科研之友
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摘要
We report results of nitrogen and argon adsorption experiments performed at 77.4 and 87.3 K on novel micro/ mesoporous silica materials with morphologically different networks of mesopores embedded into microporous matrixes: SE3030 silica with wormlike cylindrical channels of mode diameter of similar to 95 A, KLE silica with cagelike spheroidal pores of ca. 140 angstrom, KLEAL silica with spheroidal pores of similar to 140 angstrom connected by cylindrical channels of similar to 26 angstrom, and, also for a comparison, on Vycor glass with a disordered network of pores of mode diameter of similar to 70 angstrom. We show that the type of hysteresis loop formed by adsorption/desorption isotherms is determined by different mechanisms of condensation and evaporation and depends upon the shape and size of pores. We demonstrate that adsorption experiments performed with different adsorptives allow for detecting and separating the effects of pore blocking/percolation and cavitation in the course of evaporation. The results confirm that cavitation-controlled evaporation occurs in ink-bottle pores with the neck size smaller than a certain critical value. In this case, the pressure of evaporation does not depend upon the neck size. In pores with larger necks, percolation-controlled evaporation occurs, as observed for nitrogen (at 77.4 K) and argon (at 87.3 K) on porous Vycor glass. We elaborate a novel hybrid nonlocal density functional theory (NLDFT) method for calculations of pore size distributions from adsorption isotherms in the entire range of micro- and mesopores. The NLDFT method, applied to the adsorption branch of the isotherm, takes into account the effect of delayed capillary condensation in pores of different geometries. The pore size data obtained by the NLDFT method for SE3030, KLE, and KLE/IL silicas agree with the data of SANS/SAXS techniques.
- 出版日期2006-1-17
