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High-resolution sorption studies of argon and nitrogen on large crystals of microporous zeolite ZSM-5

Sorptionsuntersuchungen zur Hochauflösung von Argon und Stickstoff an großen Kristallen von mikroporösem Zeolit ZSM-5

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Summary

High resolution adsorption (HRADS) with argon and nitrogen at 77 K were performed on large crystals of zeolite ZSM-5 using a novel volumetric device. Multi-step isotherms for both adsorptives could be observed for the first time. The micropore filling was followed by low temperature microcalorimetry. Exothermic heats of adsorption were found to be correlated with steps in the adsorption isotherms. Based on results from atom-atom potential energy calculations (AAP) as well as from independent model building it is shown that 24 kinetic adsorbate molecules can be situated in a ZSM-5 unit cell. Localized adsorption is presented as possible filling mechanisms. Experimental results are reasonably interpreted assuming primary filling of narrow channels and secondary adsorption in the wider channel intersections. At least for nitrogen there is evidence for a transition of fluid-like to a solid-like adsorbate phase.

Compared to argon, Henry's constants and the initial isosteric heat of adsorption indicate a stronger adsorption of nitrogen which is thought to be due to additional interactions of the nitrogen quadrupole moment with the zeolite framework.

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Authors and Affiliations

  1. Institut für Anorganische und Analytische Chemie, Gutenberg-Universität, P. O. Box 3980, D-6500, Mainz, Federal Republic of Germany

    U. Müller, H. Reichert, E. Robens & K. K. Unger

  2. Centre de Thermodynamique et de Microcalorimetrie du C.N.R.S., 26 Rue du 141e R.I.A., F-13003, Marseille, France

    U. Müller, H. Reichert, E. Robens, K. K. Unger, Y. Grillet, F. Rouquerol, J. Rouquerol, Dongfeng Pan & A. Mersmann

  3. Institut für Verfahrenstechnik, Lehrstuhl B, Technische Universität, Arcisstrasse 21, D-8000, München 2, Federal Republic of Germany

    Y. Grillet, F. Rouquerol, J. Rouquerol, Dongfeng Pan & A. Mersmann

Authors
  1. U. Müller
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  2. H. Reichert
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  3. E. Robens
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  4. K. K. Unger
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  5. Y. Grillet
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  6. F. Rouquerol
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  7. J. Rouquerol
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  8. Dongfeng Pan
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  9. A. Mersmann
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Müller, U., Reichert, H., Robens, E. et al. High-resolution sorption studies of argon and nitrogen on large crystals of microporous zeolite ZSM-5. Z. Anal. Chem. 333, 433–436 (1989). https://doi.org/10.1007/BF00572345

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  • DOI: https://doi.org/10.1007/BF00572345

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