ࡱ>   @LMbjbjVV 1Tr<r<)::::^^^r))))TN*4r E>*****.. .DDDDDDD$JGRIt'D^1}..11'D::**D(;;;1T:*^*D;1D;;6A^B ** @`g)*6DB}CD< EB@Jn8.J8Crr::::J^Cx.]/|;/d=0...'D'Drr v$;rrv$ PRECIPITATION OF MESOPOROUS NANOSIZED CALCIUM CARBONATE J. Kontrec, M. Ukrainczyk, Lj. Bre evi, D. Kralj Laboratory for Precipitation Processes, Ruer Boakovi Institute, Zagreb, Croatia (jasminka.kontrec@irb.hr) Keywords: calcium carbonate, nanoparticles, porous material Mesoporous calcium carbonate particles of nanosized dimensions were produced by bubbling CO2 gas through a suspension of calcium hydroxide. The precipitates were formed through initial generation of an amorphous precursor phase on the surface of Ca(OH)2 particles, its transformation into nanosized crystalline calcite and finally by aggregation into nanostructural mesoporous calcite particles. The structure and morphology of the product were investigated by using scanning and transmission electron microscopy, X-ray diffraction, specific surface area and porosity measurements. The mean particle diameter was found to be approximately 150 nm with the pore size of about 50 nm. Introduction Calcium carbonate is an extremely versatile filler and pigment that is utilized in a wide variety of products including paper, plastics, rubber and pharmaceuticals. Its final application is determined by different physical and chemical properties. In the last years, an interest for preparation of hollow particles appeared. Such particles can be used as the capsule agents for drug delivery, catalysis, coatings, composite materials and protecting sensitive agents, such as enzymes and proteins.(1-3( Up to now several methods have been applied for hollow particles creation. The methods are based on templating principle, with either hard or soft templates. The hard templating method involves the incorporation/encapsulation of various substances into solid particles/capsules.(4,5( The soft templating methods are the double emulsion route(6( and the bubble templating method. (7-8( In this method CO2 gas plays the role of reactant and also the template. The prinicple advantage of the bubble template method is that no subsequent decomposition or removal of the template is needed. A number of studies, using organic additives, have been carried out in order to successfully prepare calcium carbonate of hollow or porous structure.(9,10( In this work we report the preparation of porous calcium carbonate nanoparticles via carbonation of slaked lime, i.e. bubbling CO2 gas through an aqueous Ca(OH)2 suspension. In this way any possible side-effect of ions other than the calcium carbonate constituent ions was avoided. 2. Experimental Calcium carbonate preparation was performed in a 300 cm3 double-walled glass reactor equipped with two vertical baffle plates to prevent the vortex formation during stirring and a flat-bladed stirrer with two perpendicular blades (n = 300 min-1) of diameter being 1/3 of the reactor diameter. CO2 gas was introduced into the vessel through the nozzles placed at the bottom of the two baffles. The flow rate of CO2 was kept constant, Q = 820 cm3 min-1. Initially, the reactor was filled with 200 cm3 of deionised water, saturated with CO2 gas (100% CO2, Messer). The suspension of Ca(OH)2 (p.a., Merck) was injected into water saturated with CO2, so that the initial mass concentration in the system varied in the range 13.0 g dm-3 > ((Ca(OH)2) > 28.6 g dm-3. The propagation of the reaction was followed by measuring the electrical conductivity of the reaction mixture, 25 (normalized to the value which refers to 25 C). The temperature was kept constant during each experiment in the range 25 %C <  < 45 %C. At the end of each experiment, the obtained suspension was treated in a centrifuge for 10 min, nc = 4000 min-1. The precipitate was washed with deionized water, separated and dried at 105 %C for three hours. Samples were analyzed by means of scanning electron microscopy, transmission electron microscopy, FT-IR, spectroscopy, X-ray powder diffraction and by measuring the specific surface area and pore size distributions. 3. Results and discussion The results of mineralogical analyses of the final products (FT-IR and XRD analyses) showed that calcite was the only CaCO3 polymorph obtained at the end of each carbonation experiment. By comparison of experiments performed at different temperatures it was evident that the measured specific surface area of CaCO3 particles decreases with increasing the temperature. The highest specific surface area, S = 25.7 m2 g-1, was obtained for the sample prepared at 25 oC and the highest mass concentration of Ca(OH)2. Figure 1 illustrates particles of this sample, which are porous and rhombohedral in shape. This SEM image together with particle size distribution histograms, shown in Figure 2, demonstrate that the mean diameter of the CaCO3 particles is approximately 150 nm. Figure 1 Scanning electron micrograph of PCC sample prepared at 25 C and initial mass concentration g = 28.6 g dm-3 of Ca(OH)2,  The average crystal size estimated using the Scherrer formula from the broadening of the XRD peaks was found to be D = 52 nm (FWHM = 0.2367 at (104) diffraction peak). The particle size revealed from SEM are larger than the crystal size calculated from XRD pattern, which indicates that the calcite particles may arrange and form cubic aggregates with porous structure. Figure 3 shows the pore size distribution in CaCO3 particles. The average pore size is about 50 nm. The obtained results seem to suggest that the precipitation process is most probably controlled by the formation of amorphous calcium carbonate. It is believed that amorphous calcium carbonate nanoparticles precipitate on the suspended Ca(OH)2 particles. Since the precursor is extremely unstable it rapidly transforms into stable calcite. Dissolution of the Ca(OH)2 core particles and transformation of precursor phase results in the formation of nanoporous structure of calcite particles.  EMBED Origin50.Graph Figure 2 Particle size distribution histogram of PCC sample prepared at 25 C and initial mass concentration of Ca(OH)2, g = 28.6 g dm-3.Figure 3 Pore size distribution in PCC sample prepared at 25 C and initial mass concentration of Ca(OH)2, g = 28.6 g dm-3. 4. Conclusion Porous CaCO3 nanoparticles are successfully synthesized by bubbling CO2 gas through an aqueous suspension of Ca(OH)2. The particles prepared in this way are pure calcium carbonate of high crystallinity and purity. The mean particle diameter is approximately 150 nm with pore size of about 50 nm. The mechanism of the formation of such particles is discussed. 5. 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