Abstract
Calix[4]arene-crown-6 compounds are promising ligands in the removal of cesium. With this aim, a macrocyclic compound, calix[4]arene-crown-6, was chemically immobilized onto inorganic ordered mesoporous carbon material. Several adsorption parameters such as nitric acid concentration, contact time, initial cesium content, operation temperature, and competing ions were studied. The results demonstrated the prepared material conserved high cesium selectivity of calix[4]arene-crown-6 and physicochemistry stability of the ordered mesoporous carbon matrix and showed the superior cesium adsorption performance. The optimum adsorption acidity determined as 3.0 M nitric acid was consistent with the actual acidity value in the back-end of the nuclear fuel cycle. The Langmuir model indicated the monolayer coverage adsorption and the highest mass adsorption capacity was calculated as 128.06 mg cesium/g. The pseudo-second-order model and D-R model proved the adsorption was a chemical process. Thermodynamics parameters showed the adsorption was spontaneous and exothermal in nature. Competing ions hardly affected cesium adsorption. Furthermore, the adsorbent showed almost intact adsorption capacity after five adsorption-elution cycles. The comprehensive performance highlights the composite material as a promising adsorbent for cesium adsorption from wastewaters.
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Aid, A., Amokrane, S., Nibou, D., Mekatel, E., Trari, M., & Hulea, V. (2018). Modeling biosorption of Cr(VI) onto ulva compressa L. from aqueous solutions. Water Science and Technology, 77, 60–69.
Awual, M. R., Hasan, M. M., Shahat, A., Naushad, M., Shiwaku, H., & Yaita, T. (2015). Investigation of ligand immobilized nano-composite adsorbent for efficient cerium (III) detection and recovery. Chemical Engineering Journal, 265, 210–218.
Baig, U., Rao, R. A. K., Khan, A. A., Sanagi, M. M., & Gondal, M. A. (2015). Removal of carcinogenic hexavalent chromium from aqueous solutions using newly synthesized and characterized polypyrrole–titanium (IV) phosphate nanocomposite. Chemical Engineering Journal, 280, 494–504.
Bedin, K. C., Martins, A. C., Cazetta, A. L., Pezoti, O., & Almeida, V. C. (2016). KOH-activated carbon prepared from sucrose spherical carbon: adsorption equilibrium, kinetic and thermodynamic studies for methylene blue removal. Chemical Engineering Journal, 286, 476–484.
Bhatti, A. A., Memon, S., & Memon, N. (2014). Dichromate extraction by calix [4] arene appended amberlite XAD-4 resin. Separation Science and Technology, 49, 664–672.
Biswas, R., Malviya, A., Banerjee, T., Ghosh, P., & Ali, S. M. (2018). Alkali metal ion partitioning with calix [4] arene-benzo-crown-6 ionophore in acidic medium: insights from a experiments, statistical mechanical framework and molecular dynamics simulations. Journal of Physical Chemistry B, 122(7), 2102–2112.
Borai, E. H., Harjula, R., & Paajanen, A. (2009). Efficient removal of cesium from low-level radioactive liquid waste using natural and impregnated zeolite minerals. Journal of Hazardous Materials, 172, 416–422.
Chen, Z., Wu, Y., & Wei, Y. (2014). Adsorption characteristics and radiation stability of a silica-based DtBuCH18C6 adsorbent for Sr(II) separation in HNO3 medium. Journal of Radioanalytical and Nuclear Chemistry, 299, 485–491.
Christensen, J. J., Hill, J. O., & Izatt, R. M. (1971). Ion binding by synthetic macrocyclic compounds. Science, 174, 459–467.
Dechojarassri, D., Asaina, S., Omote, S., Nishida, K., Furuike, T., & Tamura, H. (2017). Adsorption and desorption behaviors of cesium on rayon fibers coated with chitosan immobilized with Prussian blue. International Journal of Biological Macromolecules, 104, 1509–1516.
Erdemir, S., Tabakci, B., & Tabakci, M. (2016). A highly selective fluorescent sensor based on calix [4] arene appended benzothiazole units for Cu2+, S2− and HSO4 − ions in aqueous solution. Sensors and Actuators B: Chemical, 228, 109–116.
Etienne, M., & Walcarius, A. (2003). Analytical investigation of the chemical reactivity and stability of aminopropyl-grafted silica in aqueous medium. Talanta, 59, 1173–1188.
Fan, C., Nguyen, V., Zeng, Y., Phadungbut, P., Horikawa, T., Do, D. D., & Nicholson, D. (2015a). Novel approach to the characterization of the pore structure and surface chemistry of porous carbon with Ar, N2, H2O and CH3OH adsorption. Microporous and Mesoporous Materials, 209, 79–89.
