SYNTHESIS OF GRANULAR LOW-MODULUS ZEOLITES FROM METAKAOLIN USING MECHANOCHEMICAL ACTIVATION AND ULTRASONIC TREATMENT
Abstract
The process of synthesis of granular low-modulus zeolites from a mixture of metakaolin and solid sodium hydroxide depending on the method of pre-treatment (mechanochemical activation or ultrasonic treatment) has been investigated. The vibration roller-ring mill VM-4 (vibration frequency 930 min–1) was used for mechanochemical activation (MCA) of the powder mixtures. Ultrasonic treatment of the aqueous suspensions was carried out in the ultrasonic disperser UD-20 (oscillation frequency 22 kHz). X-ray analysis of the samples was performed on DRON-3M diffractometer using CuKα radiation. Identification of crystalline phases was carried out using ASTM and IZA databases. The size of the coherent scattering region and the value of the microdeformations were calculated from the broadening of the reflections. Scanning electron microscopy was performed on JSM-6460 LV. Infrared spectra of the samples were obtained on Fourier spectrometer AVATAR 360 FT-IR. It was established that Na2Al2O4 and SiO2 are formed in the system after MCA as a result of leaching, and after UST, Na2Al2O4 is formed only. It was shown that thermal treatment at 650 °C of the mixture after mechanochemical activation and ultrasonic treatment leads to the synthesis of sodium aluminosilicates of cubic syngony, but with different parameters of the crystal lattice. Thermal treatment of the mixture without treatment gives the formation of sodium aluminosilicates and silicon oxide. It was found that after hydrothermal crystallization in NaOH solution with a concentration of 2 mol l–1, the LTA zeolite is synthesized. Crystallization in an alkali solution with a concentration of 6 mol l–1 gives the formation of SOD. It was ascertained that the use of ultrasonic treatment of the initial mixture results in the synthesis of a maximum amount of LTA zeolite (80 %) and SOD (98 %).
References
Breck D. Zeolite molecular sieves. Structure, chemistry and use. New York: Wiley. 1974. 781 p.
The International Zeolite Association (IZA) http://www.izastructure.org/databases/
Zeolite chemistry and catalysis. Ed. by J.A. Rabo. Washington: American Chemical Society. 1976. 924 p.
Johnson E.B.G., Arshad S.E. Hydrothermally synthesized zeolites based on kaolinite: A review. Appl. Clay Sci. 2014. P. 215–221. DOI: 10.1016/j.clay.2014.06.005.
Pavlov M.L., Travkina O.S., Kutepov B.I. Grained binderfree zeolites: Synthesis and properties. Catal. Ind. 2012. V. 4. N 1. P. 11–18. DOI: 10.1134/S2070050412010096.
Cejka J., Corma A., Zones S. Zeolites and Catalysis: Synthesis, Reactions and Applications. New York: John Wiley & Sons. 2010. 254 p.
Avvakumov E., Senna M., Kosova N. Soft mechanochemical synthesis: A Basis for New Chemical Technolo-gies. New York: Kluwer Academic Publishers. 2002. 324 p.
Prokof’ev V.Yu., Gordina N.E. Natural Mechanisms of Mechanochemical Interactions in Oxide Powders. Glass Ceram. 2014. V. 71. N 1–2. P. 10–14. DOI: 10.1007/s10717-014-9605-2.
Prokof’ev V.Yu., Gordina N.E., Zhidkova A.B. Investigation of mechanochemical synthesis of zeolite NaA made of metakaolin in the mills with shock-shear type of strain. Rus. J. Appl. Chem. 2012. V. 85. N 7. P. 1077–1082. DOI: 10.1134/S1070427212070142.
Yamamoto K., García S.E.B., Muramatsu A. Zeolite synthesis using mechanochemical reaction. Micropor. Mesopor. Mater. 2007. 101. N 1-2. P. 90–96. DOI: 10.1016/j.micromeso.2006.09.034.
Prokof’ev V.Yu., Gordina N.E., Zhidkova A.B., Efremov A.M. Mechanochemical synthesis of granulated LTA zeolite from metakaolin. J. Mater. Sci. 2012. V. 47. N 14. P. 5385–5392. DOI: 10.1007/s10853-012-6421-3.
Prokof’ev V.Yu., Gordina N.E. A study of thermal treatment and hydrothermal crystallization stages in pro-duction of granulated naa zeolite from mechanically activated metakaolin. Rus. J. Appl. Chem. 2013. V. 86. N 3. P. 332−338. DOI: 10.1134/S1070427213030075.
Prokof'ev V.Yu., Gordina N.E. Preparation of granulated LTA and SOD zeolites from mechanically activated mixtures of metakaolin and sodium hydroxide. Appl. Clay Sci. 2014. V. 101. P. 44–51. DOI: 10.1016/j.clay.2014.07.008.
Li H., Guo Z., Liu Y. The application of power ultrasound to reaction crystallization. Ultrason. Sonochem. 2006. V. 13. N. 4. P. 359–363. DOI: 10.1016/j.ultsonch.2006.01.002.
Vaičiukynienė D., Kantautas A., Vaitkevičius V., Jakevičius L., Rudžionis Ž., Paškevičius M. Effects of ultrasonic treatment on zeolite NaA synthesized from byproduct silica. Ultrason. Sonochem. 2015. V. 27. P. 515–521. DOI: 10.1016/j.ultsonch.2015.06.001.
Askari S., Alipour Sh.M., Halladj R., Farahani M.H.D.A. Effects of ultrasound on the synthesis of zeolites: a review. J. Porous Mater. 2013. V. 20. N 1. P. 285–302. DOI: 10.1007/s10934-012-9598-6.
Askari S., Alipour Sh.M., Halladj R., Farahani M.H.D.A. Effects of ultrasound on the synthesis of zeolites: a review. J. Porous Mater. 2013. V. 20. N 1. P. 285–302. DOI: 10.1007/s10934-012-9598-6.
Andaç Ö., Tatlıer M., Sirkecioğlu A., Ece I., Erdem-Şenatalar A. Effects of ultrasound on zeolite A synthesis. Micropor. Mesopor. Mater. 2015. V. 79. N 1–3. P. 225–233. DOI: 10.1016/j.micromeso.2004.11.007.
Boldyrev V.V. Experimental methods in mechanochemistry of solid inorganic substances. Novosibirsk: Nauka. 1983. 64 p. (in Russian).
Boldyrev A.I. Infrared spectra of minerals. M.: Nedra. 1976. 382 p. (in Russian).
Kul’pina Yu.N., Prokof’ev V.Yu., Gordina N.E., Khmylova O.E., Petukhova N.V., Gazakhova S.I. The use of IR spectroscopy to study the structure of low-modulus zeolites. Izv. Vyssh. Uchebn. Zaved. Khim. Khim. Tekhnol. 2017. V. 60. N 5. P. 44–60 (in Russian). DOI: 10.6060/tcct.2017605.5405.
Plusnina I.I. Infrared Spectra of Silicates. M.: Izd. MGU. 1977. 248 p. (in Russian).
