell powder as a low-cost sorbent: kinetic and thermodynamic studies, Desalin. Water Treat., 53 (1), 214–220.

[11] Athieh, M.A., 2011, Removal of chromium(VI) from polluted water using carbon nanotubes supported with activated carbon, Procedia Environ. Sci, 4, 281–293.

[12] Liu, H., Zhang, F., and Peng, Z., 2019, Adsorption mechanism of Cr(VI) onto GO/PAMAMS composites, Sci. Rep., 9 (1), 3663.

[13] Yussuff, A.S., 2019, Adsorption of hexavalent chromium from aqueous solution Leucaena leucocephala seed pod activated carbon: Equilibrium, kinetic and thermodynamic studies, Arab J. Basic Appl. Sci., 26 (1), 89–102.

[14] Li, I.L., Feng, X.Q., Han, R.P., Zang, S.Q., and Yang, G., 2017, Cr(VI) removal via anion exchange on a silver-triazolate MOF, J. Hazard. Mater., 321, 622–628.

[15] Pagilla, K.R., and Canter, L.W., 1999, Laboratory studies on remediation of chromium-contaminated soils, J. Environ. Eng., 125 (3), 243–248.

[16] Gheju, M., and Balcu, I., 2011, Removal of chromium from Cr(VI) polluted wastewaters by reduction with scrap iron and subsequent precipitation of resulted cations, J. Hazard. Mater., 196, 131–138.

[17] Golbaz, S., Jafari, A.J., Rafiee, M., and Kalantary, R.R., 2014, Separate and simultaneous removal of phenol, chromium, and cyanide from aqueous solution by coagulation/precipitation: Mechanisms and theory, Chem. Eng. J., 253, 251–257.

[18] Maximous, N.N., Nakhla, G.F., and Wan, W.K., 2010, Removal of heavy metals from wastewater by adsorption and membrane processes: A comparative study, World Acad. Sci. Eng. Technol., 40, 599–604.

[19] Hu, J., Chen, G., and Lo, I.M.C., 2005, Removal and recovery of Cr(VI) from wastewater by maghemite nanoparticles, Water Res., 39 (18), 4528–4536.

[20] Yang, T., Han, C., Liu, H., Yang, L., Liu, D., Tang, J., and Luo, Y., 2019, Synthesis of Na-X zeolite from low aluminium coal fly: Characterization and high efficient As(V) removal, Adv. Powder Technol., 30 (1), 199–206.

[21] Nor, N.M., Kamil, N.H.N., Mansor, A.I., and Maarof, H.I., 2020, Adsorption analysis of fluoride removal using graphene oxide/eggshell adsorbent, Indones. J. Chem., 20 (3), 579–586.

[22] Razzouki, B., El Hajjaji, S., El Yahyaoui, A., Lamhamdi, A., Jaafar, A., Azzaoui, K., Bousaoud, A., and Zarouk, A., 2015, Kinetic investigation on arsenic(III) adsorption onto iron(III) hydroxide, Pharm. Lett., 7 (9), 53–59.

[23] Alvarez-Ayusco, E., Garcia Sanchez A., and Querol, X., 2007, Adsorption of Cr(VI) from synthetic solutions and electroplating wastewaters on amorphous aluminium oxide, J. Hazard. Mater., 142 (1-2), 191–198.

[24] Hyder, A.H.M.G., Begum, S.A., and Egiebor, N.O., 2015, Adsorption isotherm and kinetic studies of hexavalent chromium removal from aqueous solution onto bone char, J. Environ. Chem. Eng., 3 (2), 1329–1336.

[25] Suryanti, V., Hastuti, S., Wahyuningsih, T.D., Mudasir, Kresnadipayana, D., and Wiratna, I., 2018, Heavy metal removal from aqueous solution using biosurfactants produced by Pseudomonas aeruginosa with corn oil as substrate, Indones. J. Chem., 18 (3), 472–478.

[26] Selvi, K., Pattabhi, S., and Kadirvelu, K., 2001, Removal of Cr(VI) from aqueous solutions by adsorption onto activated carbon, Bioresour. Technol., 80 (1), 87–89.

[27] El Batouti, M., Ahmed, A.M.M., and Salam, S.M., 2016, Adsorption of toxic Ni(II) from aqueous solution by activated carbon, Mor. J. Chem., 4 (4), 1130–1143.

