Comparative quantum chemical studies in the framework of Gaussian approximations of the acidic characteristics of the simplest zeolite clusters and of the sulfuric acid molecule

Abstract

Different variants of the Gaussian approximation, giving the energetic characteristics of molecules with chemical accuracy (±2 kcal mol−1), are applied to calculations of the deprotonation energy of the sulfuric acid molecule in the gas phase as well as to the simplest clusters modeling the bridging hydroxyl groups in zeolites, The conclusion is made that the bridging hydroxyls am more acidic than the sulfuric acid molecule. The estimated range of deprotonation energy in zeolites (275±15 kcal mol−1), is in good agreement with experimental data and with results ofab initio calculations for extended models including several tens of atoms. The effects of the quality of the basis set and electron correlation on deprotonation energy are also discussed.