Document Type : Full article

Authors

Chemical Engineering Department, Babol Noshirvani University of Technology, Babol, Iran

Abstract

In this study, ZIF-67 was synthesized through solvothermal method to remove Cr(VI) ions from aqueous solution. To improve the structural properties of ZIF-67 and its adsorption capacity, optimization of the synthesis conditions was carried out based on maximum Cr(VI) uptake. From experiments, the optimum condition was revealed as solvent: metal ion molar ratio of 4.6:1, ligand: metal ion molar ratio of 318:1 and temperature of 23℃. The physio-chemical properties of as-synthesized ZIF-67 were investigated by BET, XRD, FTIR and FESEM analyses. Effect of adsorption pH, adsorbent dosage, initial concentration and contact time on adsorption process was investigated. Based on the results, the maximum adsorption capacity of Cr(VI) was 26.27 mg/g which was obtained at 35℃, pH= 5, adsorbent dosage of 3 g/l and initial concentration of 107.82 mg/l. The equilibrium time for Cr(VI) adsorption varied from 180 min for low initial concentration of 9 mg/L to 240 min for a high initial concentration of 90 mg/L. For the synthesized ZIF-67, maximum uptake capacity was reported 26.27 mg/g at initial concentration of 107.82 mg/l. The equilibrium data were described better by Langmuir-Freundlich isotherm model than the other models at three different temperatures. Pseudo-second-order model fitted the experimental data better than pseudo-first-order one. Adsorption thermodynamics indicated that the adsorption process was endothermic and spontaneous in nature. The regenerability of ZIF-67 was also studied in three sequential cycles and the Cr(VI) adsorption was almost retained after two cycles.

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Main Subjects

[1]      Kano, N., Tanabe, K., Pang, M., Deng, Y. and Imaizumi, H., “Biosorption of chromium from aqueous solution using chitosan”, J. Chem. Chem. Eng., 8, 1049 (2014).
[2]      Dai, J., Ren, F. and Tao, C., “Adsorption of Cr (VI) and speciation of Cr (VI) and Cr (III) in aqueous solutions using chemically modified chitosan”, International Journal of Environmental Research and Public Health, 9 (5), 1757 (2012).
[3]      Arenas, L. T., Lima, E. C., dos Santos, A. A., Vaghetti, J. C., Costa, T. M. and Benvenutti, E. V., “Use of statistical design of experiments to evaluate the sorption capacity of 1, 4-diazoniabicycle [2.2. 2] octane/silica chloride for Cr (VI) adsorption”, Colloids and Surfaces, A: Physicochemical and Engineering Aspects, 297 (1), 240 (2007).
[4]      Khedr, S., Shouman, M., Fathy, N. and Attia, A., “Effect of physical and chemical activation on the removal of hexavalent chromium ions using palm tree branches”, ISRN Environmental Chemistry, (2014).
[5]      Chen, J., Hong, X., Zhao, Y. and Zhang, Q., “Removal of hexavalent chromium from aqueous solution using exfoliated polyaniline/montmorillonite composite”, Water Science and Technology, 70 (4), 678 (2014).
[6]      Khosravi, R., Fazlzadehdavil, M., Barikbin, B. and Taghizadeh, A. A., “Removal of hexavalent chromium from aqueous solution by granular and powdered Peganum Harmala”, Applied Surface Science, 292, 670 (2014).
[7]      Teng, H., Xu, S., Zhao, C., Lv, F. and Liu, H., “Removal of hexavalent chromium from aqueous solutions by sodium dodecyl sulfate stabilized nano zero-valent iron: A kinetics, equilibrium, thermodynamics study”, Separation Science and Technology, 48 (11), 1729 (2013).
[8]      Li, X., Gao, X., Ai, L. and Jiang, J., “Mechanistic insight into the interaction and adsorption of Cr (VI) with zeolitic imidazolate framework-67 microcrystals from aqueous solution”, Chemical Engineering Journal, 274, 238 (2015).
