Basis sets for ab initio periodic Hartree-Fock studies of zeolite/adsorbate interactions: He, Ne, and Ar in silica sodalite

Journal Article · Fri Nov 15 04:00:00 EST 1996 · International Journal of Quantum Chemistry

DOI:https://doi.org/10.1002/(SICI)1097-461X(1996)60:4<809::AID-QUA3>3.3.CO;2-F· OSTI ID:486254

Nada, R; Nicholas, J B; McCarthy, M I; Hess, A C ^[1]

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1. Pacific Northwest National Lab., Richland, WA (United States)

Silica sodalite is an ideal model system to establish base-line computer requirements of ab initio periodic Hartree-Fock (PHF) calculations of zeolites. In this article, the authors investigate the effect of various basis sets on the structural and electronic properties of bulk silica sodalite. They also study the interaction of He, Ne, and Ar with the sodalite cage. This work shows that basis-set superposition errors (BSSE) in calculations using STO-3G and 6-21G(*) basis sets are as large as the interaction energies, leading to poor confidence in the results. To cure this problem, the authors present high-quality basis sets for si, O, He, Ne, and Ar, optimized for use with PHF methods, and demonstrate that the new basis set greatly reduces BSSE. The theoretical barriers for transfer of the rare gases between sodalite cages are 5.6, 13.2, and 62.1 kcal/mol for He, Ne, and Ar. 27 refs., 6 figs., 8 tabs.

• DOE Contract Number: AC06-76RL01830
• OSTI ID: 486254
• Journal Information: International Journal of Quantum Chemistry, Journal Name: International Journal of Quantum Chemistry Journal Issue: 4 Vol. 60; ISSN IJQCB2; ISSN 0020-7608
• Country of Publication: United States
• Language: English

Related Subjects

40 CHEMISTRY
ADSORPTION
ARGON
HARTREE-FOCK METHOD
HELIUM
MATHEMATICAL MODELS
NEON
SILICA
SORPTIVE PROPERTIES
ZEOLITES