Efficient removal of reactive Blue-19 from textile wastewater by adsorption on methyl Imidazolium modified LUS-1 and MCM-48 nanoporous

Document Type : Reasearch Paper


1 Department of Chemistry, Yadegar -e- Imam Khomeini (RAH) Shahre Rey Branch, Islamic Azad University, Tehran, Iran.

2 Department of Chemistry, Savadkooh Branch, Islamic Azad University, Savadkooh, Iran.

3 School of Chemistry, College of Science, University of Tehran, Tehran, Iran.

4 Center of Excellence in Electrochemistry, School of Chemistry, College of Science, University of Tehran, Tehran, Iran.

5 Biosensor Research Center, Endocrinology & Metabolism Molecular-Cellular Sciences Institute, Tehran University of Medical Sciences, Tehran, Iran.

6 Department of Chemistry, Alzahra University, Tehran, Iran.


In this study, N-methyl-N'propyltrimethoxysilylimidazoliummodified LUS-1 and MCM-48 nonoporous materials were prepared and employed as adsorbent for removing Reactive Blue-19 from aqueous solutions.LUS-1 and MCM-48 were made based on the previous procedure and modified with N-methyl-N'propyltrimethoxysilylimidazolium chloride. XRD analyses did not show any lattice alteration between modified and unmodified adsorbents. A hexagonal mesophase structure with the P6mm symmetry for LUS-1 and IM-LUS-1, and a cubic Ia3d space group for MCM-48 and IM-MCM-48 were observed. UV/Vis spectrophotometry was used to determine of the dye concentration in the solution. Batch studies were conducted in order to find the optimum adsorption conditions and investigation of different empirical parameters like the pH impact, contact time, the amount of adsorbent, and concentration of dye on adsorption process. The best dye removal efficiency of the adsorbents were more than 93% at pH= 3.0-7.0 after about 3 min for IM-LUS-1 and after 30 min for IM-MCM-48. RB-19 dye was desorbed from both of the adsorbents with 10 mL of sodium hydroxide 2 M during 5 min. There was well match between the data and the Langmuir model with maximum adsorption capacities 476.2 mg/g IM-LUS-1 and 277.8 mg/g IM-MCM-48. The reusability of the sorbents were higher than 4 cycles. In addition, removal percent of RB-19 dye from 50 mL of real textile wastewater with 20 mg of IM-LUS-1 and IM-MCM-48 were 93.0 (± 0.6) and 90.2 (± 0.7), respectively. The results showed that this method might be appropriate for removing the pollutant dyes from textile wastewater.


