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Title: Diffusion of ion-exchanging electrolytes in montmorillonite gels

Thesis/Dissertation ·
OSTI ID:7079699

The primary contributions of this work are: (1) Development of a unique radially perfused diffusion cell suitable for measuring transient diffusion rates in compacted, highly adsorbing and swelling porous media such as montmorillonite clay gels; (2) examination of the effective diffusion coefficient (D{sub 6}) of electrolytes in montmorillonite clay gels; and (3) Measurement of the transient diffusion rates of cesium, chloride and tritium in 15 w/o montmorillonite clay gels at pH 9 and sodium chloride backgrounds of 10{sup {minus}1} to 10{sup {minus}3} kmol/m{sup 3}. Results are interpreted by using the dilute limit of the multicomponent transport equations derived for species migration in a single clay pore after macroscopic averaging. The tortuosity of the clay gel is found by tritium diffusion. Transient chloride diffusion rates are found to be at molecular rates. Negative adsorption of anions from the clay gel, required for an a priori prediction of chloride profiles, are calculated from site-binding theory. Surface diffusion is the primary mode of cesium transport in montmorillonite clay gels. Migration of cesium is primarily along the inner Helmholtz plane of clay particles. The primary implication for the montmorillonite clay-based packing as a nuclear waste migration barrier is that surface diffusion must be included to describe properly diffusion rates of either anions or cations. Currently surface diffusion is neglected and cesium penetration into the packing is drastically underestimated. Penetration depths of anions is grossly overestimated. In either case, the appropriate diffusion coefficient of ions in compacted packing will be in considerable error relative to current design recommendations.

Research Organization:
California Univ., Berkeley, CA (USA)
OSTI ID:
7079699
Resource Relation:
Other Information: Thesis (Ph. D.)
Country of Publication:
United States
Language:
English