[28] Duranoğlu, D., Buyruklardan Kaya, İ.G., Beker, U., and Şenkal, B.F., 2012, Synthesis and adsorption properties of polymeric and polymer-based hybrid adsorbent for hexavalent chromium removal, Chem. Eng. J., 181-182, 103–112.

[29] Kobielska, P.A., Howarth, A.J., Farha, O.K., and Nayak, S., 2018, Metal-Organic frameworks for heavy metal removal from water, Coord. Chem. Rev., 358, 92–107.

[30] Yang, T., Han, C., and Luo, Y., 2019, Removal performance and mechanisms of Cr(VI) by an in-situ self-improvement of mesoporous biochar derived from chicken bone, Environ. Sci. Pollut. Res., 27 (5), 5018–5029.

[31] Kristianto, H., Daulay, N., and Arie, A.A., 2019, Adsorption of Ni(II) ion onto calcined eggshells: A study of equilibrium adsorption isotherm, Indones. J. Chem., 19 (1), 143–150.

[32] Taher, T., Irianty, Y., Mohadi, R., Said, M., Andreas, R., and Lesbani, A., 2019, Adsorption of cadmium(II) using Ca/Al layered double hydroxides intercalated with Keggin ion, Indones. J. Chem., 19 (4), 873–881.

[33] Mahatmanti, F.W., Nuryono, and Narsito, 2016, Adsorption of Ca(II), Mg(II), Zn(II), and Cd(II) on chitosan membrane blended with rice hull ash silica and polyethylene glycol, Indones. J. Chem., 16 (1), 45–52.

[34] Handayani, D.S., Jumina, Siswanta, D., Mustofa, Ohto, K., and Kawakita, H., 2011, Adsorption of Pb(II), Cd(II), and Cr(III) from aqueous solution by poly-5-allyl-calix[4]arene tetracarboxylic acid, Indones. J. Chem., 11 (2), 191–195.

[35] Abdul, A.S., Muhammad, A.S., Ibrahim, M.A., and Ibrahim, M.B., 2019, Thermodynamic study on the adsorptive removal of Cr(VI) and Ni(II) metal ions using Schiff base as adsorbent, Mor. J. Chem., 7 (3), 506–515.

[36] Jang, E.H., Pack, S.P., Kim, I., and Chung, S., 2020, A systematic study of hexavalent chromium adsorption and removal from aqueous environments using chemically functionalized amorphous and mesoporous silica nanoparticles, Sci. Rep., 10, 5558.

[37] Tang, B., and Hang, Z., 2014, Essence of disposing the excess sludge and optimizing the operation of wastewater treatment: Rheological behavior and microbial ecosystem, Chemosphere, 105, 1–13.

[38] Jolivet, J.P., Henry, M., and Livage, J., 1994, De la Solution à l’Oxyde. Condensation des cations en solution aqueuse, chimie de surface des oxydes, CNRS Editions, Inter Editions, Paris.

[39] Elyahyaoui, A., Ellouzi, K., Al Zabadi, H., Razzouki, B., Bouhlassa, S., Azzaoui, K., Mejdoubi, E., Hamed, O., Jodeh, S., and Lahmamdi, A., 2017, Adsorption of chromium(VI) on calcium phosphate: Mechanisms and stability constants of surface complexes, Appl. Sci., 7 (3), 222.

[40] Forsling, L., Wu, W., and Schindler, P.W., 1991, Surface complexation of calcium minerals in aqueous solution: 1. Surface protonation at fluorapatite-water interfaces, J. Colloid Interface Sci., 147 (1), 178–185.

[41] AFNOR-French Agency for Standardization, 1997, Water Quality. Tome1: Terminology, Sampling and Assessment Methods, 3^rd Ed., AFNOR Publishing, Paris, France.

[42] Samaké, D., 2008, Traitement des eaux usées de tannerie à l'aide de matériaux à base d'argile, Dissertation, Université Joseph Fourier-Grenoble et de Bamako, Mali.

[43] Lorphensri, O., Intravijit, J., Sabatini, D.A., Kibbey, T.C.G., Osathaphan, K., and Saiwan, C., 2006, Sorption of acetaminophen, 17α-ethynyl estradiol, nalidixic acid, and norfloxacin to silica, alumina and a hydrophobic medium, Water Res., 40 (7), 1481–1491.

