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The water diffusion in four different, highly compacted clays [montmorillonite in the Na- and Ca-forms, illite in the Na- and Ca-forms, kaolinite, and pyrophyllite (bulk dry density rho(b)=1.85+/-0.05 gcm(3))] was studied at the atomic level by means of quasielastic neutron scattering. The experiments were performed on two time-of-flight spectrometers and at three different energy resolutions [FOCUS at SINQ, PSI (3.65 and 5.75 A), and TOFTOF at FRM II (10 A)] for reliable data analysis and at temperatures between 27 and 95 degrees C. Two different jump diffusion models were used to describe the translational motion. Both models describe the data equally well and give the following ranking of diffusion coefficients: Na-montmorillonite<or=Ca-montmorillonite<Ca-illite<Na-illite<water<or=pyrophyllite<or=kaolinite. Uncharged clays had slightly larger diffusion coefficients than that of bulk water due to their hydrophobic surfaces. The time between jumps, tau(t), follows the sequence: Ca-montmorillonite>or=Na-montmorillonite>Ca-illite>Na-illite>or=kaolinite>pyrophyllite>or=water, in both jump diffusion models. For clays with a permanent layer charge (montmorillonite and illite) a reduction in the water content by a factor of 2 resulted in a decrease in the self-diffusion coefficients and an increase in the time between jumps as compared to the full saturation. The uncharged clay kaolinite exhibited no change in the water mobility between the two hydration states. The rotational relaxation time of water was affected by the charged clay surfaces, especially in the case of montmorillonite; the uncharged clays presented a waterlike behavior. The activation energies for translational diffusion were calculated from the Arrhenius law, which adequately describes the systems in the studied temperature range. Na- and Ca-montmorillonite (approximately 11-12 kJmol), Na-illite (approximately 13 kJmol), kaolinite and pyrophyllite (approximately 14 kJmol), and Ca-illite (approximately 15 kJmol) all had lower activation energies than bulk water (approximately 17 kJmol in this study). This may originate from the reduced number and strength of the H-bonds between water and the clay surfaces, or ions, as compared to those in bulk water. Our comparative study suggests that the compensating cations in swelling clays have only a minor effect on the water diffusion rates at these high densities, whereas these cations influence the water motion in non-swelling clays.

Translational diffusion of water and its dependence on temperature in charged and uncharged clays: A neutron scattering study