Mohamed El Miz, Samira Salhi, Ikrame Chraibi, Ali El Bachiri, Marie-Laure Fauconnier, Abdesselam Tahani

Show more
LACPRENE, Faculté des Sciences, Université Mohamed 1er, Oujda, Morocco.
Département de Géologie, Faculté des Sciences, Université Mohamed 1er, Oujda, Morocco.
Unité de Chimie Générale et Organique, Gembloux Agro-Bio Tech, Université de Liège, Gembloux, Belgique.
Show less

Abstract: Pillared clay (PILC) was prepared from Moroccan clay and characterized, and its aqueous thymol adsorption capacities were studied using a batch equilibrium technique. So, we tested the encapsulation of thymol by aluminum pillared clay (PILC). The PILCs displayed a total surface area of 270 m2/g, a total pore volume of 0.246 cm3/g and an average pore diameter of 8.9 A, which corresponds to the size of Al13 forming the pillars between the clay layers. The adsorption capacity shown by the PILCs for thymol from water is close to 319 mg?g-1 for low solid/liquid ratio (0.2%). This result suggests that the PILCs have both hydrophobic and hydrophilic characteristics, as a result of the presence of silanol and siloxane groups formed during the pillaring and calcination of the PILCs. The experimental data were analyzed by the Freundlich and the Langmuir isotherm types for low values of equilibrium concentration. The rise of the isotherm in this range of concentrations was related to the affinity of thymol for clay sites, and the equilibrium data fitted well with the Freundlich model with maximum adsorption capacity of 319.51 mg/g for a ratio RS/L = 0.2%. Pseudo-first and pseudo-second-order kinetic models were tested with the experimental data and pseudo-first order kinetics was the best for the adsorption of thymol with coefficients of correlation R2 ≥0.986, and the adsorption was rapid with 90% of the thymol adsorbed within the first 20 min.

Keywords: Clays, Bentonite, Thymol, Adsorption, Desorption, Kinetics, Pillared Clay

Cite this paper: El Miz, M. , Salhi, S. , Chraibi, I. , El Bachiri, A. , Fauconnier, M. and Tahani, A. (2014) Characterization and Adsorption Study of Thymol on Pillared Bentonite. Open Journal of Physical Chemistry, 4, 98-116. doi: 10.4236/ojpc.2014.43013.

References

[1]   Brindley, G.W. and Sempels, R.E. (1977) Preparation and Properties of Some Hydroxy-Aluminum Beidellites. Clay Minerals, 12, 229-237. http://dx.doi.org/10.1180/claymin.1977.012.3.05

[2]   Barrer, R.M. (1989) Shape-Selective Sorbents Based on Clay Minerals: A Review. Clays Clay Minerals, 37, 381-395. http://dx.doi.org/10.1346/CCMN.1989.0370501

[3]   Bergaya, F., Hassoun, N., Barrault, J. and Gatineau, L. (1993) Pillaring of Synthetic Hectorite by Mixed [Al13?xFex] Pillars. Clay Minerals, 28, 109-122. http://dx.doi.org/10.1180/claymin.1993.028.1.10

[4]   Bergaya, F. (1994) Focus on Pillaring and Mixed Al13-xFex PILCs. CEA-PLS Newsletter, 7, 11-12.

[5]   Beneke, K., Thiesen, P. and Lagaly, G. (1995) Synthesis and Properties of the Sodium-Lithium Silicate Silinaite. Inorganic Chemistry, 34, 900-907. http://dx.doi.org/10.1021/ic00108a022

[6]   Pinnavaia, T.J., Tzou, M.S., Landau, S.D. and Raythatha, R.H. (1984) On the Pillaring and Delamination of Smectite Clay Catalyst by Polyoxo Cations of Aluminium. Journal of Molecular Catalysis, 27, 195-212. http://dx.doi.org/10.1016/0304-5102(84)85080-4

[7]   Lahav, N., Sham, U. and Shabtai, J. (1978) Cross-Linked Smectites. I. Synthesis and Properties of Hydrox-Aluminum-Montmorillonite. Clays Clay Minerals, 26, 107-115.
http://dx.doi.org/10.1346/CCMN.1978.0260205

[8]   Bergaya, F. (1995) The Meaning of Surface Area and Porosity Measurements of Clays and Pillared Clays. Journal of Porous Materials, 2, 91-96. http://dx.doi.org/10.1007/BF00486575