[44] Harding, I.S., Rashid, N., and Hing, K.A., 2005, Surface charge and the effect of excess calcium ions on the hydroxyapatite surface, Biomaterials, 26 (34), 6818–6826.

[45] Demetriou, A., and Pashalidis, I., 2012, Spectrophotometric studies on the competitive adsorption of boric acid (B(III)) and chromate (Cr(VI)) onto iron (oxy) hydroxide (Fe(O)OH), Global NEST J., 14 (1), 32–39.

[46] Chowdhury, S.R., and Yanful, E.K., 2010, Arsenic and chromium removal by mixed magnetite-maghemite nanoparticles and the effect of phosphate on removal, J. Environ. Manage., 91 (11), 2238–2247.

[47] Krishna, H.R., and Swamy, A.V.V.S., 2012, Investigation on the adsorption of hexavalent chromium from the aqueous solutions using powder of papaya seeds as a sorbent, Int. J. Environ. Sci. Res., 2 (1), 119–125.

[48] Talokar, A.Y., 2011, Studies on removal of chromium from waste water by adsorption using low cost agricultural biomass as adsorbents, Int. J. Adv. Biotechol. Res., 2 (4), 452–456.

[49] Gholipour, M., Hashemipour, H., and Mollashahi, M., 2011, Hexavalent chromium removal from aqueous solution via adsorption on granular activated carbon: Adsorption, desorption, modeling and simulation studies, ARPN J. Eng. Appl. Sci., 6 (9), 10–18.

[50] Wu, X.W., Ma, H.W., and Zhang, Y.R., 2010, Adsorption of chromium(VI) from aqueous solution by a mesoporous aluminosilicate synthesized from microcline, Appl. Clay Sci., 48, 538–541.

[51] Pandey, P.K., Sharma, S.K., and Sambi, S.S., 2010, Kinetics and equilibrium study of chromium adsorption on zeolite NaX, Int. J. Environ. Sci. Technol., 7 (2), 395–404.

[52] Soundarrajan, M., Gomathi, T., and Sudha, P.N., 2013, Understanding the adsorption efficiency of chitosan coated carbon on heavy metal removal, IJSRP, 3 (1), 1–10.

[53] Fellenz, N., Martin, P., Marchetti, S., and Bengoa, F., 2015, Aminopropyl-modified mesoporous silica nanospheres for the adsorption of Cr(VI) from water, J. Porous Mater., 22 (3), 429–738.

[54] Abbas, M., and Trari, M., 2015, Kinetic, equilibrium and thermodynamic study on the removal of Congo Red from aqueous solutions, Process Saf. Environ. Prot., 98, 424–436.

[55] Dula, T., Siraj, K., and Kitte, S.A., 2014, Adsorption of hexavalent chromium from aqueous solution using chemically activated carbon prepared from locally available waste of bamboo (Oxytenanthera abyssinica), Int. Scholarly Res. Not., 2014, 438245.

[56] Ghazi, M., Oladipo, A.A., and Azalok, K.A., 2018, High efficient and magnetically separable palm seed-based biochar for the removal of nickel, Sep. Sci. Technol., 53 (7), 1124–1131.

[57] Farley, K.J., Dzombak, D.A., and Morel, F.M.M., 1985, A surface precipitation model for the sorption of cations on metal oxides, J. Colloid Interface Sci., 106 (1), 226–242.

[58] Attia, A.A., Khedr, S.A., and Elkholy, S.A., 2010, Adsorption of chromium ion (VI) by acid activated carbon, Braz. J. Chem. Eng., 27 (1), 183–193.

[59] Correa, F.G., Gómez, J.S., and Martínez, J.B., 2010, “Síntesis y caracterización de materiales inorgánicos para ser empleados como adsorbentes de metales tóxicos y de interés nuclear” in Contribuciones del Instituto Nacional de Investigaciones Nucleares al avance de la Ciencia y la Tecnología en México, Commemorative Edition 2010, Instituto Nacional de Investigaciones Nucleares, Ocoyoacac, Mexico, 195–210.

[60] Müller, A., and Sigg, L., 1992, Adsorption of lead(II) on the goethite surface: Voltammetric evaluation of surface complexation parameters, J. Colloid Interface Sci., 148 (2), 517–532.

DOI: https://doi.org/10.22146/ijc.60634