[1]     Habibi S., Hajiaghababaei L., Badiei A., Yadavi M., Dehghan Abkenar S., Ganjali M. R., Mohammadi Ziarani, G., (2017), Removal of reactive black 5 from water using carboxylic acid-grafted SBA-15 nanorods. Desalination Water Treat. 95: 333-341. 
[2]     Ferreira A. M., Coutinho J. A. P., Fernandes A. M., Freire M. G., (2014), Complete removal of textile dyes from aqueous media using ionic-liquid-based aqueous two-phase systems. Sep. Purif. Technol. 128: 58–66.
[3]     Siddique M., Farooq R., Khan Z. M., Khan Z., Shaukat S. F., (2011),  Enhanced decomposition of reactive Blue 19 dye in ultrasound assisted electrochemical reactor. Ultrason. Sonochem. 18: 190–196.
[4]     Tanyildizi M. S., (2011), Modeling of adsorption isotherms and kinetics of reactive dye from aqueous solution by peanut hull. Chem. Eng. J. 168: 1234–1240.
[5]     Beltrame L. T. C., Dantas Neto A. A., Castro Dantas T. N., Barros Neto E. L., Lima F. F. S., (2005), Influence of cosurfactant in microemulsion systems for color removal from textile wastewater. J. Chem. Technol. Biotechnol. 80: 92–98.
[6]     Lin J., Zhang X., Li Z., Lei L., (2010), Biodegradation of reactive blue 13 in a two-stage anaerobic/aerobic fluidized beds system with a Pseudomonas sp. Isolate. Bioresour. Technol. 101: 34–40.
[7]     Rajkumar D., Song B. J., Kim J. G., (2007), Electrochemical degradation of Reactive Blue 19 in chloride medium for the treatment of textile dyeing wastewater with identification of intermediate compounds. Dyes Pigm. 72: 1–7.
[8]     Sandhya S., Swaminathan K., (2006), Kinetic analysis of treatment of textile wastewater in hybrid column upflow anaerobic fixed bed reactor. Chem. Eng. J. 122: 87–92.
[9]     Weber E. J., Stickney V. C., (1993), Hydrolysis kinetics of Reactive Blue 19-vinyl sulfone. Water Res. 27: 63–67.
[10]  Melo R. P. F., Barros Neto E. L., Moura M. C. P. A.,  Castro Dantas T. N., Dantas Neto A. A., Oliveira H. N. M., (2014), Removal of reactive Blue 19 using nonionic surfactant in cloud point extraction. Sep. Purif. Technol. 138: 71–76.
[11]  Rajeev J., Megha M., Shalini S., Alok M., (2007), Removal of the hazardous dye rhodamine B through photocatalytic and adsorption treatments. J. Environ. Manage. 85: 956-964.
[12]  Chang S. H., Wang K. S., Li H. C., We M. Y., Chou J. D., (2009), Enhancement of Rhodamine B removal by low-cost fly ash sorption with Fenton pre-oxidation. J. Hazard. Mater. 172: 1131-1136.
[13]  Zhao K., Zhao G., Li P., Gao J., Lv B., Li D., (2010), A novel method for photodegradation of high-chroma dye wastewater via electrochemical pre-oxidation. Chemosphere. 80: 410-415.
[14]  Kilic A., Orhan R., (2019), Removal of cationic dyes by adsorption in a single and binary system using activated carbon prepared from the binary mixture. Separation Sci. Technol. 54: 2147-2163. 
[15]  Malik R., Ramteke D. R., Wate S. R., (2007), Adsorption of malachite green on groundnut shell waste based powdered activated carbon. Waste Manage. 27: 1129-1138.
[16]  Dehghan Abkenar S., Hosseini M., Sadeghpour Karimi M., Ganjali M. R., (2019), Efficient removal of methylene blue from aqueous solution by adsorption on cerium vanadate nanoparticles. Pollution. 5: 339-349.
[17]  Adeyi A. A.,Jamil S. N. A. M., Abdullah L. C., Choong T. S. Y., Lau K. Li., Abdullah M., (2019), Adsorptive removal of methylene blue from aquatic environments using thiourea-modified poly(acrylonitrile-co-acrylic acid). Materials (Basel). 12: 1734- 1750.
[18]  Golshan Tafti A., Rashidi A., Tayebi H. A., Yazdanshenas M. E., (2018), Comparison of different kinetic models for adsorption of acid blue 62 as an environmental pollutant from aqueous solution onto mesoporous Silicate SBA-15 modified by Tannic acid. Int. J. Nano Dimens. 9: 79-88.
[19]  Nasirizadeh N., (2016), Synthesize and characterization of Aminosilane functionalized MCM-41 for removal of anionic dye: Kinetic and thermodynamic study. Int. J. Nano Dimens. 7: 295-307.
[20]  Ghamkhari A., Mohamadi L., Kazemzadeh S., Zafar M. N., Rahdar A., Khaksefidi R., (2020), Synthesis and characterization of poly (styrene-block-acrylic acid) diblock copolymer modified magnetite nanocomposite for efficient removal of penicillin G. Compos. B. Eng. 182: 107643-107649.
[21]  Rahdar A., Rahdar S., Labuto G., (2020), Environmentally friendly synthesis of Fe2O3@SiO2 nanocomposite: characterization and application as an adsorbent to aniline removal from aqueous solution. Environ. Sci. Pollut. Res. 27: 9181-9191.
[22]  Rahdar S., Rahdar A., Zafar M. N., Shafqat S. S., Ahmadi S., (2019), Synthesis and characterization of MgO supported Fe–Co–Mn nanoparticles with exceptionally high adsorption capacity for Rhodamine B dye. J. Mater. Res. Technol. 8: 3800-3810.
[23]  Ahmadi S., Mohammadi L., Rahdar A., Rahdar S., Dehghani R., Igwegbe C. A., Kyzas G. Z., (2020), Acid dye removal from aqueous solution by using neodymium (III) oxide nanoadsorbents. Nanomater. 10: 556-561.‎
[24]  Forgacs E., Cserhati T., Oros G., (2004), Removal of synthetic dyes from wastewaters: a review.   Environ. Int. 30: 953-971.
[25]  Messina P. V., Schulz P. C., (2006), Adsorption of reactive dyes on titania-silica mesoporous materials.  J. Colloid Interf. Sci. 299: 305-320.