Fan, T., Zeng, W., Tang, W., Yuan, C., Tong, S., Cai, K., Liu, Y. D., Huang, W., Min, Y., & Epstein, A. J. (2015b). Controllable size-selective method to prepare graphene quantum dots from graphene oxide. Nanoscale Research Letters, 10, 55.
Guo, G., Xu, Y., Yang, X., Wang, F., Zhou, F., Yu, J., & Chi, R. (2017). Effect of HNO3 concentration on a novel silica-based adsorbent for separating Pd (II) from simulated high level liquid waste. Scientific Reports Uk, 7, 11290.
Haddad, D., Mellah, A., Nibou, D., & Khemaissia, S. (2018). Promising enhancement in the removal of uranium ions by surface-modified activated carbons: kinetic and equilibrium studies. Journal of Environmental Engineering, 144, 04018027.
Hassan, E. (2016). Comparative study on the biosorption of Pb (II), Cd (II) and Zn (II) using lemon grass (Cymbopogon citratus): kinetics, isotherms and thermodynamics. Chemistry International, 2, 89–102.
Hong, S., Bradshaw, C. J., & Brook, B. W. (2015). Global zero-carbon energy pathways using viable mixes of nuclear and renewables. Applied Energy, 143, 451–459.
Houhoune, F., Nibou, D., Chegrouche, S., & Menacer, S. (2016). Behaviour of modified hexadecyltrimethylammonium bromide bentonite towards uranium species. Journal of Environmental Chemical Engineering., 4(3), 3459–3467.
Hu, K., Huang, X., Gao, Y., Huang, X., Xiao, H., & McClements, D. J. (2015). Core–shell biopolymer nanoparticle delivery systems: synthesis and characterization of curcumin fortified zein–pectin nanoparticles. Food Chemistry, 182, 275–281.
Husnain, S. M., Um, W., Chang, Y. Y., & Chang, Y. S. (2017). Recyclable superparamagnetic adsorbent based on mesoporous carbon for sequestration of radioactive cesium. Chemical Engineering Journal, 308, 798–808.
Jagasia, P., Ansari, S. A., Raut, D. R., Dhami, P. S., Gandhi, P. M., Kumar, A., & Mohapatra, P. K. (2016). Hollow fiber supported liquid membrane studies using a process compatible solvent containing calix [4] arene-mono-crown-6 for the recovery of radio-cesium from nuclear waste. Separation and Purification Technology, 170, 208–216.
Jaiswal, M. K., Muwal, P. K., Pandey, S., & Pandey, P. S. (2017). A novel hybrid macrocyclic receptor based on bile acid and calix [4] arene frameworks for metal ion recognition. Tetrahedron Letters, 58, 2153–2156.
Jia, Z., Cheng, X., Guo, Y., & Tu, L. (2017). In-situ preparation of iron (III) hexacyanoferrate nano-layer on polyacrylonitrile membranes for cesium adsorption from aqueous solutions. Chemical Engineering Journal, 325, 513–520.
Kim, J., Ohki, A., Ueki, R., Ishizuka, T., Shimotashiro, T., & Maeda, S. (1999). Cesium-ion selective electrodes based on calix[4]arene dibenzocrown ethers. Talanta, 48, 705–710.
Kim, J., Lee, W., Lee, S., Kim, J., Suh, I., Kim, J., & Kim, J. (2001). Cesium complex of an unsymmetrical calix [4] crown-dibenzocrown-6. Journal of Inclusion Phenomena and Macrocyclic Chemistry, 40, 183–187.
Kim, H., Kang, S. O., Park, S., & Park, H. S. (2015). Adsorption isotherms and kinetics of cationic and anionic dyes on three-dimensional reduced graphene oxide macrostructure. Journal of Industrial and Engineering Chemistry, 21, 1191–1196.
Kocyigit, O., Erdemir, S., & Yilmaz, M. (2012). Sorption of Cu(II) onto silica gel immobilized calix [4] arene derivative with tripodal structure. Journal of Inclusion Phenomena and Macrocyclic Chemistry, 72, 137–147.
Kok, B., & Benli, H. (2017). Energy diversity and nuclear energy for sustainable development in Turkey. Renewable Energy, 111, 870–877.
Kudo, T., Ito, T., & Kim, S. Y. (2017). Adsorption behavior of Sr(II) from high-level liquid waste using crown ether with ionic liquid impregnated silica adsorbent. Energy Procedia, 131, 189–194.
Li, Z., Pranolo, Y., Zhu, Z., & Cheng, C. Y. (2017). Solvent extraction of cesium and rubidium from brine solutions using 4-tert-butyl-2-(α-methylbenzyl)-phenol. Hydrometallurgy, 171(1–7).