[9]   Tahani, A., Karroua, M., El Farissi, M., Levitz, P., Van Damme, H., Bergaya, F. and Margulies, L. (1999) Adsorption of Phenol and Its Chlorine Derivatives on PILCS and Organo-PILCS. Journal of Chemical Physics, 96, 464-469. http://dx.doi.org/10.1051/jcp:1999153

[10]   Cooper, C. and Burch, R. (1999) Mesoporous Materials for Water Treatment Processes. Water Research, 33, 3689-3694. http://dx.doi.org/10.1016/S0043-1354(99)00095-0

[11]   Danis, T.G., Albanis, T.A., Petrakis, D.E. and Pomonis, P.J. (1998) Removal of Chlorinated Phenols from Aqueous Solutions by Adsorption on Alumina Pillared Clays and Mesoporous Alumina Aluminum Phosphates. Water Research, 32, 295-302. http://dx.doi.org/10.1016/S0043-1354(97)00206-6

[12]   Dyer, A. and Gallardo, V.T. (1990) Cation and Anion Exchange Properties of Pillared Clays. In: Williams, P.A. and Hudson, M.J., Eds., Recent Developments in Ion Exchange, Springer Netherlands, Berlin, 75-84. http://dx.doi.org/10.1007/978-94-009-0777-5_8

[13]   Dyer, A., Gallardo, V.T. and Roberts, C.W. (1989) Preparation and Properties of Clays Pillared with Zirconium and Their Use in HPLC Separations. Zeolites, Facts, Figures, Future.

[14]   Konstantinuo, I.K., Albanis, T.A., Petrakis, D.E. and Pomonis, P.J. (2000) Removal of Herbicides from Aqueous Solutions by Adsorption on Al-Pillared Clays, Fe-Al Pillared Clays and Mesoporous Alumina Aluminum Phosphates. Water Research, 34, 3123-3136.
http://dx.doi.org/10.1016/S0043-1354(00)00071-3

[15]   Osorio-Revilla, G., Gallardo-Velázquez, T., López-Cortés, S. and Arellano-Cárdenas, S. (2006) Immersion Drying of Wheat Using Al-PILC, Zeolite, Clay and Sand as Particulate Media. Drying Technology, 24, 1033-1038. http://dx.doi.org/10.1080/07373930600776225

[16]   Theopharis, G.D., Triantafyllos, A.A., Dimitrios, E.P. and Philip, J.P. (1998) Removal of Chlorinated Phenols from Aqueous Solutions by Adsorption on Alumina Pillared Clays and Mesoporous Alumina Aluminum Phosphates. Water Research, 32, 295-302. http://dx.doi.org/10.1016/S0043-1354(97)00206-6

[17]   Nennemann, A., Mishael, Y., Nir, S., Rubin, B., Polubesova, T., Bergaya, F., Damme, H.V. and Lagaly, G. (2001) Clay-Based Formulations of Metolachlor with Reduced Leaching. Applied Clay Science, 18, 265-275. http://dx.doi.org/10.1016/S0169-1317(01)00032-1

[18]   Helander, I.K., Alakomi, H.L., Latva-Kala, K., Sandholm, T.M., Pol, I., Smid, E.J. and von Wright, A. (1998) Characterization of the Action of Selected Essential Oil Components on Gram-Negative Bacteria. Journal of Agricultural and Food Chemistry, 46, 3590-3595.
http://dx.doi.org/10.1021/jf980154m

[19]   Cox, S.D., Mann, C.M., Markhan, J.L., Bell, H.C., Gustafson, J.E., Warmington, J.R. and Wyllie, S.G. (2000) The Mode of Antimicrobial Action of the Essential Oil of Melaleuca alternifolia (Tea Tree Oil). Journal of Applied Microbiology, 88, 170-175. http://dx.doi.org/10.1046/j.1365-2672.2000.00943.x

[20]   Lambert, R.J.W., Skandamis, P.N., Coote, P.J. and Nychas, G.J.E. (2001) A Study of the Minimum Inhibitory Concentration and Mode of Action of Oregano Essential Oil, Thymol and Carvacrol. Journal of Applied Microbiology, 91, 453-462. http://dx.doi.org/10.1046/j.1365-2672.2001.01428.x

