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Cage occupancy and compressibility of deuterated N2-clathrate hydrate by neutron diffraction

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Citation:
Kuhs, W. F. , Chazallon, B. , Radaelli, P. G. and Pauer, F. (1997): Cage occupancy and compressibility of deuterated N2-clathrate hydrate by neutron diffraction , Journal of Inclusion Phenomena and molecular recognition in chemistry, Vol 29, no. 1, pp. 65-77 .
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Abstract:

This paper reports pressure dependent high resolution neutron diffraction work on N-2-clathrates, which for the first time provides numbers on the compressibility as well as the location and degree of filling of the guest molecules in the small and large cages. N-2-clathrates crystallize, at least at lower pressures and temperatures near 0 degrees C, in the Stackelberg type II structure. However, during the diffraction experiments we have observed the transient and partial formation of the von Stackelberg type I N-2-clathrate at pressures exceeding several hundred bar. The filling of the small cages in the type II clathrate roughly follows a Langmuir isotherm, In contrast to most previous assumptions there is strong evidence that the large cages are doubly occupied in both type I and type II N-2-clathrates. The observed filling can be fitted reasonably well by a two-constant Langmuir model.

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