Lindley, B. A., Fiorina, C., Gregg, R., Franceschini, F., & Parks, G. T. (2016). The effectiveness of full actinide recycle as a nuclear waste management strategy when implemented over a limited timeframe–part II: thorium fuel cycle. Progress in Nuclear Energy, 87, 144–155.
Liu, H., Xie, S., Wang, T., Liu, Y., & Zeng, T. (2017). Effect of coexisting cations on the adsorption of cesium onto poly (β-cyclodextrin)/bentonite composite. Journal of Radioanalytical and Nuclear Chemistry, 312, 557–565.
Lo, P., & Wong, M. (2008). Extended calix[4]arene-based receptors for molecular recognition and sensing. Sensors, 8, 5313–5335.
Luo, H., Dai, S., Bonnesen, P. V., Buchanan, A. C., Holbrey, J. D., Bridges, N. J., & Rogers, R. D. (2004). Extraction of cesium ions from aqueous solutions using calix [4] arene-bis (tert-octylbenzo-crown-6) in ionic liquids. Analytical Chemistry, 76, 3078–3083.
Makrlík, E., & Vaňura, P. (2018). Synergistic extraction of some univalent cations into phenyltrifluoromethyl sulfone by using cesium dicarbollylcobaltate and calix [4] arene-bis (t-octylbenzo-18-crown-6). Journal of Molecular Liquids, 250, 100–102.
Nayak, P. K., Kumaresan, R., Chaurasia, S., Venkatesan, K. A., Subramanian, G. G. S., Prathibha, T., Syamala, K. V., Selvan, B., Rajeswari, S., Antony, M. P., Vasudeva, Rao, P. V., & Bhanage, B. M. (2015). Studies on the feasibility of using completely incinerable reagents for the single-cycle separation of americium (III) from simulated high-level liquid waste. Radiochimica Acta, 103, 265–275.
Nibou, D., Khemaissia, S., Amokrane, S., Barkat, M., Chegrouche, S., & Mellah, A. (2011). Removal of UO2 2+ onto synthetic NaA zeolite. Characterization, equilibrium and kinetic studies. Chemical Engineering Journal, 172, 296–305.
Ning, S., Zou, Q., Wang, X., Liu, R., Wei, Y., Zhao, Y., & Ding, Y. (2016). Evaluation study on silica/polymer-based CA-BTP adsorbent for the separation of minor actinides from simulated high-level liquid wastes. Journal of Radioanalytical and Nuclear Chemistry, 307, 993–999.
Ofomaja, A. E., Pholosi, A., & Naidoo, E. B. (2015). Application of raw and modified pine biomass material for cesium removal from aqueous solution. Ecological Engineering, 82, 258–266.
Park, Y., Lee, Y. C., Shin, W. S., & Choi, S. J. (2010). Removal of cobalt, strontium and cesium from radioactive laundry wastewater by ammonium molybdophosphate–polyacrylonitrile (AMP–PAN). Chemical Engineering Journal, 162, 685–695.
Park, Y., Shin, W. S., & Choi, S. J. (2013). Ammonium salt of heteropoly acid immobilized on mesoporous silica (SBA-15): an efficient ion exchanger for cesium ion. Chemical Engineering Journal, 220, 204–213.
Qian, J., Cai, S., Yang, S., & Hua, D. (2017). A thermo-sensitive polymer network crosslinked by Prussian blue nanocrystals for cesium adsorption from aqueous solution with large capacity. Journal of Materials Chemistry, A, 5, 22380–22388.
Roach, B. D., Williams, N. J., & Moyer, B. A. (2015). Thermal degradation of the solvent employed in the next-generation caustic-side solvent extraction process and its effect on the extraction, scrubbing, and stripping of cesium. Solvent Extraction and Ion Exchange, 33, 576–591.
Rogelj, J., Luderer, G., Pietzcker, R. C., Kriegler, E., Schaeffer, M., Krey, V., & Riahi, K. (2015). Energy system transformations for limiting end-of-century warming to below 1.5 C. Nature Climate Change, 5, 519–527.
Roosen, J., Mullens, S., & Binnemans, K. (2017). Chemical immobilization of 8-hydroxyquinoline and 8-hydroxyquinaldine on chitosan-silica adsorbent materials for the selective recovery of gallium from Bayer liquor. Hydrometallurgy, 171, 275–284.
Sepehri, S., Rezaei, M., & Garbarino, G. (2016). Facile synthesis of a mesoporous alumina and its application as a support of Ni-based autothermal reforming catalysts. International Journal of Hydrogen Energy, 41(5), 3456–3464.
Shizuma, K., Fujikawa, Y., Kurihara, M., & Sakurai, Y. (2018). Identification and temporal decrease of 137Cs and 134Cs in groundwater in Minami-Soma City following the accident at the Fukushima Dai-ichi nuclear power plant. Environmental Pollution, 234, 1–8.