[21]   Walsh, S.E., Maillard, J.Y., Russel, A.D., Catrenich, C.E., Charbonneau, D.L. and Bartolo, R.G. (2003) Activity and Mechanism of Action of Selected Biocidal Agents on Gram-Positive and -Negative Bacteria. Journal of Applied Microbiology, 94, 240-247.
http://dx.doi.org/10.1046/j.1365-2672.2003.01825.x

[22]   Lis-Balchin, M. and Deans, S.G. (1997) Bioactivity of Selected Plant Essential Oils against Listeria Monocytogenes. Journal of Applied Microbiology, 82, 759-762.
http://dx.doi.org/10.1046/j.1365-2672.1997.00153.x

[23]   El-Miz, M., Salhi, S., El bachiri, A., Wathelet, J.P. and Tahani, A. (2013) Adsorption Study of Thymol on Na-Bentonite. Journal of Environmental Solution, 2, 31-37.

[24]   Platon, N., Sminiceanu, I., Miron, N.D., Muntianu, G., Zavada, R.M., Isopencu, G. and Nistor, D. (2011) Preparation and Characterization of New Products Obtained by Pillaring Process. Revista de Chimie (Bucharest), 62, 799-805.

[25]   Rybicka, E.H., Calmano, W. and Breeger, A. (1995) Heavy Metals Sorption/Desorption on Competing Clay Minerals: An Experimental Study. Applied Clay Science, 9, 369-381.
http://dx.doi.org/10.1016/0169-1317(94)00030-T

[26]   Gregg, S.J. and Sing, S.W. (1982) Adsorption, Surface Area and Porosity. Academic Press, London.

[27]   Remy, M.J., Coelho, A.C.V. and Poncelet, G. (1996) Surface Area and Microporosity of 1.8 nm Pillared Clays from the Nitrogen Adsorption Isotherm. Microporous Materials, 7, 287-297.
http://dx.doi.org/10.1016/S0927-6513(96)00021-1

[28]   Bankovi?, P., Milutinovi?, N., Rosi?, A. and Jovièi?, N.J. (2009) Structural and Textural Properties of Al, Fe Pillared Clay Catalysts, Russian. Journal of Physical Chemistry, 83, 1485.

[29]   Bankovic, P., Nikolic, A.M., Jovic, N., Dostanic, J., Cupic, Z., Loncarevic, D. and Jovanovic, D. (2009) Synthesis, Characterization and Application of Al, Fe-Pillared Clays. Acta Physica Polonica A, 4, 811-814.

[30]   Olaya, A., Moreno, S. and Molina, R. (2009) Synthesis of Pillared Clays with Al13-Fe and Al13-Fe-Ce Polymers in Solid State Assisted by Microwave and Ultrasound: Characterization and Catalytic Activity. Applied Catalysis A: General, 370, 7-15. http://dx.doi.org/10.1016/j.apcata.2009.08.018

[31]   Madejova, J., Janek, M., Komadel, P., Herbert, H.J. and Moog, H.C. (2002) FTIR Analyses of Water in MX-80 Bentonite Compacted from High Salinary Salt Solutions Systems. Applied Clay Science, 20, 255-271. http://dx.doi.org/10.1016/S0169-1317(01)00067-9

[32]   Salerno, P., Asenjo, M.B. and Mendioroz, S. (2001) Influence of Preparation Method on Thermal Stability and Acidity of Al-PILCs. Thermochimica Acta, 379, 101-109.
http://dx.doi.org/10.1016/S0040-6031(01)00608-6

[33]   Xue, W., He, H., Zhu, J. and Yuan, P. (2007) FTIR Investigation of CTAB-Al-Montmorillonite Complexes. Spectrochimica Acta Part A: Molecular and Biomolecular Spectroscopy, 67, 1030-1036.
http://dx.doi.org/10.1016/j.saa.2006.09.024

[34]   Tomul, F. and Balci, S. (2007) Synthesis and Characterization of Al-Pillared Interlayered Bentonites. G. U. Journal of Science, 21, 21-31.