[9]      Gheju, M. and Balcu, I., “Removal of chromium from Cr (VI) polluted wastewaters by reduction with scrap iron and subsequent precipitation of resulted cations”, Journal of Hazardous Materials, 196, 131 (2011).
[10]  Zhao, S., Chen, Z., Shen, J., Qu, Y., Wang, B. and Wang, X., “Enhanced Cr (VI) removal based on reduction-coagulation-precipitation by NaBH4 combined with fly ash leachate as a catalyst”, Chemical Engineering Journal, 322, 646 (2017).
[11]  Mamais, D., Noutsopoulos, C., Kavallari, I., Nyktari, E., Kaldis, A., Panousi, E., Nikitopoulos, G., Antoniou, K. and Nasioka, M., “Biological groundwater treatment for chromium removal at low hexavalent chromium concentrations”, Chemosphere, 152, 238 (2016).
[12]  Yang, R., Aubrecht, K. B., Ma, H., Wang, R., Grubbs, R. B., Hsiao, B. S. and Chu, B., “Thiol-modified cellulose nanofibrous composite membranes for chromium (VI) and lead (II) adsorption”, Polymer, 55 (5), 1167 (2014).
[13]  Zhang, Y., Yu, L., Wu, D., Huang, L., Zhou, P., Quan, X. and Chen, G., “Dependency of simultaneous Cr (VI), Cu (II) and Cd (II) reduction on the cathodes of microbial electrolysis cells self-driven by microbial fuel cells”,  Journal of Power Sources, 273, 1103-1113 (2015).
[14]  Rafati, L., Mahvi, A., Asgari, A. and Hosseini, S., “Removal of chromium (VI) from aqueous solutions using Lewatit FO36 nano ion exchange resin”, International Journal of Environmental Science & Technology, 7 (1), 147 (2010).
[15]  Vaiopoulou, E. and Gikas, P., “Effects of chromium on activated sludge and on the performance of wastewater treatment plants: A review”, Water Research, 46 (3), 549 (2012).
[16]  Uysal, M. and Ar, I., “Removal of Cr (VI) from industrial wastewaters by adsorption, Part I: Determination of optimum conditions”, Journal of Hazardous Materials, 149 (2), 482 (2007).
[17]  Rowsell, J. L., Spencer, E. C., Eckert, J., Howard, J. A. and Yaghi, O. M., “Gas adsorption sites in a large-pore metal-organic framework”, Science, 309 (5739), 1350 (2005).
[18]  Haque, E., Jun, J. W. and Jhung, S. H., “Adsorptive removal of methyl orange and methylene blue from aqueous solution with a metal-organic framework material, iron terephthalate (MOF-235)”, Journal of Hazardous Materials, 185 (1), 507 (2011).
[19]  Yang, D. -A., Cho, H. -Y., Kim, J., Yang, S. –T. and Ahn, W. –S., “CO2 capture and conversion using Mg-MOF-74 prepared by a sonochemical method”, Energy & Environmental Science, 5 (4), 6465 (2012).
[20]  Kim, J., Kim, S. –N., Jang, H. –G., Seo, G. and Ahn, W. –S., “CO2 cycloaddition of styrene oxide over MOF catalysts”, Applied Catalysis, A: General, 453, 175 (2013).
[21]  Rocha, J., Carlos, L. D., Paz, F. A. A. and Ananias, D., “Luminescent multifunctional lanthanides-based metal-organic frameworks”, Chemical Society Reviews, 40 (2), 926 (2011).
[22]  Achmann, S., Hagen, G., Kita, J., Malkowsky, I. M., Kiener, C. and Moos, R., “Metal-organic frameworks for sensing applications in the gas phase”, Sensors, 9 (3), 1574 (2009).
[23]  Humphrey, S. M. and Wood, P. T., “Multiple areas of magnetic bistability in the topological ferrimagnet [Co3(NC5H3(CO2)2-2,5)23-OH)2(OH2)2] ”, Journal of the American Chemical Society, 126 (41), 13236 (2004).