[26]  Wang S., Zhu Z. H., (2006), Characterisation and environmental application of an Australian natural zeolite for basic dye removal from aqueous solution. J. Hazard. Mater. B. 136: 946-952.
[27]  Arab A., Hajiaghababaei L., Badiei A., Karimi M., Ganjali M. R., Mohammadi Ziarani G., (2019), 8-Hydroxyquinoline grafted nanoporous SBA-15 as a novel solid phase extractor for preconcentration of trace amount of Copper. Int. J. Nano Dimens. 10: 340-349.
[28]  Hajiaghababaei L., Abozari S., Badiei A., Zarabadi Poor P., Dehghan Abkenar S., Ganjali M. R., Mohammadi Ziarani G., (2017), Amino Ethyl-Functionalized SBA-15: A promising adsorbent for anionic and cationic dyes removal. Iran. J. Chem. Chem. Eng. 36: 97-108.
[29]  Hosseini M., Ganjali M. R., Rafiei Sarmazdeh Z., Faridbod F., Goldooz H., Badiei A., Nourozi P., Mohammadi Ziaranim G., (2013), A novel Lu3+ fluorescent nano-chemosensor using new functionalized mesoporous structures. Anal. Chim. Acta. 771: 95– 101.
[30]  Saadat A., Hajiaghababaei L., Badiei A., Ganjali M. R., Mohammadi Ziarani G., (2019), Amino functionalized silica coated Fe3O4 magnetic nanoparticles as a novel adsorbent for removal of Pb2+ and Cd2+Pollution. 5: 847-857.
[31]  Abdollahi F., Yousefi M., Hekmati M., Khajehnezhad A., Seyyed Afghahi S. S., (2020), Adsorption and photodegrading of Methylene Blue by using of BaLa‌xGdxFe12-2xO19 (x=0.2, 0.4, 0.6 and 0.8)/PANI nanocomposites. Int. J. Nano Dimens.11: 41-49.
[32]  Rajabi M., Moradi O., Mazlomifar A., (2015), Adsorption of Methyl orange dye from Water solutions by Carboxylate group functionalized multi-walled Carbon nanotubes. Int. J. Nano Dimens. 6: 227-240.
[33]  Kiani Gh., (2015), Adsorption kinetics and thermodynamics of Malachite Green from aqueous solutions onto expanded Graphite nanosheets. Int. J. Nano Dimens. 6: 55-66.
[34]  Ho K. Y.,  McKay G., Yeung K. L., (2003), Selective adsorbents from ordered mesoporous silica. Langmuir. 19: 3019 – 3024.
[35]  Salahshoor Z., Shahbazi A., (2014), Review of the use of mesoporous silicas for removing dye from textile wastewater. Eur. J. Environ. Sci. 4: 116–130.
[36]  Brunel, B., Cauvel, A., Fajula, F., DiRenzo, F., (1995), MCM-41 type silicas as supports for immobilized catalysts. Stud. Surf. Sci. Catal., 97: 173-180.
[37]  Abry S., Albela B., Bonneviot L., (2005), Toward dual function patterning onto surface of as-made mesostructured silica. Comptes Rendus Chimie. 8: 741-752.
[38]  Macquarrie D. J., Jackson D. B., Mdoe J. E. G., Clark J. H., (1999), Organomodified hexagonal mesoporous silicates.  New J. Chem. 23: 539-544.
[39]  Benhamou A., Basly J. P., Baudu M., Derriche Z., Hamacha R., (2013), Amino-functionalized MCM-41 and MCM-48 for the removal of chromate and arsenate. J. Colloid Interf. Sci. 404: 135–139.
[40]  Bonneviot L., Morin M., Badiei A., (2001), Mesostructured metal or non-metal oxides and method for making same. WO 01/55031 A1.
[41]  Hamad B., Alshebani A., Pera-Titus M., Wang S., Dalmon J. A., (2008), Synthesis and characterization of nanocomposite MCM-41 (‘LUS’) ceramic membranes. Microporous Mesop. Mater. 115: 40–50.
[42]  Rahdar S., Shikhe L., Ahmadi S., (2018), Removal of reactive Blue 19 dye using a combined sonochemical and modified pistachio Shell adsorption processes from aqueous solutions. Iran. J. Med. Sci. 6: 8-20.
[43]  Mauceca D., Suligoja A.,  Ristica A., Drazicb G., Pintarc A., Novak Tusara N., (2018), Titania versus zinc oxide nanoparticles on mesoporous silica supports as photocatalysts for removal of dyes from wastewater at neutral pH. Catal.Today. 310: 32-41. 
[44]  Monsef khoshhesab Z., Ahmadi M., (2016), Removal of reactive blue 19 from aqueous solutions using NiO nanoparticles: equilibrium and kinetic studies. Desalination Water Treat. 57: 20037-20048.
[45]  Gholami J., Badiei A., Abbasi A., Mohammadi Ziarani G., (2009), Synthesis and characterization of VOx/LUS-1 nanoporous silica and application for direct oxidation of benzene to phenol. Int. J. Chem. Tech. Res. 1: 426-429.
[46]  Badiei A., Goldooz H., Mohammadi Ziarani G., (2010), Effect of Benzyltrimethylammonium Ion as a Co-directing agent on phase transitions in a nanostructure silica/surfactant composite. E- J Chem. 7: 1407-1411.
[47]  Badiei A., Gholami J., Khaniani Y., (2009), Synthesis and characterization of Titanium supported on high order nanoporous silica and application for direct oxidation of benzene to phenol. E- J Chem. 6: S324-S328.
[48]  Valkenberg M. H., deCastro C., Hölderich W. F., (2001), Immobilisation of chloroaluminate ionic liquids on silica materials. Top. Catal. 14: 139–144.
[49]  Langmuir I., (1918), The adsorption of gases on plane surfaces of glass, mica and platinum. J. Am. Chem. Soc. 40: 1361-1403.
[50]  Freundlich H. M. F., (1906), Over the adsorption in solution. J. Phys. Chem. 57: 385-470.
[51]  Temkin M. I., Pyzhev V., (1940), Kinetics of ammonia synthesis on promoted iron catalysts. Acta Physiochim. USSR. 12: 327-356.
[52]  Zarezadeh-Mehrizi M., Badiei A., Rashidi Mehrabadi A., (2013), Ionic liquid functionalized nanoporous silica for removal of anionic dye. J. Mol. Liq. 180: 95–100.