[35]   Guerra, D.L., Lemos, V.P., Airoldi, C. and Angélica, R.S. (2006) Influence of the Acid Activation of Pillared Smectites from Amazon (Brazil) in Adsorption Process with Butylamine. Polyhedron, 25, 2880-2890. http://dx.doi.org/10.1016/j.poly.2006.04.015

[36]   Puls, R.W., Powell, R.M., Clark, D. and Eldred, C.J. (1991) Effects of pH, Solid/Solution Ratio, Ionic Strength, and Organic Acids on Pb and Cd Sorption on Kaolinite. Water, Air, and Soil Pollution, 57-58, 423-430. http://dx.doi.org/10.1007/BF00282905

[37]   Langmuir, I. (1918) The Adsorption of Gases on Plane Surfaces of Glass, Mica and Platinum. Journal of the American Chemistry Society, 40, 1361-1403. http://dx.doi.org/10.1021/ja02242a004

[38]   Hall, K.R., Eagleton, L.C., Acrivos, A. and Vermeulen, T. (1966) Pore and Solid-Diffusion Kinetics in Fixed-Bed Adsorption under Constant-Pattern Conditions. Industrial Engineering Chemistry Fundamentals, 5, 212-223. http://dx.doi.org/10.1021/i160018a011

[39]   Freundlich, H. (1906) über dieadsorption in l?sungen (Adsorption Insolution). Zeitschrift für Physikalische Chemie, 57, 384-470.

[40]   Treybal, R.E. (1968) Mass Transfer Operations. 2nd Edition, McGraw Hill, New York.

[41]   Ho, Y.S. and McKay, G. (1998) Sorption of Dye from Aqueous Solution by Peat. Chemical Engineering, 70, 115-124.

[42]   Temkin, M.J. and Pyzhev, V. (1960) Recent Modifications to Langmuir Isotherms. Acta Physicochimica USSR, 12, 217-222.

[43]   Cardenas, S.A., Velazquiz, T.G., Revilla, G.O., Cortez, M.D. and Perea, B.G. (2005) Adsorption of Phenol and Dichloro-Phenol from Aqueous Solutions by Porous Clay Hetero-Structure (PCH). Mexican Journal of Chemical Society, 49, 287-291.

[44]   Lagergren, S. (1898) Zur theorie der sogenannten adsorption geloester stoffe. Kungliga Svenska Vetenskapsakad, Handlingar, 24, 1-39.

[45]   Ho, Y.S. and McKay, G. (1998) Sorption of Dye from Aqueous Solution by Peat. Journal of Chemical Engineering, 70, 115-124.

[46]   Ho, Y.S. and McKay, G. (1999) The Sorption of Lead(II) Ions on Peat. Water Research, 33, 578-584. http://dx.doi.org/10.1016/S0043-1354(98)00207-3

[47]   Hameed, B.H., Salman, J.M. and Ahmad, A.L. (2009) Adsorption Isotherm and Kinetic Modeling of 2,4-D Pesticide on Activated Carbon Derived from Date Stones. Journal of Hazardous Materials, 163, 121-126. http://dx.doi.org/10.1016/j.jhazmat.2008.06.069

[48]   Ho, Y.S. and McKay, G. (2000) The Kinetics of Sorption of Divalent Metal Ions onto Sphagnum Moss Peat. Water Research, 34, 735-742. http://dx.doi.org/10.1016/S0043-1354(99)00232-8

[49]   Weber Jr., W.J. and Morris, J.C. (1963) Kinetics of Adsorption on Carbon from Solution. Journal of the Sanitary Engineering Division, 89, 31-59.

[50]   Srivastava, S.K., Tyagi, R. and Pant, N. (1989) Adsorption of Heavy Metal Ions on Carbonaceous Material Developed from the Waste Slurry Generated in Local Fertilizer Plants. Water Research, 23, 1161-1165. http://dx.doi.org/10.1016/0043-1354(89)90160-7

[51]   Igwe, J.C. and Abia, A.A. (2007) Adsorption Kinetics and Intra-Particulate Diffusivities for Bioremediation of Co(II), Fe(II) and Cu(II) Ions from Waste Water Using Modified and Unmodified Maize Cob. International Journal of Physical Sciences, 2, 119-127.

[52]   Dermirbas, E., Kobya, M., Senturk, E. and Ozkan, T. (2004) Adsorption Kinetics for the Removal of Chromium(VI) from Aqueous Solutions on the Activated Carbons Prepared from Agricultural Wastes. Water SA, 30, 533-539.