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Comparison of factors influencing acidity of hydroxyl groups in zeolites. Quantum chemical study

Journal Article · · Journal of Physical Chemistry; (USA)
DOI:https://doi.org/10.1021/j100364a057· OSTI ID:6731446
 [1]
  1. J. Heyrovsky Institute of Physical Chemistry and Electrochemistry, Prague (Czechoslovakia)

The nonempirical quantum chemical method with a STO-3G basis set is employed to study the effect of changes in the chemical composition of the environment of the {r arrow}Si-OH-Al{l arrow} fragment in zeolites on the acidity of the bridging OH groups modeled by the H-OX-TH{sub 2}-O-SiH{sub 2}-OH-AlH{sub 3} molecule model (T = Si or Al and X = H or Na). It is shown that the substitution of Si by Al (i.e., variation in the Si/Al ratio) is the most important factor influencing the OH group acidity. Its effect on the acidity is approximately twice as great as the effect of substitution of H by Na (i.e., variation in the degree of decationization). The bridging OH groups in immediate proximity to a terminal OH group were calculated to be somewhat more acidic than the OH groups surrounded by only Si or Al atoms. Neutral oxide-like species of metals occluded in the zeolite pores were found to increase the acidity of the adjacent OH groups.

OSTI ID:
6731446
Journal Information:
Journal of Physical Chemistry; (USA), Journal Name: Journal of Physical Chemistry; (USA) Vol. 94:1; ISSN 0022-3654; ISSN JPCHA
Country of Publication:
United States
Language:
English