Single-file diffusion is the restricted propagation of particles that cannot pass each other. The occurrence of this phenomenon should be reflected by a change in the time dependence of the mean particle displacement in comparison with ordinary diffusion. Although this process is considered to be the rate-controlling mechanism in a large variety of processes, so far no direct evidence of this phenomenon has been provided. Diffusion measurements made with pulsed field gradient nuclear magnetic resonance (NMR) in unidimensional pore systems (zeolites AlPO4-5 and Theta-1) reflect the expected time dependence of single-file diffusion.
The n.m.r. pulsed field-gradient technique has been used to study systematically the intracrystalline self-diffusion of methane, ethane and propane in ZSM-5. In conjunction with the information obtained from nuclear magnetic relaxation studies the elementary steps of diffusion are found to be activated jumps between the channel intersections. Only for sorbate concentrations > 2.5 molecules per intersection is a decrease in the jump lengths observed. The results are compared with alkane self-diffusion measurements in zeolites A and X, as well as with the self-diffusion of water in ZSM-5 and zeolites A and X.
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