Open Porosity and Pore Size Distribution of Mesoporous Silica Films Investigated by Positron Annihilation Lifetime Spectroscopy and Ellipsometric Porosimetry

Tunable mesoporous silica films were prepared though a sol-gel process directed by the self-assembly of various triblock copolymers. Positron annihilation gamma-ray energy spectroscopy and positron annihilation lifetime spectroscopy (PALS) based on intense pulsed slow positron beams as well as ellipsometric porosimetry (EP) combined with heptane adsorption were utilized to characterize the open porosity/interconnectivity and pore size distribution for the prepared films. The consistency between the open porosities was examined by the variations of orthopositronium (o-Ps) 3 gamma annihilation fractions and the total adsorbed volumes of heptane. The average pore sizes deduced by PALS from the longest-lived o-Ps lifetimes are in good agreement with those by EP on the basis of the Barrett-Joyner-Halenda model, as indicated by a well fitted line of slope k = 1. The results indicate that the EP combined with heptane adsorption is a useful method with high sensitivity for calibrating the mesopore size in highly interconnected mesoporous films, whereas PALS is a novel, complementary tool for characterizing both closed and open pores in them.

Automated summary

In this study, tunable mesoporous silica films were characterized using positron annihilation gamma-ray energy spectroscopy, positron annihilation lifetime spectroscopy, ellipsometric porosimetry, and heptane adsorption. The results showed that ellipsometric porosimetry combined with heptane adsorption is a highly sensitive method for calibrating mesopore size in interconnected films, while positron annihilation lifetime spectroscopy is a novel complementary tool for characterizing closed and open pores.