Issue 12, 1989

Molecular self-diffusion of methane in zeolite ZSM-5 by quasi-elastic neutron scattering and nuclear magnetic resonance pulsed field gradient technique

Abstract

The translational mobility of methane sorbed on an NaZSM-5 sample of proven crystallinity has been studied by quasi-elastic neutron scattering (QENS) and an n.m.r. pulsed field gradient technique (n.m.r. PFGT) at different loadings and temperatures. In both methods, long-range self-diffusion is detected. However, owing to the different timescales of the two experimental methods applied, the mean diffusion paths followed are of different magnitude: in QENS, molecular translation is measured up to 6nm; in n.m.r. PFGT, the mean molecular displacements amount to some µm. Nevertheless, since the r.m.s. molecular displacements followed by both methods considerably exceed the distances between the pore intersections of the ZSM-5 channel network, in both techniques the translational self-diffusion coefficient of guest molecules inside the zeolite pores is detected. For the intracrystalline self-diffusion coefficient, D, as well as for the activation energy of self-diffusion, Ea, the values determined by the two independent methods agree very well. In the temperature region 200–250 K, the intracrystalline self-diffusion coefficients of methane in ZSM-5 are found to be of the order of 10–5–10–4 cm2 s–1, with only slight concentration and temperature dependence. The activation energy determined by both methods amounts to 4–5 kJ mol–1. Further agreement between QENS and n.m.r. PFGT is obtained by comparing the mean molecular jump lengths, which by both techniques are found to be ca. 1 nm for light hydrocarbons in ZSM-5, slightly decreasing with increasing loading.

Article information

Article type
Paper

J. Chem. Soc., Faraday Trans. 1, 1989,85, 4201-4209

Molecular self-diffusion of methane in zeolite ZSM-5 by quasi-elastic neutron scattering and nuclear magnetic resonance pulsed field gradient technique

H. Jobic, M. Bée, J. Caro, M. Bülow and J. Kärger, J. Chem. Soc., Faraday Trans. 1, 1989, 85, 4201 DOI: 10.1039/F19898504201

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