[24]  Horcajada, P., Chalati, T., Serre, C., Gillet, B., Sebrie, C., Baati, T., Eubank, J. F., Heurtaux, D., Clayette, P. and Kreuz, C., “Porous metal-organic-framework nanoscale carriers as a potential platform for drug delivery and imaging”, Nature Materials, 9 (2), 172 (2010).
[25]  Bakhtiari, N. and Azizian, S., “Adsorption of copper ion from aqueous solution by nanoporous MOF-5: A kinetic and equilibrium study”, Journal of Molecular Liquids, 206, 114 (2015).
[26]  Bertke, J. A., “Synthesis and characterization of coordination polymers and studies for carbon dioxide capture”, University of Notre Dame, (2012).
[27]  Rowsell, J. L. and Yaghi, O. M., “Metal-organic frameworks: A new class of porous materials”, Microporous and Mesoporous Materials, 73 (1), 3 (2004).
[28]  McKinstry, C., Cathcart, R. J., Cussen, E. J., Fletcher, A. J., Patwardhan, S. V. and Sefcik, J., “Scalable continuous solvothermal synthesis of metal organic framework (MOF-5) crystals”, Chemical Engineering Journal, 285, 718 (2016).
[29]  Qian, J., Sun, F. and Qin, L., “Hydrothermal synthesis of zeolitic imidazolate framework-67 (ZIF-67) nanocrystals”, Materials Letters, 82, 220 (2012).
[30]  Liu, Y., Hu, J., Li, Y., Shang, Y. T., Wang, J. Q., Zhang, Y. and Wang, Z. L., “Microwave assisted synthesis of metal-organic framework MIL-101 nanocrystals as sorbent and pseudostationary phase in capillary electrophoresis for the separation of anthraquinones in environmental water samples”, Electrophoresis, (2017).
[31]  Son, W. –J., Kim, J., Kim, J. and Ahn, W. –S., “Sonochemical synthesis of MOF-5”, Chemical Communications, 47, 6336 (2008).
[32]  Pirzadeh, K., Ghoreyshi, A. A., Rahimnejad, M. and Mohammadi, M., “Electrochemical synthesis, characterization and application of a microstructure Cu3(BTC)2 metal organic framework for CO2 and CH4 separation”, Korean Journal of Chemical Engineering, 1 (2018).
[33]  Yang, H., Orefuwa, S. and Goudy, A., “Study of mechanochemical synthesis in the formation of the metal-organic framework Cu3(BTC)2 for hydrogen storage”, Microporous and Mesoporous Materials, 143 (1), 37 (2011).
[34]  Lee, J., Farha, O. K., Roberts, J., Scheidt, K. A., Nguyen, S. T. and Hupp, J. T., “Metal-organic framework materials as catalysts”, Chemical Society Reviews, 38 (5), 1450 (2009).
[35]  Moggach, S. A., Bennett, T. D. and Cheetham, A. K., “The Effect of Pressure on ZIF-8: Increasing pore size with pressure and the formation of a high-pressure phase at 1.47 GPa”, Angewandte Chemie, 121 (38), 7221 (2009).
[36]  Fairen-Jimenez, D., Moggach, S., Wharmby, M., Wright, P., Parsons, S. and Duren, T., “Opening the gate: Framework flexibility in ZIF-8 explored by experiments and simulations”, Journal of the American Chemical Society, 133 (23), 8900 (2011).
[37]  Park, K. S., Ni, Z., Côté, A. P., Choi, J. Y., Huang, R., Uribe-Romo, F. J., Chae, H. K., O’Keeffe, M. and Yaghi, O. M., “Exceptional chemical and thermal stability of zeolitic imidazolate frameworks”, Proceedings of The National Academy of Sciences, 103 (27), pp. 10186-10191 (2006).
[38]  Wang, F., Tan, Y. -X., Yang, H., Zhang, H. -X., Kang, Y. and Zhang, J., “A new approach towards tetrahedral imidazolate frameworks for high and selective CO2 uptake”, Chemical Communications, 47 (20), 5828 (2011).