Soliman, M. A., Rashad, G. M., & Mahmoud, M. R. (2015). Fast and efficient cesium removal from simulated radioactive liquid waste by an isotope dilution–precipitate flotation process. Chemical Engineering Journal, 275, 342–350.
Sun, C., Zhang, F., Wang, X., & Cheng, F. (2015). Facile preparation of ammonium molybdophosphate/Al-MCM-41 composite material from natural clay and its use in cesium ion adsorption. European Journal of Solid State and Inorganic Chemistry, 2015, 2125–2131.
Tanhaei, B., Ayati, A., Lahtinen, M., & Sillanpää, M. (2015). Preparation and characterization of a novel chitosan/Al2O3/magnetite nanoparticles composite adsorbent for kinetic, thermodynamic and isotherm studies of methyl orange adsorption. Chemical Engineering Journal, 259, 1–10.
Thuéry, P., Nierlich, M., Lamare, É., Dozol, J. F., Asfari, Z., & Vicens, J. (2000). Bis(crown ether) and azobenzocrown derivatives of calix[4]arene. A review of structural information from crystallographic and modelling studies. Journal of Inclusion Phenomena and Macrocyclic Chemistry, 4, 375–408.
Uddin, M. K. (2017). A review on the adsorption of heavy metals by clay minerals, with special focus on the past decade. Chemical Engineering Journal, 308, 438–462.
Vargas, A., Camacho, A., Laubenstein, M., & Plastino, W. (2016). Dry deposition velocity of 137Cs and 134Cs in Spain after the Fukushima Dai-Ichi nuclear power plant accident. Applied Radiation and Isotopes, 109, 441–443.
Wang, Y., Liu, Z., Li, Y., Bai, Z., Liu, W., Wang, Y., Xu, X., Xiao, C., Sheng, D., Diwu, J., Su, J., Chai, Z., Albrecht-Schmitt, T. E., & Wang, S. A. (2015a). Umbellate distortions of the uranyl coordination environment result in a stable and porous polycatenated framework that can effectively remove cesium from aqueous solutions. Journal of the American Chemical Society, 137, 6144–6147.
Wang, Y., Shi, L., Gao, L., Wei, Q., Cui, L., Hu, L., Yan, L., & Du, B. (2015b). The removal of lead ions from aqueous solution by using magnetic hydroxypropyl chitosan/oxidized multiwalled carbon nanotubes composites. Journal of Colloid and Interface Science, 451, 7–14.
Yamauchi, S., Yamagishi, T., Kirikoshi, K., & Yatagai, M. (2015). Cesium adsorption from aqueous solutions onto Japanese oak charcoal II: effects of metal ions eluted from the charcoal. Journal of Wood Science, 61, 185–191.
Zhang, A., & Hu, Q. (2010). Adsorption of cesium and some typical coexistent elements onto a modified macroporous silica-based supramolecular recognition material. Chemical Engineering Journal, 159, 58–66.
Zhang, H., Zhao, X., Wei, J., & Li, F. (2015). Removal of cesium from low-level radioactive wastewaters using magnetic potassium titanium hexacyanoferrate. Chemical Engineering Journal, 275, 262–270.
Zhang, A., Chen, C., Wang, Y., & Gao, T. (2016). Adsorption of cesium and some typical elements on a novel solid-state macroporous silica-calix [4] arene material. Separation Science and Technology, 51, 1962–1970.
Zheng, T., Yang, Z., Gui, D., Liu, Z., Wang, X., Dai, X., Liu, S., Zhang, L., Gao, Y., Chen, L., Sheng, D., Wang, Y., Diwu, J., Wang, J., Zhou, R., Chai, Z., Albrecht-Schmitt, T. E., & Wang, S. A. (2017a). Overcoming the crystallization and designability issues in the ultrastable zirconium phosphonate framework system. Nature Communications, 8, 15369.
Zheng, Y., Qiao, J., Yuan, J., Shen, J., Wang, A. J., & Niu, L. (2017b). Electrochemical removal of radioactive cesium from nuclear waste using the dendritic copper hexacyanoferrate/carbon nanotube hybrids. Electrochimica Acta, 257, 172–180.
Acknowledgments
The present work was funded by the National Natural Science Foundation of China (No. 11605027, 11705060, 41361088), the Project of the Jiangxi Provincial Department of Education (No. GJJ170400), and Natural Science Foundation of Jiangxi Province (No. 20161BAB213086).
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Tao, Q., Wang, X., Huang, D. et al. Adsorption of Cesium from Aqueous Solution of Highly Concentrated Nitric Acid Using Supermolecule/Ordered Mesoporous Carbon Composite. Water Air Soil Pollut 229, 361 (2018). https://doi.org/10.1007/s11270-018-4016-6
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DOI: https://doi.org/10.1007/s11270-018-4016-6