[39]  Shahrak, M. N., Ghahramaninezhad, M. and Eydifarash, M., “Zeolitic imidazolate framework-8 for efficient adsorption and removal of Cr (VI) ions from aqueous solution”, Environmental Science and Pollution Research, 24 (10), 9624 (2017).
[40]  Lai, L. S., Yeong, Y. F., Ani, N. C., Lau, K. K. and Shariff, A. M., “Effect of synthesis parameters on the formation of zeolitic imidazolate framework 8 (ZIF-8) nanoparticles for CO2 adsorption”, Particulate Science and Technology, 32 (5), 520 (2014).
[41]  Özgen, C., “Production and performance evaluation of ZIF-8 based binary and ternary mixed matrix gas separation membranes”, Middle East Technical University, (2012).
[42]  Venna, S. R., Jasinski, J. B. and Carreon, M. A., “Structural evolution of zeolitic imidazolate framework-8”, Journal of The American Chemical Society, 132 (51), 18030 (2010).
[43]  Cravillon, J., Nayuk, R., Springer, S., Feldhoff, A., Huber, K. and Wiebcke, M., “Controlling zeolitic imidazolate framework nano-and microcrystal formation: Insight into crystal growth by time-resolved in situ static light scattering”, Chemistry of Materials, 23 (8), 2130 (2011).
[44]  Tsai, C. -W. and Langner, E. H., “The effect of synthesis temperature on the particle size of nano-ZIF-8”, Microporous and Mesoporous Materials, 221, 8 (2016).
[45]  Jiang, Z., Li, Z., Qin, Z., Sun, H., Jiao, X. and Chen, D., “LDH nanocages synthesized with MOF templates and their high performance as supercapacitors”, Nanoscale, 5 (23), 11770 (2013).
[46]  Shao, J., Wan, Z., Liu, H., Zheng, H., Gao, T., Shen, M., Qu, Q. and Zheng, H., “Metal organic frameworks-derived Co3O4 hollow dodecahedrons with controllable interiors as outstanding anodes for Li storage”, Journal of Materials Chemistry, A, 2 (31), 12194 (2014).
[47]  Torad, N. L., Hu, M., Kamachi, Y., Takai, K., Imura, M., Naito, M. and Yamauchi, Y., “Facile synthesis of nanoporous carbons with controlled particle sizes by direct carbonization of monodispersed ZIF-8 crystals”, Chemical Communications, 49 (25), 2521 (2013).
[48]  Guo, X., Xing, T., Lou, Y. and Chen, J., “Controlling ZIF-67 crystals formation through various cobalt sources in aqueous solution”, Journal of Solid State Chemistry, 235, 107 (2016).
[49]  Shi, Z., Yu, Y., Fu, C., Wang, L. and Li, X., “Water-based synthesis of zeolitic imidazolate framework-8 for CO2 capture”, RSC Advances, 7 (46), 29227 (2017).
[50]  Yan, X., Komarneni, S., Zhang, Z. and Yan, Z., “Extremely enhanced CO2 uptake by HKUST-1 metal-organic framework via a simple chemical treatment”, Microporous and Mesoporous Materials, 183, 69 (2014).
[51]  Khoshhal, S., Ghoreyshi, A. A., Jahanshahi, M. and Mohammadi, M., “Study of the temperature and solvent content effects on the structure of Cu–BTC metal organic framework for hydrogen storage”, RSC Advances, 5 (31), 24758 (2015).
[52]  Biemmi, E., Christian, S., Stock, N. and Bein, T., “High-throughput screening of synthesis parameters in the formation of the metal-organic frameworks MOF-5 and HKUST-1”, Microporous and Mesoporous Materials, 117 (1-2), 111 (2009).
[53]  Xia, W., Zhu, J., Guo, W., An, L., Xia, D. and Zou, R., “Well-defined carbon polyhedrons prepared from nano metal-organic frameworks for oxygen reduction”, Journal of Materials Chemistry, A, 2 (30), 11606 (2014).
[54]  Juan, Y. and Ke-Qiang, Q., “Preparation of activated carbon by chemical activation under vacuum”, Environmental Science & Technology, 43 (9), 3385 (2009).
[55]  Qin, Q., Wang, Q., Fu, D. and Ma, J., “An efficient approach for Pb (II) and Cd (II) removal using manganese dioxide formed in situ”, Chemical Engineering Journal, 172 (1), 68 (2011).
[56]  El-Ashtoukhy, E. -S., Amin, N. K. and Abdelwahab, O., “Removal of lead (II) and copper (II) from aqueous solution using pomegranate peel as a new adsorbent”, Desalination, 223 (1-3), 162 (2008).
[57]  Tandon, R., Crisp, P., Ellis, J. and Baker, R., “Effect of pH on chromium (VI) species in solution”, Talanta, 31 (3), 227 (1984).
[58]  Gorzin, F. and Ghoreyshi, A. A., “Synthesis of a new low-cost activated carbon from activated sludge for the removal of Cr (VI) from aqueous solution: Equilibrium, kinetics, thermodynamics and desorption studies”, Korean Journal of Chemical Engineering, 30 (8), 1594 (2013).
[59]  Zhao, N., Wei, N., Li, J., Qiao, Z., Cui, J. and He, F., “Surface properties of chemically modified activated carbons for adsorption rate of Cr (VI)”, Chemical Engineering Journal, 115 (1), 133 (2005).
[60]  Giri, A. K., Patel, R. and Mandal, S., “Removal of Cr (VI) from aqueous solution by Eichhornia crassipes root biomass-derived activated carbon”, Chemical Engineering Journal, 185, 71 (2012).
[61]  Pirzadeh, K. and Ghoreyshi, A. A., “Phenol removal from aqueous phase by adsorption on activated carbon prepared from paper mill sludge”, Desalination and Water Treatment, 52 (34-36), 6505 (2014).
[62]  Al-Othman, Z. A., Ali, R. and Naushad, M., “Hexavalent chromium removal from aqueous medium by activated carbon prepared from peanut shell: Adsorption kinetics, equilibrium and thermodynamic studies”, Chemical Engineering Journal, 184, 238 (2012).
[63]  Yadav, S., Srivastava, V., Banerjee, S., Weng, C. -H. and Sharma, Y. C., “Adsorption characteristics of modified sand for the removal of hexavalent chromium ions from aqueous solutions: Kinetic, thermodynamic and equilibrium studies”, Catena, 100, 120 (2013).
[64]  Jung, C., Heo, J., Han, J., Her, N., Lee, S. -J., Oh, J., Ryu, J. and Yoon, Y., “Hexavalent chromium removal by various adsorbents: Powdered activated carbon, chitosan, and single/multi-walled carbon nanotubes”, Separation and Purification Technology, 106, 63 (2013).
[65]  Deng, H., Yang, L., Tao, G. and Dai, J., “Preparation and characterization of activated carbon from cotton stalk by microwave assisted chemical activation: Application in methylene blue adsorption from aqueous solution”, Journal of Hazardous Materials, 166 (2), 1514 (2009).
[66]  Lin, K. -Y. A. and Chang, H. -A., “Ultra-high adsorption capacity of zeolitic imidazole framework-67 (ZIF-67) for removal of malachite green from water”, Chemosphere, 139, 624 (2015).
[67]  Maleki, A., Hayati, B., Naghizadeh, M. and Joo, S. W., “Adsorption of hexavalent chromium by metal organic frameworks from aqueous solution”, Journal of Industrial and Engineering Chemistry, 28, 211 (2015).
[68]  Debnath, S. and Ghosh, U. C., “Kinetics, isotherm and thermodynamics for Cr (III) and Cr (VI) adsorption from aqueous solutions by crystalline hydrous titanium oxide”, The Journal of Chemical Thermodynamics, 40 (1), 67 (2008).
[69]  Huo, S. -H. and Yan, X. -P., “Metal-organic framework MIL-100 (Fe) for the adsorption of malachite green from aqueous solution”, Journal of Materials Chemistry, 22 (15), 7449 (2012).